condensed mlatter nluclear slcience proceedings of the I I th international conference on cold fusion
editor jean-paul biberian
clondensed mlatter n uclear cience proceedings of the I Ith international conference on cold fusion
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c ondensed m after n uclear
cience proceedings of the I Ith international conference on cold fusion
Marseilles, France 31 October-5 November 2004
Editor
Jean-Paul Biberian Universitede la Mediterranee, France
YJ? World Scientific N E W J E R S E Y • L O N D O N • S I N G A P O R E • B E I J I N G • S H A N G H A I • H O N G KONG • T A I P E I •
CHENNAI
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CONDENSED MATTER NUCLEAR SCIENCE Proceedings of the Eleventh International Conference on Cold Fusion Copyright © 2006 by World Scientific Publishing Co. Pte. Ltd. All rights reserved. This book, or parts thereof, may not be reproduced in any form or by any means, electronic or mechanical, including photocopying, recording or any information storage and retrieval system now known or to be invented, without written permission from the Publisher.
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FOREWORD Background It has been a great honor for me to organize I C C F l l in Marseille, France, my hometown. During the ICCF10 in Cambridge, it occurred to me t h a t Marseille was an ideal choice for the I C C F l l . T h e field had matured, and it was obvious t h a t the scientific demonstration of Cold Fusion had been made, and so I proposed to organize the I C C F l l . Certainly, a lot more is needed to be accomplished in the field of research and technology, but we had answers to many of the questions of the scientific community. We knew then for sure t h a t the phenomenon announced in 1989 by Professors Martin Fleischmann and Stan Pons was real. Moreover, they had not foreseen all the discoveries t h a t have been made since their announcement, in particular, the discovery t h a t hydrogen, not only deuterium may be nuclear active under certain conditions. Although much work needs t o be done, it had been shown t h a t transmutations of elements were occurring, indicating t h a t the simple D + D producing helium reaction was not the only reaction channel. It occurred to me at t h a t time t h a t more t h a n science and technology; we had to focus on public relations. My goal in proposing to organize I C C F l l was to bring Cold Fusion to the attention of b o t h the scientists and to the ordinary citizens. There are many things t h a t we do not know a b o u t our research, but we are sure of one thing; it is not only about fusion. We have observed fission and t r a n s m u t a t i o n beyond doubts but there are probably more reactions t h a n we currently know. T h e name of the conference is now International Conference on Condensed Matter Nuclear Science. For the sake of simplicity and continuity, we have decided to keep the old acronym I C C F . In order t o meet our goal of creating awareness a b o u t this, we had the great honor to have Brian Josephson come to the conference. He is the Nobel Prize winner in 1973 in physics for the discovery of the effect t h a t bears his name. I would like to use this opportunity to thank him for his support, as he took the risk by associating his name to a controversial topic. He came to the conference and lectured on "Good and Bad ways of doing Science." It was a great pleasure for me to meet him. He added a lot of weight to the conference. The city of Marseilles under the patronage of the Societe Frangaise de Physique (French Physical Society) granted him and Martin Fleischmann the medal of the city during a ceremony at the City Hall. One full day of the conference was held at the Faculte des Sciences de Luminy, the University where I teach and do research, so t h a t my peers at the university could attend. This has been an opportunity for students and faculty members to come and listen to other scientists t h a n myself on the subject. A demonstration unit was even displayed in the hall of the cafeteria, where many students could see for themselves the reality of the phenomenon.
vi
As we now known, the international thermonuclear experimental fusion reactor (ITER) will be built in Cadarache, which is less t h a n 1 h by car from the conference location. Support for I T E R was very popular in France at the time of the conference and it was very difficult to get the local press to talk about alternative energies. T h e television stations refused to cover the event, although 170 people from 20 different countries had come to the conference, and the keynote speaker was Brian Josephson, the Nobel Prize Laureate. This goes to show how science and politics are mixed up. Nevertheless, a couple of short papers were published in the newspapers, and a few months later a national business newspaper "Les Echos" published a half page article on the conference and CMNS. T h e conference was held at the hotel Mercure. This was a posteriori a good choice because it means mercury in French, and is one of the key ingredients used by the alchemists in the past to make gold! T h e Conference Several important new results were presented during the conference. The joint US/Israeli team, headed by MD Irving Dardik, confirmed t h a t the superwaves they use in their electrolytic experiments help in producing more heat. Also Iwamura et al. showed new t r a n s m u t a t i o n effects in their experiments of diffusion of deuterium gas through a complex structure of palladium and calcium oxide. In addition to the traditional Cold Fusion community, a t e a m of Russian scientists claimed t h a t their experiments show the existence of light monopoles. T h e theory was developed by Lochak from France. They t r y to explain the Chernobyl nuclear accident by the interaction of the monopoles with uranium nuclei, changing the half-life of the nucleus. A German team, comprising of Czerski and Huke, who were working in high-energy physics, discovered CMNS when they lowered the energy of the deuterium beam. They demonstrated t h a t the cross section of the deuterium with deuterated metals was much higher t h a n expected. To explain their experimental d a t a they needed to add a large screening potential. T h e y came to the conclusion t h a t they were doing Cold Fusion, and for the first time attended to the conference. Another important contribution was the one from the Vysotskii t e a m from Ukraine, who confirmed their biological t r a n s m u t a t i o n experiments. Certainly there is a lot more to be discovered. This is very exciting news for science, mankind, and us as scientists. O n t h e theory front, I must confess t h a t there appears t o be far too many. T h e initial idea of the necessity of high deuterium loading in metals to obtain the effect seems to be relevant only for cathodically loaded P d wires. The fact t h a t hydrogen is also active, and t h a t in some cases the loading is obviously low indicates t h a t something else is happening. Storms mentions "active sites," but what are they? Can we use classical q u a n t u m mechanics or q u a n t u m electro dynamics? Do we need poly-neutrons, neutron band structures, or magnetic monopoles? Nobody knows for sure, but every theory developer is convinced t h a t he/she is on the right p a t h to obtain the solution.
vii
The Proceedings When accepting papers for the conference, we decided to be open and to avoid filtering. This is in reaction to the attitude of the scientific community, in its large majority, regarding CMNS. If we publish everything, all kinds of foolish and false ideas can be put forward, but if we are too narrow in our choices, great ideas can be lost. By opening up, we took the position that everyone is capable of deciding for oneself what is good and bad science. We did not want to have a committee to decide and thereby take the risk of missing a great opportunity. These proceedings follow the same philosophy, and therefore the reader must use his/her own understanding to judge the quality of the works presented here. As the editor of this book, I take full responsibility for this choice, and I hope that the future will prove me more right than wrong. Peter Hagelstein from MIT, who organized ICCF10, was a great support in helping me with the quality of the proceedings. He found a company that reformatted all the papers that I had received in numerous formats. This was a precious help and I believe the readers will appreciate it. The Future The ICCF12, as has been decided, will be held in Japan, and the following one in Russia. This is good news because both the countries are very active in the field. After ICCF10, the International Society for Condensed Matter Nuclear Science was created, and helped us to organize the conference. In the future, this society is likely to play a major role in organizing international events. My feeling is that we have now entered a new era, and that the various effects of CMNS will revolutionize science and technology in the near future. Acknowledgements First of all, I would like to thank Jed Rothwell who has put in tremendous work by improving the quality of the papers. English has become the international language for science. However, more than two-thirds of the contributions were made by people coming from non-English-speaking countries. Jed read them all and did his best to understand their contents. Especially, difficult papers were theoretical papers. All my thanks to Vittorio Violante as well from ENEA Frascatti, who co-chaired the conference. I am also grateful to the scientific committee who trusted me and helped me in making decisions. This is also a good place to recognize the role of the sponsors: Infinite Energy, the City of Marseilles, the Departement des Bouches du Rhone, the University who financially helped and made this conference a success. Finally, I am very proud of the help of my two elder children, Melanie and Gabriel without whom this conference would have been a disaster. They worked day and night to the satisfaction of all the attendees. Dr. Jean-Paul Siberian, Chairman, ICCF11, Marseilles, October 2005
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CONTENTS Foreword
v 1. G E N E R A L
A tribute to gene Mallove - the "Genie" reactor K. Wallace and R. Stringham
1
An update of LENR for ICCF-11 (short course, 10/31/04) E. Storms
11
New physical effects in metal deuterides P. L. Hagelstein, M. C. H. McKubre, D. J. Nagel, T. A. Chubb, and R. J. Hekman
23
Reproducibility, controllability, and optimization of LENR experiments D. J. Nagel
60
2. E X P E R I M E N T S Electrochemistry Evidence of electromagnetic radiation from Ni-H systems S. Focardi, V. Gabbani, V. Montalbano, F. Piantelli, and S. Veronesi
70
Superwave reality 7". Dardik
81
Excess heat in electrolysis experiments at energetics technologies I. Dardik, T. Zilov, H. Branover, A. El-Boher, E. Greenspan, B. Khachaturov, V. Krakov, S. Lesin, and M. Tsirlin
84
"Excess heat" during electrolysis in platinum/I^COa/Nickel light water system J. Tian, L. H. Jin, Z. K. Weng, B. Song, X. L. Zhao, Z. J. Xiao, G. Chen, and B. Q. Du
102
Innovative procedure for the, in situ, measurement of the resistive thermal coefficient of H(D)/Pd during electrolysis; cross-comparison of new elements detected in the Th-Hg-Pd-D(H) electrolytic cells F. Celani, A. Spallone, E. Right, G. Trenta, C. Catena, G. DAgostaro, P. Quercia, V. Andreassi, P. Marini, V. Di Stefano, M. Nakamura, A. Mancini, P. G. Sona, F. Fontana, L. Gamberale, D. Garbelli, E. Celia, F. Falcioni, M. Marchesini, E. Novaro, and U. Mastromatteo
108
Emergence of a high-temperature superconductivity in hydrogen cycled Pd compounds as an evidence for superstoihiometric H/D sites A. Lipson, C. Castano, G. Miley, B. Lyakhov, and A. Mitin Plasma electrolysis Calorimetry of energy-efficient glow discharge - apparatus design and calibration T. B. Benson and T. 0. Passell Generation of heat and products during plasma electrolysis T. Mizuno, Y. Aoki, D. Y. Chung, and F. Sesftel Glow discharge Excess heat production in P d / D during periodic pulse discharge current in various conditions A. B. Karabut Beam experiments Accelerator experiments and theoretical models for the electron screening effect in metallic environments A. Huke, K. Czerski, and P. Heide Evidence for a target-material dependence of the neutron-proton branching ratio in d + d reactions for deuteron energies below 20keV A. Huke, K. Czerski, T. Dorsch, and P. Heide
128
147
161
178
194
210
Experiments on condensed matter nuclear events in Kobe University T. Minari, R. Nishio, A. Taniike, Y. Furuyama, and A. Kitamura
218
Electron screening constraints for the cold fusion K. Czerski, P. Heide, and A. Huke
228
Cavitation Low mass 1.6 MHz sonofusion reactor R. Stringham Particle detection Research into characteristics of X-ray emission laser beams from solidstate cathode medium of high-current glow discharge A. B. Karabut Charged particles from Ti and Pd foils L. Kowalski, S. E. Jones, D. Letts, and D. Cravens
238
253
269
Cr-39 track detectors in cold fusion experiments: Review and perspectives A. S. Roussetski
274
Energetic particle shower in the vapor from electrolysis R. A. Oriani and J. C. Fisher
281
Nuclear reactions produced in an operating electrolysis cell R. A. Oriani and J. C. Fisher
295
Evidence of microscopic ball lightning in cold fusion experiments E. H. Lewis
304
Neutron emission from D2 gas in magnetic fields under low temperature T. Mizuno, T. Akimoto, A. Takahashi, and F. Celani
312
Energetic charged particle emission from hydrogen-loaded Pd and Ti cathodes and its enhancement by He-4 implantation A. G. Lipson, G. H. Miley, B. F. Lyakhov, and A. S. Roussetski
324
H-D Permeation Observation of nuclear transmutation reactions induced by D2 gas permeation through Pd complexes Y. Iwamura, T. Itoh, M. Sakano, N. Yamazaki, S. Kuribayashi, Y. Terada, T. Ishikawa, and J. Kasagi
339
Deuterium (hydrogen) flux permeating through palladium and condensed matter nuclear science Q. M. Wei, B. Liu, Y. X. Mo, X. Z. Li, S. X. Zheng, D. X. Cao, X. M. Wang, and J. Tian Triggering Precursors and the fusion reactions in polarized P d / D - D 2 0 system: effect of an external electric field S. Szpak, P. A. Mosier-Boss, and F. E. Gordon Calorimetric and neutron diagnostics of liquids during laser irradiation Yu. N. Bazhutov, S. Yu. Bazhutova, V. V. Nekrasov, A. P. Dyad'kin, and V. F. Sharkov
351
359
374
Anomalous neutron capture and plastic deformation of Cu and Pd cathodes during electrolysis in a weak thermalized neutron field: Evidence of nuclei-lattice exchange A. G. Lipson and G. H. Miley H-D Loading An overview of experimental studies on H/Pd over-loading with thin Pd wires and different electrolytic solutions A. Spallone, F. Celani, P. Marini, and V. Di Stefano
379
392
3. T R A N S M U T A T I O N S Photon and particle emission, heat production, and surface transformation in Ni-H system E. Campari, G. Fasano, S. Focardi, G. Lorusso, V. Gabbani, V. Montalbano, F. Piantelli, C. Stanghini, and S. Veronesi
405
Surface analysis of hydrogen-loaded nickel alloys E. Campari, S. Focardi, V. Gabbani, V. Montalbano, F. Piantelli, and S. Veronesi
414
Low-energy nuclear reactions and the leptonic monopole G. Lochak and L. Urutskoev
421
Results of analysis of Ti foil after glow discharge with deuterium I. B. Savvatimova and D. V. Gavritenkov
438
Enhancement mechanisms of low-energy nuclear reactions F. A. Gareev, I. E. Zhidkova, and Y. L. Ratis
459
Co-deposition of palladium with hydrogen isotopes J. Dash and A. Ambadkar
477
Variation of the concentration of isotopes copper and zinc in human plasmas of patients affected by cancer A. Triassi Transmutation of metal at low energy in a confined plasma in water D. Cirillo and V. Iorio The conditions and realization of self-similar Coulomb collapse of condensed target and low-energy laboratory nucleosynthesis S. V. Adamenko and V. I. Vysotskii
485
492
505
The spatial structure of water and the problem of controlled low-energy nuclear reactions in water matrix V. I. Vysotskii and A, A. Kornilova Experiments on controlled decontamination of water mixture of longlived active isotopes in biological cells V. I. Vysotskii, A. Odintsov, V. N. Pavlovich, A. B. Tashirev, and A. A. Kornilova
521
530
Assessment of the biological effects of "Strange" radiation E. A. Pryakhin, G. A. Tryapitsina, L. I. Urutskoyev, and A. V. Akleyev
537
Possible nuclear transmutation of nitrogen in the earth's atmosphere M. Fukuhara
546
Evidences on the occurrence of LENR-type processes in alchemical transmutations J. Perez-Pariente History of the discovery of transmutation at Texas A&M University J. O.-M. Bockris
554
562
4. THEORY Quantum electrodynamics Concerning the modeling of systems in terms of quantum electro dynamics: The special case of "Cold Fusion" M. Abyaneh, M. Fleischman, E. Del Giudice, and G. Vitiello Screening Theoretical model of the probability of fusion between deuterons within deformed lattices with microcracks at room temperature F. Fulvio Resonant tunnelling Effective interaction potential in the deuterium plasma and multiple resonance scattering T. Toimela Multiple scattering theory and condensed matter nuclear science"super-absorption" in a crystal latice X. Z. Li, B. Liu, Q. M. Wei, N. N. Cai, S. Chen, S. X. Zheng, and D. X. Cao
587
612
622
635
Ion band states Framework for understanding LENR processes, using conventional condensed matter physics S. R. Chubb
646
I. Bloch ions T. A. Chubb
665
II. Inhibited diffusion driven surface transmutations T. A. Chubb
678
III. Bloch nuclides, Iwamura transmutations, and Oriani showers T. A. Chubb
685
Bose-Einstein condensate Theoretical study of nuclear reactions induced by Bose-Einstein condensation in Pd K.-I. Tsuchiya and H. Okumura Proposal for new experimental tests of the Bose-Einstein condensation mechanism for low-energy nuclear reaction and transmutation processes in deuterium loaded micro- and nano-scale cavities Y. E. Kim, D. S. Koltick, R. G. Reifenberger, and A. I. Zubarev Mixtures of charged bosons confined in harmonic traps and BoseEinstein condensation mechanism for low-energy nuclear reactions and transmutation processes in condensed matters Y. E. Kim and A. L. Zubarev
694
703
711
Alternative interpretation of low-energy nuclear reaction processes with deuterated metals based on the Bose-Einstein condensation mechanism Y. E. Kim and T. O. Passell
718
Multi-body fusion 3 He/ 4 He Production ratios by tetrahedral symmetric condensation A. Takahashi
730
Phonon coupling Phonon-exchange models: Some new results P. L. Hagelstein
743
Neutron clusters Cold fusion phenomenon and solid state nuclear physics H. Kozima
769
Neutrinos, magnetic monopoles Neutrino-driven nuclear reactions of cold fusion and transmutation V. Filimonov
776
Light monopoles theory: An overview of their effects in physics, chemistry, biology, and nuclear science (weak interactions) G. Lochak
787
Electrons clusters and magnetic monopoles M. Rambaut
798
Others Effects of atomic electrons on nuclear stability and radioactive decay D. V. Filippov, L. I. Urutskoev, and A. A. Rukhadze
806
Search for erzion nuclear catalysis chains from cosmic ray erzions stopping in organic scintillator Yu. N. Bazhutov and E. V. Pletnikov
818
Low-energy nuclear reactions resulting as picometer interactions with similarity to K-shell electron capture H. Hora, G. H. Miley, X. Z. Li, J. C. Kelly, and F. Osman
822
5. OTHER TOPICS On the possible magnetic mechanism of shortening the runaway of RBMK-1000 reactor at Chernobyl Nuclear Power Plant D. V. Filippov, L. I. Urutskoev, G. Lochak, and A. A. Rukhadze
838
Cold fusion in the context of a scientific revolution in physics: History and economic ramifications E. Lewis
854
The nucleovoltaic cell D. D. Moon
868
Introducing the book "Cold Fusion and the Future" J. Rothwell
871
xvi
Recent cold fusion claims: Are they valid? L. Kowalski
879
History of attempts to publish a paper L. Kowalski
888
Author Index
895
A T R I B U T E TO G E N E MALLOVE - THE "GENIE" R E A C T O R
K. W A L L A C E A N D R. S T R I N G H A M PO Box 1230, Kilauea,
HI 96754,
USA
"Genie", a 40kHz sonofusion reactor consists of two opposing 40kHz piezos separated by 4 mm of D2O, with a centered Ti target foil, with one piezo transmitting, the other receiving and taking that signal, amplifying it, then feeding it back to the transmitter as the resonating frequency of the reactor. This process makes for efficient watt input, Q{, where 80% of these watts will be used as the acoustic input, Q a , to the "Genie" sonofusion reactor. In the reactor the transient cavitation bubbles, TCBs, produce billions of low-energy high-density jets per second that accelerate deuterons into foil targets producing excess heat, Qx. The Qx is determined by calorimetric measurements of experiments that use coolant water circulated to the surface of the well insulated reactor and data collected in the form of T-ln and Tout at steady-state temperatures and coolant flow rate. The total watts out, Q0, minus Q a ideally should equal zero, and we know that this calorimetry method has several losses that are not measured. This makes the method very conservative when looking for Qx. The Qx must make up those heat losses before making its presence known. The result from experiments of system I using flow x DT x 4.184 for Q0 — Q\ = Qx shows that Qx values over unity are the norm. System II used a more realistic calculation for Qx, where flow X DT X 4.184 for Qo — <2a = Qx showed increased results. The calibration of the reactor with a Joule heater (JH) and the substitution of H2O for D2O produced measurements that showed the reactor calorimetry was close to zero Qx production as one would expect. These measurements showed that heat in = heat out, a good zero indicating no Qx, for the operation of the "Genie" sonofusion reactor.
1. Introduction Gene Mallove would be pleased to know that his work and the work at NERL laboratory, NH produced a cavitation fusion device with reproducible excess heat capabilities after a few modifications. Even better, a sonofusion device produced Q0 (the heat out) in an amount that exceeds Q\ (the total heat input). The original work on this device came to a close because of a shortage of money and time. The NERL laboratory reactor was sent to SRI for testing where problems developed with D2O and Ar leakage and therefore was not suitable for testing. The abandoned device was purchased from Gene Mallove by Kip Wallace, my brother-in-law, who was present during the device testing at SRI and Kip proceeded to modify the device. The two major modifications were making the reactor capable of operating at 6 atm. of Ar pressure without leaking and a feedback oscillator based on the natural resonance of the reactor. Kip brought the modified device to First Gate's laboratory in Hawaii for calorimetry measurements, which showed positive Qx, excess heat. The initial input from Gene Mallove, Ken Rauen, Jan Roos, Chris 1
2
Eddy and the rest of the NERL lab with some more time and thought supplied by Kip Wallace resulted in experiments that produced positive Qx. The original sonofusion reactor that Gene purchased from First Gate is stored with other equipment at the NERL laboratory. The main tool for demonstrating the presence of Qx is the discovery of a system robust enough to demonstrate a sizable amount of unexplained heat coming from a fully understood system. The product for commercial use is Qx and other products such as 4 He, T, and other possible nuclear products may also be of commercial value. We have such a system with conservative data showing that the "Genie" sonofusion reactor produces Qx where Q0 exceeds Q\. Calorimetry is the method for measuring the amount of heat produced by a system regardless of its source. The calorimetry that was used for this 3 kg sonofusion reactor with opposing 40 kHz piezos was limited to a simple methodology. We isolated the reactor in the center of an insulated box. The maximum operating steady-state temperature was 70 °C with the heat removed from the surface of the reactor by copper coils with circulating water. The ratio of surface area of the insulation box to the reactor was 100. The coolant flow rates were varied from 0.5 to 6ml/s, which when multiplied by DT measurements (T out — T;n) produced the Q0. To calibrate the circular reactor (a 15cm tube with a 9 cm diameter), a long resistance Joule heater (JH), 100 W, was coiled at each end of the reactor. Calorimetry is always imperfect and the flaws in this methodology will show a lower Qx than generated. The Qx of this device demonstrates an over-unity system and will show the way to others to explore cavitation that has the robust nature for future energy systems. The economics of cavitation sonofusion systems are here today. 1 2. Calorimetry A 30 cm x 40 cm x 40 cm Styrofoam box is filled with a polyurethane foam with the sonofusion reactor placed at the center. The circulating water flows through a 4-mm diameter copper tubing that is 350-cm long and tightly coiled on the surface of the steel reactor housing. The thermocouple measurements of T;n and T out provide for the DT values of this water coolant flow for the calculation of Qx. Coolant water is pumped through the circulation system by a variable FMI pump with a 0.635 cm ceramic piston. The system starting from the pump goes though a flow meter. The coolant then flows into the copper coil (Tin), removing heat, and out of the coil (Tout) and finally into the coolant bath heat exchanger reservoir. The flow was calibrated at regular intervals with a volume measurement over a 1 min time period taken at the output coolant flow into an 81 water coolant bath. The reservoir is the recipient of the heat from the reactor. Its large volume and open surface allows for steady-state Tm temperature measurements. From the reservoir the cool flow continues and completes its cycle to the pump. Note that the diurnal temperature fluctuation is only 2°C in the Kauai First Gate laboratory (Fig. 1). The flow rate
3
Insulation -
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— JH r x
Ti impedance matching slug transmitter Bolt assembly Piezo Mass backing
Figure 1. The experimental set-up. This figure shows the Genie reactor in its operating mode. The insulated 3 kg cylindrical steel reactor where TCs measure the steady-state reactor DT and where the partitioned Qi, gives Q a , the oscillator's input to the transmitter piezo. The transmitter signal is picked up by the receiver stack, which is amplified for the 40 kHz transmitting piezo output. The system resonates at its feedback resonance. The 81 of coolant water is circulated with an FMI pump while the reactor is powered by the sonicator, Q\, or JH as data are collected. The reactor is sealed to hold the 7 a t m of Ar. The 15 cc of D2O holds a target of Ti about 50 cm 2 surface area. The insulation about 15 cm thick is polyurethane foam and there is no perceptible temperature change from the outside surface of the reactor at steady-state temperature. The oscillator is in its calorimeter with its JH calibrator to measure the Qi's partition into Q a - The Q0 is found from F x DT x k.
has an effect on the efficiency of heat removal and on the DT that influences the Qx measurement. A low-coolant flow rate provides a high DT but a low Qx and a high-flow rate provides a low DT but a better Qx value. A compromise flow rate between 3 and 4ml/s realizing that the Qx measurement will be low but a better DT measurement is the result. It is important that the measurements of Q0 be made at steady-state temperatures and steady flow rates. This provides the only good values for DT °C. The TC data are collected at lmin intervals where QQ = F x DT x 4.184W (F is the
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Figure 2. The reduced data for Qx determination. This figure shows the measurement of Qx in four different systems. Two using Joule heater calibration inputs with data points clustered around the zero line for JH (open circles). The other two using acoustic inputs with data points that are above the Q a = Q0 zero line for the sonication input. Those data points that are on or below the zero line are high temperature runs or low flow runs (HT or LF).
flow rate in ml/s) and Q0 — Qi = Qx. If you want a more realistic value add Qoc, the heat lost from the oscillator (Qoc = 0.2 x Q;) to the Qx value (Qa = 0.8 x Q ; ) and Q[ = Qos + Q& (Fig. 2). Calorimetry data established the 20% values of Q\ that are lost to the environment, Qoc. 3. Experimental The sonofusion reactor consists of a heavy steel pipe housing with two opposing piezo stacks with Ti faces and 6 mm between the Ti piezo faces (Fig. 1). In the volume between the faces is the reactor's D2O with a Ti foil suspended in the center. This is a static system as the D2O is not flowing. At the top of the reactor is an Ar port and small pressure gauge. The reactor is sealed with " 0 " rings and placed at the center of an insulated box. The copper coils remove the flow of hot coolant water from the reactor to the heat exchange water bath reservoir. Another set of copper coils contains a thin wire JH for calibration purposes. An FMI piston pump with variable speed control circulates the coolant, and the coolant flow is measured with a flow meter. The flow is also checked by its volumetric flow (Fig. 3). The piezo stacks are made up 1/2 wave Ti slugs with 4 mm PZT piezo. One stack is a 40 kHz transmitter, the other a receiver - a matched pair. The electrical input to the transmitter comes from the line to a controlling variac to a wattmeter and a high voltage transformer, then to the oscillator. The oscillator is located in a box calorimeter with the high frequency (40 kHz) input going to the piezo, Q a . The other
5
Calibration of the flow meter
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Flow meter reading gal/h Figure 3. The coolant flow calibration. This figure shows the flowmeter reading vs. the volumetric measurement for each run.
piezo stack is the receiver and picks up the reactor resonant frequency - the piezo and reactor's primary resonance - and sends that frequency back to the oscillator to be amplified as the input signal. The advantage is a single amplitude and frequency that follows small resonance changes in the reactor as the temperature and small geometry change in the reactor. The oscillator heat production is measured and can be subtracted from Q; to give more accuracy and added value to Qx. The box is a JH used to calibrate the heat loss of Q\ and determine its efficiency (the loss averaged over 20 runs from the oscillator and transformer was 20%) (Fig. 2). The D2O was degassed and put into an Ar filled reactor. The Ar was added via a syringe port to a pressure of 5atm over the D2O. The loaded reactor with the thermocouples in place was located at the center of the styrofoam box and filled with an expanding foam polymer. The 81 coolant reservoir was filled and the pump started for the circulation of coolant through the Cu coolant coils. After checking the seven TCs (40 gauge, type K) and the coolant flow rate, the power was turned on, a wait of 120 min before the system reached steady-state temperature, then the Qx measurements were started. The reactor was sampled every minute for data and the runs lasted about 400min. The data could be checked in real time for Qx. We used an Omega 16 channel PCI-DAS-TC for the data gathering. The data were collected in a spreadsheet on a Windows 2000 PC.
4. Data and Interpretation The data was collected over a 6-week period and was divided into SF I and II (sonofusions I and II). SF I did not have a JH and SF II was reloaded with D 2 0 and Ar with the second JH installed (the first was in the SF reactor) in the Qoc
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calorimeter and finally reinsulated (Fig. 1). The collected data were reduced in a spreadsheet to show variations in important parameters (Table 1). We can look at QQ and Q\ of the sonocation runs of D2O and H2O and compare with the JH calibration runs with D2O and H2O. The calibration runs show no Qx. In the simplest form Q0-(Qi + Qx), heat out = heat in, and always equals 0 if there is no Qx, so Qx = Qo — Qi (SF I). In the case where reactor JH is the energy input into D2O and H 2 0 in calibration runs, the Qx should equal 0, which it does. Also in the case where there is sonication in H2O runs, Qx is much less than with D2O runs. This data indicates a small Qx with H 2 0 in sonication runs. The data in the case of sonication of D 2 0 shows varying degrees of Qx production. Figure 2 shows the reduced data of Qx from two slightly different reactor configurations. The SF I system runs and the SF II system runs are shown. Also shown are the JH runs that serve as a calibration for the SF runs. The data from the JH runs are treated exactly the same as the SF runs and show no Qx production. The zero line in the graph represents Qi, the input watts, and any data above that line is a Qx production point (the error is ± 1W). The light line from the origin slanting down from left to right is that part of Q; that is lost as heat to the oscillator and has a value of 20% of Q[. So any point above that line is a real Qx production run (the error is ± 1W). The data from the SF I is all above the zero line which means it was over unity - more energy out than in. In Fig. 3, the SF II D2O system is producing Qx at a much higher level than in SF II H2O, which is consistent with our old data. 2 ' 3 At 40kHz the Qx data are not truly reproducible but are consistent in the Qx effect. 5. Discussion The data presented shows that Qx is produced in a static 40 kHz system with no circulation of the cavitation liquid. The results are very similar to old work with the main difference being the way in which the opposing piezos are used and powered. In the old work both piezos were transmitting and used a frequency sweep through several kHz coupled with a variable voltage input. 2 ' 3 Compare this with the input of a single resonant frequency of the "Genie" reactor amplified from the receiver piezo. The single frequency may be just off the sweet spot and the introduction of a narrow sweep may improve Qx results. The Qi efficiency of 80% for the "Genie" reactor was much higher than that of the old Mark III 2 with an efficiency of 30%. The operating temperatures for the Mark III were 100°C and higher with similar Ar pressures. The parameters of operating temperatures, of pressures, and of Qa inputs are coupled and will have one of three outcomes. These are cavitation bubble frothing, no cavitation bubbles, and TCB production. It is the TCB production that relates the correct balance of the three parameters. 2 It appears that SF I had higher Ar pressure and with the other two parameters at about the correct magnitude, temperature and increased Q a input, produce the largest Qx. The lower Ar pressures in SF II produces a more moderate Qx production. A reactor
9
temperature of runs in the SF II reactor system of 30°C produced a measureable Qx and at high temperatures around 60° C produced no QX' The answer may be that the cavitating D 2 0 was frothing at 60° C. More work should be done in this area. A tentative path and mechanism to Qx have been proposed by several theorists 4 - 7 and a path has been put forward for the TCBs that depends on the tremendous transient deuteron pressures that are generated during the final stages of TCB collapse and the following deuteron lattice implantation. 8 The effect of the flow rates on the measurement of Qx was always an issue. At low-flow rates there was a large DT, which is good but DT x F was low. At the other extreme was a high flow rate with a low DT and its DT x F product was higher and closer to the real Qx. One can slowly vary the flow rate and see an asymptotic value for Qx. This is a good idea but very time consuming and we were satisfied with the lower Qx values we were measuring. In our calculations, we used two different measured relationships. One was the rate of flow measurements and the other the DT measurements. We did a volumetric measurement as well as using a flow meter for the water circulation flow measurements. A graph of this data puts the flow data on a solid footing, although there was some error (±3%) (Fig. 3). The second was the DT temperature measurements of the water flow in and out of the "Genie" SF reactor measured at ±0.2°C. The measurement of the heat loss of the oscillator, Qos, was simple. The insertion of a TC into the oscillator's Al heat sink produced a relative oscillator temperature value for each run. These oscillator heat sink temperatures were converted into watts via a 15 W variable JH. Both the oscillator and the JH were housed in a box calorimeter (see Sect. 2 and Fig. 1). 6. Conclusion The "Genie" sonofusion reactor produces Qx in amounts that are robust enough to overcome the shortcomings of the calorimetry measurements. The insulation was substantial and allowed for the enclosed reactor to be observed as a point heat source. The reactor (small, hot, and conductive) was placed in the center of a large insulated box. The small amount heat loss from the exterior surface of the box was viewed as heat arriving from a point source in the center of the insulated box. In the reactor there was no heat perceived at the surface of the insulating box because the circulating water removed the reactor heat. The water flowing through the copper tubing at a rate around 4 ml/s facilitated the majority of the heat removal from the reactor. As an example a DT of 1.5°C with a Q0 around 25 W and a Q\ of 20 W produced nominal Qx of 5 W not considering any heat losses. The use of the two calibration Joule heaters, one for the oscillator and one for the reactor, provided the comparative rates of heat loss to verify the SF I and II data (Fig. 3). The "Genie" sonofusion reactor is robust and with the calorimetry used by the NERL laboratory would give much better results than presented in this paper.
10
7.
Summary
T h e reactor consists of 3 kg of steel, two opposing piezos, a reactor filled with 20 ml of D2O s a t u r a t e d with Ar, and a 50 g power supply. T h e calorimetry involved measurements of T; n and T o u t of a circulating water coolant t h a t produced steadystate temperatures and flow rates. T h e Q\, input, was subtracted from the Q0, to give the excess heat Qx- T h e maximum Qx was nearly double Q\. Future improvements should focus on reducing the weight of the "Genie" to 1 kg along with an increase in Qx. B o t h can be accomplished with a redesign. This would increase t h e power density o u t p u t of this reactor.
Acknowledgments We want to t h a n k Gene Mallove, Ken Rauen, J a n Roos, Chris Eddy, and all the people associated with the N E R L laboratory who risked a lot of resources and personal energy to make this "Genie" work. Time was the factor as there was a learning curve with the new "Genie" t h a t was difficult to overcome. We want to t h a n k Kip's associates who donated their time and energy to continue this project t h a t started in the year 2000.
References 1. R. Stringham, in Proceedings ICCF 11 (Marseille, France, 30 Oct.-Nov.5, 2004) to be published. 2. R. Stringham, in Proceedings of the IEEE Ultras. Intern. Symp. (Sendai, Japan, vol. 2, 1107, Oct. 5-6, 1998). 3. R.S. Stringham, in Proceedings of the ICCF-8 (Lerici (La Spezia), Italy, May 21-26, 2000), pp. 299-304. 4. S.R. Chubb, in Proceedings of the ICCF 10 (Boston, MA, USA, Aug. 24-29, 2003) to be published. 5. Y.E. Kim, in Proceedings of the ICCF 10 (Boston, MA, USA, Aug. 24-29, 2003) to be published. 6. RL. Hagelstein, in Proceedings of the ICCF 10 (Boston, MA, USA, Aug. 24-29, 2003) to be published. 7. X.Z. Li, in Proceedings of the ICCF 10 (Boston, MA, USA, Aug. 24-29, 2003) to be published. 8. R. Stringham, in Proceedings of the ICCF 10 (Boston, MA, USA, Aug. 24-29, 2003) to be published.
A N U P D A T E OF L E N R FOR I C C F - l l ( S H O R T C O U R S E , 10/31/04)*
EDMUND STORMS Lattice
Energy,
LLC,
Santa
Fe, NM,
USA
1. Introduction Shortly after Fleischmann and Pons made their announcement, a myth was created by people who could not accept their claims. This myth stated that the claims were impossible and could not be replicated. Like most myths, this one was not true at the time it was created and continues to grow even less true today. Replication has become easy using some methods and evidence has now reached a quality typical of that accepted in other fields of science. From the beginning of the field in 1989, people used the term "Cold Fusion" to describe what was proposed to happen when anomalous power was observed using, usually, an electrolytic cell. Such a term was accurate when D-D fusion was thought to be the source of energy. However, now many other kinds of nuclear reactions have been observed. Therefore, a more general and accurate term is Low Energy Nuclear Reactions (LENR). If a person wishes to emphasize the mechanism, the term Chemically Assisted Nuclear Reactions (CANR) can be used instead. The general field of study founded by Fleischmann and Pons is now known as Condensed Matter Nuclear Science. The reaction paths for fusion are: (1) (2) (3) (4)
d+ d+ d+ p+
d d d d
=» 3 He(0.82MeV) + neutron(2.45MeV), =>• proton(3.02MeV) + tritium(1.01 MeV), ^ 4 H e + "energy" (23.5MeV), = > 3 H e + "energy"(5.6MeV).
The first two paths, giving detectable neutrons and tritium, are taken when fusion occurs in a plasma or when sufficient energy is applied to the system, so called "Hot Fusion". The third path is hardly ever seen at these high energies. In sharp contrast, the third path is the main one observed under LENR conditions when deuterium is present, while paths # 1 and # 2 are absent for all practical purposes. More will be said about these paths later. People have proposed a forth path when "normal" hydrogen is present, including in a paper given in this conference *This paper was written as an overview of the field of LENR and as an introduction to the ICCF11 conference, citations for the claims are not supplied, but can be obtained from various reviews available on www.lenr-canr.org. 11
12
(Takahashi). However, no evidence exists for this reaction. The few occasions when He was detected, its presence could be explained as resulting from tritium decay. In fact, even a small amount of protium in heavy water will stop energy production from a Fleischman-Pons cell. The LENR process includes a number of anomalous effect as follows: 3
(1) Anomalous heat production was the first anomalous product reported and is the one having the greatest commercial interest. It is also a challenge to explain because it involves a nuclear reaction rate that can exceed 1011 events/s. (2) As expected, energetic particles of the expected reaction products are observed, each having the expected energies. However, the rate is much too small to be consistent with the heat producing reaction. (3) Transmutation is the term that describes any nuclear reaction that changes one element into another. Fusion is just a special form of transmutation. Evidence for many different transmutation reactions have now been reported, a few of which will be described in more detail later. (4) Electromagnetic radiations of a conventional nature, such as X-ray and 7-ray, have been observed at very low, but anomalous, intensities. In addition, anomalous types of radiation have been reported (Matsumoto, 1990), several of which will be described at this conference (Ivoilov et al, and Fisher). Different methods have been used to produce measurable energy, including the following: (1) Electrolysis. This is the method used by Fleischmann and Pons and it is the method that has been the most thoroughly investigated. It involves passing a current through a solution containing D2O or H2O and a dissolved salt, usually based on lithium. The hydrogen isotope reacts with the cathode and creates an environment that can initiate a nuclear reaction. These reactions have also been stimulated by laser light (Mastromatteo et al., this conference) and various applied RF frequencies. (2) Plasma discharge in a liquid. If the voltage applied to an electrolytic cell is increased to between 100 and 200 V, a plasma discharge can occur in addition to the usual electrolytic action. This results in many kinds of observed nuclear reactions being initiated (Cirillo et al., and Chung et al, this conference). (3) Gas discharge. If sufficient voltage is applied to D 2 or H2 gas, various kinds of discharge can be created, depending on pressure and applied voltage. This action causes hydrogen isotope ions to bombard the cathode where various nuclear reactions are observed (Savvatimova et al., this conference). These ions can also be generated external to the reaction chamber and accelerated at the cathode.
13
(4) Ambient gas. When the nuclear active material is placed in D2 gas, nuclear reactions have been observed to occur without the need to apply energy other than modest heating. (5) Deuteron electromigration. When deuterium is caused to diffuse through a material under the influence of an applied electric potential, anomalous energy is observed. (6) Sonic implantation. When intense sound is caused to pass through a liquid, cavitation bubbles are generated, which upon collapse against a metal during part of the wave cycle inject D + into the metal. As the metal loads with deuterium, nuclear reactions have been observed. A paper describing this method is presented at this conference (Stringham). 2. Anomalous Heat When anomalous heat is made in a Fleischmann-Pons cell, everyone who takes time to make such measurements observes several characteristic behaviors. Examples of three frequently observed behaviors are shown in Figs. 1-6.
• P14/D,0-Linear0 P13/H20
—0.1 J Electrochemical current density (A/cm2 Figure 1.
Measurement of current density vs. excess power made at SRI (US).
14
1.5 2.0 Cell current (A) Figure 2. Measurement of applied current vs. resulting excess power made at EKS Inc. after various times.
Figures 1 and 2 show a need for an initial amount of applied current before excess energy can be produced. After this critical current has been achieved, excess current increases in a linear manner as further current is applied. This increase eventually saturates when too much current is applied. Figure 1 shows that a cell running at the same time containing H2O instead of D2O does not show this effect. Figure 2 shows the gradual turn on of excess power as current is applied over an extended time. This time has been found to be as short as several days and as long as months. Initially, this time was thought to be necessary for the cathode to reach the required high D/Pd ratio. Although this is a partial reason, the main delay appears to be caused by slow formation of active deposit on the cathode surface. This deposit can be applied much more rapidly by electroplating proper metals on an inert cathode surface before heat measurement or during heat measurement, the so called co-deposition method. Figure 3 shows how excess power production is affected by the average D/Pd ratio of a palladium cathode. This ratio is only the average composition of the entire sample and does not represent the composition of the active surface region. This active region has a measured composition in excess of PdDx.5 and is rich is many other elements besides palladium and deuterium.
15
„ C1—Parabolic 0.875 555
0.88
0.89
0.90
0.91
0.92
0.93
0.94
0.95
0.96
0.97 0.98
Atomic ratio (D/Pd) Figure 3. Relationship between measured average composition of a palladium cathode and excess power. Work done at SRI. The large amount of scatter is partially caused by changes in temperature and applied current in addition to composition.
Palladium is not the only cathode material that is capable of generating excess power. Figure 4 shows an example of a deposit applied to a platinum cathode and Fig. 5 shows excess power obtained from a silver cathode to which a deposit was applied by using a CO2+H2O plating solution. Titanium has also successfully produced excess energy (Dash).
3. Particle Detection Increasing attention is being paid to detecting particles emitted from various kinds of apparatus and materials. Several efforts are described at the conference (Kowalski, Oriani, Kasagi, Lipson, Roussetski, and Campari) using in many cases CR-39 as the detector. Many attempts, some successful and some not, have been made to detect neutron emission. When found, most neutrons had the expected energy, but occasionally with energy greater than the expected amount. Recently, neutron emission has been detected from D2 gas cooled in a magnetic field (Mizuno, this conference). Neutron involvement may be more complex than previously thought (Lipson and Miley, this conference). Protons have been detected with the expected
16 0.8-
Figure 4. Applied current vs. excess power for a platinum cathode to which a deposit was applied. Work done at EKS Inc. The initial and final calibrations of a flow-type calorimeter are shown. The deposit became inactive when subjected to excessive current, but could be reactivated by proper treatment.
energy. Alpha particles are detected with the expected energy and as ambient helium gas (Violante, this conference). Occasionally, alpha particles are detected where they are not expected, suggesting a novel process for their formation (Oriani and Fisher, this conference). The same duel measurement of energetic particle and ambient gas has been made for tritium. However, in all cases, the rate of particle emission is less a factor of 1010 events/s below the rate of 4 He production and inconsistent with anomalous power measurements. The question people who use this information as support for a theory need to answer is, "Do these energetic particles result from the same mechanism and nuclear-active-environment as does anomalous energy or are two independent processes operating"? 4. Source of Anomalous Energy Anomalous energy is now known to result from 4 He production. Two independent and careful studies are compared in Fig. 6. The two studies are consistent with each other and with the amount of helium being about a factor of two below the expected energy for a D-D fusion reaction. The factor of two results because about
17
1/2 of the helium produced in the near-surface region is expected to be retained by the cathode and unavailable to the gas measurement. Also, notice that a sample containing boron shows a behavior consistent with samples where boron is absent. This result indicates that boron is not involved in the energy producing reaction. At least six independent studies have reported the same relationship between 4 He production and energy generation. Flow-type calorimeter
1.5
2.0
Applied current (A)
Figure 5. Effect of applied current on excess power for a silver cathode to which a deposit was applied by electrolyzing in a solution of CO2 in water.
5. Transmutation Evidence for transmutation is growing and includes results reported at this conference (Szpak et al., Iwamura et at, Cirillo et al., Chung et al., Mastromatteo et al., and Campari). A broad collection of anomalous product elements have been found including most often Ca, Cu, Zn and Fe, frequently with abnormal isotopic ratios. However, because the elements being transmuted are frequently unknown and/or in unknown amounts, the path to form the observed product element is often hard to discover. This problem has been solved by Iwamura et al. who have published a series of papers, including one at this conference, that examine the transmutation
18
10 li: Bush and Lagowski [5] §
r
fr
350,525 and 700 mA
......... Pd containing B
J 1011
,
I
A Miles et a/. [4]
0 500mA • — in 10 .
0.00
400 mA
24 MeV/Atom reaction
j
0.05
i
0.10
i
0.15
Excess power (W)
Figure 6. Comparison between two independent studies of power generation vs. helium generation plotted as atoms of He/energy produced. The dashed line shows the expected value produced by a D + D = He fusion reaction. The work was done at China Lake under Navy sponsorship and at SRI.
of individual elements. They report causing the following reactions by passing D 2 through Pd-CaO-Pd layers. 4D + 133 Cs 55 = 141 Pr 59 (within 100 A of surface), 4D + 88 Sr 38 = 96 Mo 42 (isotope ratio transfer), 6D + 138Ba56 = 150Sm62 (isotope ratio transfer). They measured target loss and product gain using XPS, SIMS, XANES, ICP-MS, and X-ray Fluorescence. The latter two reactions show a transfer of isotopic ratio from the reactant to the product nuclei. The basic process has been replicated in Italy and Japan, and replication is underway in the US. Important to note that the 133 Cs 5 5 is transformed only in the first 100 A of the surface on which it has been deposited even though some Cs occurs at deeper regions. This behavior suggests that the CaO layer, residing 400 A below the surface, plays no direct role in the transmutation process. The study also shows that clusters of deuterons are involved in the reactions with clusters of different sizes interacting with different target nuclei. Energy associated with each of the known transmutation reactions
19
involving deuterons is shown in Table 1. The first reaction has been produced by living cells and will be described in more detail later. Table 1. reaction.
Energy produced by the indicated transmutation
Deuterium D 2D 4D 4D 6D
Target Mn Sr Cs Ba
Product Fe He Mo Pr Sm
Total MeV 15.61 23.84 53.41 50.49 67.61
MeV/D 15.61 11.92 13.35 12.62 11.27
Notice that the energy/deuteron is nearly the same for all reactions. This result suggests that the main source of energy results from destruction of the deuteron. 6. Biological Transmutation Nuclear reaction occurring in living cells is a subject that respectable scientists do not discuss, i.e. until cold fusion came along. Even so, we are encouraged not to mention the subject. However, the field has matured sufficiently to make such information socially acceptable, at least to most adults. About 40 years ago, Kervran in France claimed that analysis of seeds and the resulting plants as well as eggs and the resulting animals showed the creation of more of some elements than were present initially or in the diet. This work was rejected for obvious reasons, not the least of which is the difficulty of analyzing for the elements with sufficient accuracy. This problem was reduced by Komaki in Japan who analyzed various bacteria, yeasts and molds and showed that certain elements missing in the culture were created by the growing cells. Once again, this work was rejected for reasons that included the inability to identify the exact nuclear reaction. This problem has been solved recently by Vysotskii et al. in the Ukraine who showed that Mn can react with D to form Fe. Many years ago Kervran produced the same reaction when normal water (H2O) was used, although a different isotope of Fe resulted. This work shows an unambiguous path for a transmutation reaction as well as its rate. Later studies indicate that the reaction Na 23 + P 3 1 = Fe can also occur in a living cell. Additional studies by Vysotskii et al. and by Coleman et al. are described at this conference. 7. Nuclear-Active-Environment Having seen that living cells are capable of initiating nuclear reactions, what other kinds of environment might have the same effect? Initially solid palladium was thought to host the fusion reaction. Gradually, focus shifted from the entire cathode to the near-surface region, where the D/Pd ratio was highest and where nuclear products were found. Recent work indicates that material deposited on the cathode
20
surface, so called "crud", is the source of the nuclear activity. Palladium does not have to be used at all, although its presence does seem to support nuclear activity. Because this nuclear-activity-environment (NAE) normally forms very slowly, if at all, the LENR effect is slow to form, if at all. Furthermore, the structure and composition of this environment is unknown, therefore difficult to reproduce. This environment has now been created rapidly by co-plating and by deposition of various materials on an inert substrate outside of the F - P cells. 8. Reproducibility Aside from being the basis for believing LENR, reproducibility is required to study the phenomenon as well as to allow its use as an energy source. At the present time, the NAE is created by chance and in small amounts. Study and application require the NAE be identified so that it can be created on purpose and in large amounts. 9. Energy Production Rate Energy is produced only in the NAE. If observed power is compared to the entire sample, as was done in early work, values near 100 W/g of Pd are calculated. If this comparison is based on the amount of deposited material, the value increases to about 1000 W/g. Of course, we cannot expect all of the deposited material to be active. Using an estimated fraction for the active component, power density might go as high as 100,000 W/g. At some value, the rate of energy removal becomes a limitation in order to avoid melting and destroying active sites. Such melting has been observed. Consequently, heat removal rather than heat generation will limit the upper power capacity of such generators. 10. Relation to Other Observations Conventional physics rejects the idea that a nuclear reaction can be influenced by its chemical environment. The energy and time scales are just too different. This was the belief until LENR was observed, where a chemical environment is essential to the nuclear process. Consequently, it is worth asking if similar effects are seen under conditions that are independent of the LENR effect. The answer is yes, other nuclear reactions are in fact affected by their chemical environment. When D+ ions are caused to bombard various metals and compounds, the magnitude of the D(d,p)T fusion reaction is found to be influenced by the target composition. Kasagi et al., and Takahashi et al. (Japan), Czerski et al. and Raiola et al. (Germany), Lipson et al. (US) report seeing this effect, especially as the energy of the bombarding D+ decreases. A number of people have recently reported finding that the decay rate of radioactive nuclei can be altered by their chemical environment. Ohtsuki et al. (Japan) studied 7 Be in C 60 (0.83% decrease in half-life), Vysotskii et al. (Ukraine) and Coleman et al. report at this conference that the half-life can be changed
21
by microbes, and Reifenschweiler (The Netherlands) observed an increase in the half-life of tritium when it was absorbed by finely divided titanium. These claims are so unusual that additional studies are clearly required. Nevertheless, evidence is accumulating that the chemical environment can affect various nuclear reactions. 11. Theory Requirements Absence of a theory has been a benefit to skeptics and a handicap to experiment. Many attempts are underway, most having no hope of success because they ignore experimental facts. I would like to suggest the following list of essential experimental facts that need to be addressed by any successful theory. Explain 4 He production at rates in excess of 1012 events/s. Explain occasional production of tritium up to 104 events/s. Explain transmutation reactions involving up to six deuterons at one time. Explain how energy is coupled to lattice. Explain how energetic particles can form while most energy is coupled to the lattice. (6) Explain the nature of the NAE and why it exists in several kinds of chemical environments.
(1) (2) (3) (4) (5)
12. What We Know To Be True? The field has now matured to the point that many claims can be considered to be true and correct. I suggest these are: • nuclear reactions of nuclei, • nuclear reactions • nuclear reactions • nuclear reactions • nuclear reactions • nuclear reactions
involving 1, 2, 4 and 6 deuterons that add to a variety involve both H and D, occur only in special solid environments (NAE), produce little if any radiation or energetic particles, can occur at rates that make significant heat energy, can be initiated using many different methods.
This list is growing rapidly and continues to challenge all attempts at a consistent explanation. 13. What D o We Hope To Be True? Of course, we all hope this ideal source of energy will replace present energy sources. Energy generated by "cold fusion" is clean, is in essentially unlimited supply, and can be generated on a small scale. These features make it ideal and able to solve some very dangerous consequences of using conventional energy, such as air pollution, global warming, and radioactive contamination. In addition, oil and gas are
22
much too valuable as feed stock for making useful materials to be burned for energy. Jed Rothwell describes other benefits at the conference. On the other hand, this is a very disruptive technology t h a t can cause serious economic consequences if its introduction is not handled properly. As use of conventional energy is phased out, companies and people dependent on the sale of this energy can suffer great loss, leading to conflict and war. It is essential t h a t the process of phasing out conventional energy and phasing in L E N R energy be done with wisdom over sufficient time t o allow the economic system t o adjust. Therefore, we should t h a n k the skeptics for slowing the process and hope they remain effective in allowing the system to adjust without too much pain. All new sources of energy have always been used by some people to more effectively kill other people. A gradual increase in available energy over time has allowed this killing process to become so efficient t h a t we all are now at risk. Because L E N R energy is t h e most concentrated energy source discovered t h u s far, t h e risk has now increased once again. Consequently, while we finally have an energy source t h a t can insure our survival as a species well into the future, we also have a potential source t h a t can more effectively wipe us out. We can only hope t h a t people of wisdom will prevail in spite of recent events to the contrary.
References 1. M.H. Miles and B.F. Bush, Heat and helium measurements in deuterated palladium, Trans. Fusion Technol. 26 (4T), 156 (1994). 2. 2 B.F. Bush and J.J. Lagowski, Methods of generating excess heat with the pons and fleisehmann effect: rigorous and cost effective calorimetry, nuclear products analysis of the cathode and helium analysis, in Proceedings of the Seventh International Conference on Cold Fusion, 1998 (Vancouver, Canada; ENECO Inc., Salt Lake City, UT, USA).
N E W PHYSICAL EFFECTS IN METAL D E U T E R I D E S
PETER L. HAGELSTEIN Massachusetts Institute of Technology, Cambridge, MA, USA MICHAEL C.H. MCKUBRE SRI International, Menlo Park, CA, USA DAVID J. NAGEL The George Washington University, Washington DC, USA TALBOT A. CHUBB Research Systems Inc., Arlington, VA, USA RANDALL J. HERMAN Hekman Industries, LLC, Grand Rapids, MI, USA The experimental evidence for anomalies in metal deuterides, including excess heat and nuclear emissions, suggests the existence of new physical effects. 1. Introduction Following the initial claims of 1989,1'2 the body of research on anomalous effects in metal deuterides has grown to include thousands of papers on a wide spectrum of topics. DoE, to facilitate their review of this set of research, has asked for the preparation of the following summary. The entire body of research is not addressed. Rather, a subset of research from two areas is presented: selected issues associated with excess heat production in deuterated metals, and a brief discussion of some aspects of nuclear emissions from deuterated metals. 2. Excess Heat Effects in Fleischmann—Pons Experiments In the simplest sense, the Fleischmann-Pons experiment is an aqueous electrochemical experiment in which a palladium cathode is loaded with deuterium in a heavy water electrolyte. If the associated conditions are suitable, an excess heat a effect can be observed (e.g., see Fig. 1). In 1989, there developed both interest and concern regarding the measurement of excess energy and the conditions under which a
Excess power is the output power minus the input power as discussed in Appendix A. The time integral of excess power is excess energy, which is observed experimentally as excess heat. 23
24
the excess heat effect could be observed. In the years following the initial announcement, it was easier for most to believe that the effect was due to calorimetric errors than due to new physics. However, excess heat has been observed with a variety of calorimeters based on varying operating principles and by different groups in different labs, all largely with similar results. The hypothesis that the excess heat effect arises only as a consequence of errors in calorimetry was considered, studied, tested, and ultimately rejected. A brief discussion of calorimetric issues is provided in Appendix A (see also a recent more general discussion by Storms 3 ). The conditions under which the excess heat effect occurs remain of interest. Much has been learned since 1989. We consider briefly in what follows some of the factors that have been identified.13 I (A/cm5)'
430
454
478
o PxsD20(W)
+
502 526 550 Time of electrolysis (h)
574
PxsHzO(W)'
598
622
Figure 1. Excess power in Fleischmann-Pons experiments as a function of time in twin cells and calorimeters, driven with a common current, one with heavy water and one with light water.
2.1. Total Excess Energy
Production
The total excess energy produced in the Fleischmann-Pons experiment can greatly exceed what might be expected from chemical effects.1'4 The energy density is b
T h e excess heat effect itself is consistent neither with a conventional D + D fusion reaction mechanism, nor with any other nuclear reaction mechanism that appears in textbooks or in the mainstream nuclear physics literature. The existence of an excess heat effect with no commensurate energetic nuclear products rules out whole classes of potentially relevant reaction mechanisms, but does not provide guidance as to what kind of process is occuring. The observation of 4 He correlated with excess energy, which is discussed later, is suggestive that the reaction mechanism is consistent with D + D —> 4 He, but sheds little light on how such reactions might occur.
25
customarily quoted relative to the total cathode volume,0 corresponding to the conclusion that the excess heat effect has its origin within the metal deuteride based on measurements of cathode temperature rise and the establishment of temperature gradients in electrolytic and gas calorimetric experiments. Gozzi and coworkers reported 5 excess energy production at the level of 130MJ/cm 3 . The SRI group quoted a value of 45 MJ/mol for a measurement in a closed cell flow calorimeter, which is about 450 eV/atom of Pd. 6 There are a great many reports of energy production at this general level, and some at much higher levels as well. 2.2. Excess Heat and
Loading
Early publications by Fleischmann and Pons implied that the phenomenon they were studying was conditioned. From the material then available, it was not easy to deduce a complete set of necessary and sufficient conditions to initiate the excess heat effect. Little effort was made in early replication attempts to measure or report the bulk, interfacial and stimulus conditions employed. By the time of the first International Conference (ICCF1 in 1990), an effort was underway to evaluate systematically the various parameters of the effect. With the development7 and adoption 8 of bulk resistivity and other methods 9 as in situ probes of the Pd cathode composition, it was quickly recognized that the Fleischmann-Pons effect occurred in Pd wire cathodes only when very high average levels of loading (D:Pd atomic ratio) were achieved in the Pd bulk. d Figure 2 shows the measured correlation between thermal power production (in excess of known power input) and D:Pd bulk atomic ratio determined in situ from the measured cathode resistance. The effect appears to increase approximately parabolically above a threshold loading of D/Pd w 0.875. A very similar result with a slightly lower threshold was presented and published simultaneously by Kunimatsu et al.9'10 based on independent experiments carried out at IMRA Japan (Hokkaido). Such high loading is accompanied by high internal pressure, and it is necessary for the cathode to be able to withstand this in Fleischmann-Pons experiments. 11 This loading requirement in the basic Fleischmann-Pons experiment is thought to be a general precondition for the effect in Pd wire cathodes. 6 An analysis of 49 calorimetric results obtained at SRI in 1990 and 1991 showed that in no case was a calorimetric imbalance observed (19 examples) where an electrode failed for c
Whether the excess heat is a surface or bulk effect has not yet been clarified in the FleischmannPons experiment. There exist rather good arguments, which support the hypothesis that the reactions take place near the surface, but this discussion is beyond the scope of this manuscript. In the SRI experiments, an additional requirement was noted, namely that the loading needed to be maintained for several weeks to a month, which was at least 10 times longer than the deuterium diffusional time constant. This is consistent with the experience of other groups. 1 2 This requirement is not an absolute requirement, as there exist experimental results with shorter initiation times for cathodes of other geometry and surface deposited films. e High loading in these room temperature experiments is consistent with the presence of a high deuterium chemical potential, which would allow deuterons to reach higher energy states in the metal deuteride.
26
o C1
0.88
0.89
0.90 ___
0.91
0.92
Parabolic 0.875 555
0.93
0.94
_____ Atom_i_c__rati£_(D/Pd)
0.95
0.96
0.97
0.98
___
Figure 2. Excess power density in W / c m 3 vs. average D / P d atomic ratio measured from the axial resistance for a Johnson Matthey wire cathode 30-cm long and 1-mm diameter in 1.0 M LiOD containing 200 ppm Al.
whatever means to achieve a bulk average D/Pd loading of 0.9. However, all electrodes achieving a loading of 0.95 or greater (15) exhibited a heat excess more than three times the measurement uncertainty [a)1 in many cases many tens of a larger. Example of such heat excess is shown in Figs. 1 and 3. For the cells with cathodes achieving a maximum loading between 0.90 and 0.95, approximately half manifested measurable excess heat and half did not. The equilibrium spacing of deuterons in PdD is greater than in D2, so the proximity of deuterons at high loading alone is not expected to promote an excess heat effect. The pair-wise fusion rate of deuterons in PdD or in other metal deuterides is too small by 10s of orders of magnitude to be observable. 13 The notion that deuterons are somehow being squeezed together, so as to fuse at high loading or high fugacity in these experiments, is not considered a plausible explanation. 2.3. Surface
Chemical
Potential
Fleischmann and Pons recognized the surface chemical potential of deuterium as the variable most critically associated with the effect they were studying. If the bulk and surface are at equilibrium then the surface chemical potential can be inferred from a measurement of the bulk loading. The situation relevant to the Fleischmann-Pons effect, however, often involves inhomogeneous loading and the presence of important deuterium fluxes. Under these conditions a measure of the average composition reflects only the lower limit of the surface chemical potential for a dynamically loading cathode. Electrochemists have long used the reference voltage as a means to measure
27
8
^ref
'cell '
'
Average and error bars
Time of electrolysis (h) Figure 3. Excess power (.Pxs), reference voltage (Vref) and cell electrochemical current (-fCell) a s a function of time (hours) for an Englehard Pd wire cathode 3-cm long and 3 mm in diameter in 1.0 M LiOD containing 200 ppm Al.
a species' chemical potential. 14 Basically, the potential difference is measured between the electrode of interest and another having defined potential (the reference electrode) either in the presence of a steady current or at open circuit. FleischmannPons advocated this method as early as 1990.15 Others have made use of this method as a diagnostic in relation to the excess heat effect. 16-19 Figure 3 plots an early result at SRI where the cell current, reference voltage and excess power were recorded simultaneously. In this case, the reference voltage was measured without interruption of current, and the presence of a finite electrolyte resistance between the cathode and reference electrodes results in voltage offset proportional to current. It is clear, however, that the dynamics of the reference potential more closely correlate with the excess power than with the cell current. Unfortunately, the electrode surface potential is determined by other species in addition to deuterium. The adsorption of Li, for example, is strongly reflected in the potential plotted in Figure 3, and the maintenance of a high potential at near zero excess power at the right of this figure was thought to reflect the presence of a lithium rich, blocking surface film deposited on the cathode surface. The latter ambiguity is removed if the reference potential is measured with current interruption. 18 2.4. Temperature
Dependence
A strong sensitivity of excess heat production on the operating temperature was noted and exploited early on by Fleischmann and Pons, who developed an interesting protocol in which the temperature was allowed to rise following the onset of an
28
excess heat effect.20 The heat was found to increase over the course of a calibration heat pulse, which is attributed to a thermal positive feedback effect.21'22 Others have noted such a temperature effect.23 This basic effect was studied by Storms, 24 and the results expressed in a form consistent with p J
- pn excess
±
U
c
e-EJkBT
?
where Ea is an equivalent activation energy that was found to be about 15 kcal/mol (about 670MeV). f The observed small activation energy is thought to be associated with creating the proper chemical environment and not associated directly with the nuclear process. 2.5. Excess Heat and Current
Density
The identification of the D/Pd loading requirements as necessary criteria did not bring an understanding of the Fleischmann-Pons effect. Moreover, an initiation effect was noted that has nothing to do with D loading, an explanation for which was proposed only recently. Electrochemical current density was initially reported by Fleischmann-Pons as having a threshold effect on excess heat production that is completely independent of its effect on loading,4 and this was later widely studied and confirmed.5.6,10,24,26-31 Evidence of this current threshold behavior can be seen in Fig. 3, and more directly in Fig. 4, which shows calorimetric results from two identical cells, one with D2O and one with H2O, operated electrically in series, while interrogated with the same measurement system. 27 An approximately linear increase in excess power with a threshold of about 265 mA/cm 2 can clearly be seen for the Pd cathode operated in D2O. Data for the H2O cell do not deviate from calorimetric balance; various excursions reflect only transients following changes in input power. In no case was the Fleischmann-Pons effect observed to occur in cells containing H2O as the major component at SRI, and excess heat measured in D2O cells was observed to decrease to zero upon substantive addition of H2O. 2.6. Deuterium
Flux and Triggering
Issues
The excess heat effect is often observed to be stimulated by changes in the experimental conditions. Fleischmann-Pons noticed in their initial work that the excess heat effect was occasionally initiated or improved with the application of a heat pulse, which can be considered as a transient change in conditions within the present argument. At SRI, one of the techniques used with success to initiate a heat pulse was to alter the current density, either through sudden changes or through ramps (as in Fig. 5). Takahashi introduced a protocol in which the current density was alternated between low and high values. 32 ' 33 Bockris described a regimen in which the current periodically changed direction. 34 Yamaguchi described an experiment f
A similar rapid increase in temperature was noted by Case in a gas loading experiment at elevated temperature. The effective activation energy was reported to be 13kcal/mol (about 560MeV). 2 5
29
0.6-
» P14/D 2 0
Linear
o P13/H 2 0
Electrochemical current density (A/crrr) Figure 4. Excess power as a function of current density for Fleischmann-Pons cells with heavy water and with light water.
involving vigorous outgassing of deuterium from a rapidly heated metal deuteride sample. 3 5 - 3 7 The application of an axial current in a wire or cathode can be used to drive a significant deuterium flux against the electronic current. 38 This effect was exploited by Celani and coworkers, 39,40 and by Preparata, 41 who reported excess heat and other effects with a high axial current.
Figure 5. Excess power as a function of time and fitting function for a Johnson Matthey Pd wire cathode 10-cm long and 1mm diameter in 1.0 M LiOD containing 200 ppm Al.
30
Quantitative evidence indicating that deuterium flux plays an important role in determining the excess heat in a Fleischmann-Pons cell was found at SRI. 42 A purely empirical function was found to describe the excess heat observed for 1-mm diameter Pd cathodes. This function, and its fit to experimental data, are shown in Fig. 5. After initiation, excess power was found to be proportional to the product of three terms: (i) the square of the loading above a threshold value (x — XQ)2; (ii) the electrochemical current above a threshold; (iii) the flux of deuterium through the interface, irrespective of direction, measured as the time derivative of the average D loading, \5x/5t\.z Incoming deuterium produces a flux that increases the loading, which should improve things according to the discussion above. But experiments seem to show that deuterium flux makes a difference, independent of whether it is incoming, outgoing, axial, or traversing. 43 One question of interest concerns the functionality of the flux: what is it about the flux that makes a difference? Another interesting question, independent of any understanding of the functionality, is whether the effect of deuterium flux can be augmented or replaced by other kinds of stimulation. This question opens the door to a very much larger discussion that we are not able to pursue here. The general issue of triggering has been of interest since the early 1990s,44 and occupied a central place at recent international conferences. 43-49 3. Helium and Excess Heat Much effort has been devoted to the search for reaction products that could be associated with the excess heat. It soon became clear that there are insufficient chemical reaction products to account for the excess heat by several orders of magnitude. Attention has been directed to the search for nuclear "ash" in amounts commensurate with the energy measured. The problem is more difficult than in the case of chemical reactions as no similar processes are known. Searches for neutrons, tritons, and other energetic emissions in quantitative association with the excess heat effect have uniformly produced null results. 5 The absence of quantitative energetic emissions leads to the conjecture that the new process is somehow converting nuclear energy directly to heat. There have been numerous consequences of this within the field, one of which is that people have historically been motivated to maximize the energy produced in excess heat experiments (and not efficiency19) in the hope of maximizing the reaction products, so that they might be identified. There have been many assays performed on cathodes before and after excess heat production, seeking the presence of new elements or isotope shifts. 50 ~ 52 Although there appears to be evidence that supports the existence of both elemental and isotopic anomalies near the cathode surface in some g
T h e empirical fit in the absence of a flux term had successfully matched much experimental data previously. A cathode exhibited a "breathing mode" during an excess heat burst in which the deuterium loading varied roughly sinusoidally around a high value. The excess heat data in this case was not matched well by the earlier empirical fit. The fit was greatly improved with the inclusion of a new factor proportional to the magnitude of the flux.
31
experiments, it is generally accepted that these anomalies are not the ash associated with the primary excess heat effect. The main focus of attention has been on helium as the primary nuclear reaction product. 53
3.1. Correlation
of Excess Heat and
Helium
Numerous investigators have sought and, in many cases, found 4 He in different environments including in the gas phase, 5 4 _ 6 0 ' 1 0 7 dissolved in the cathode metal, 6 1 " 6 6 and emitted as charged particles. 67 ' 68 If helium were created in the cathode interior, then one might expect to see helium dissolved in the metal. If helium were produced near the surface, then perhaps it would show up in the surrounding gas. The presence of quantitative energetic helium would be expected to produce an associated Bremsstrahlung X-ray emission. However, there is no evidence for such signals in quantitative measure with what might be expected for a primary excess heat mechanism. The first and historically most important experiments were performed by Miles et al., to correlate the helium content of gas produced by electrolysis (D2 or H2, and O2) with the average heat excess during the interval of sampling. Because of the very low 4 He concentration expected and observed (1-10 ppb) extensive precautions were taken to ensure that samples were not substantially contaminated from the large ambient background (5.22 ppm). In an initial series of experiments, later replicated several times, 55 ' 69 eight electrolysis gas samples collected during episodes of excess heat production in two identical cells showed the presence of 4 He whereas six control samples gave no evidence for 4 He. These results were only semi-quantitative, although the statistical significance of these and later results were profound. Because of questions related to the helium permeability of sample vessels and cells, these results were taken simply as suggesting a nuclear origin and mechanism for the Fleischmann-Pons effect. Later work by Miles and Bush using sealed metal vessels, and by McKubre 70 and Gozzi71, confirmed that 4 He is presented to the gas phase above the electrolyte of a cathode demonstrating the Fleischmann-Pons effect.11 Gozzi presented some very striking results, 71 in which bursts of excess energy were time-correlated with bursts of 4 He observed in the gas stream.1 When compared one at a time, the number of helium atoms detected per burst was on the order of what might be expected from 23.8 MeV per D + D reaction, but with a variation between 0.25 and 1.0 of this amount. If the energy production in these experiments is in fact due to a reaction mechanism consistent with D + D —> 4 He + 23.8 MeV, then it seems that some of the helium may enter the gas stream and some remain within the metal. Several important conclusions can be drawn from the studies cited above: h
Issues relating to sampling, leakage, and mass spectrometry are out of the scope of this summary, but are considered in the literature. 'Reasonably prompt 4 He appearing in the gas stream is interpreted by some as supporting the notion of the excess heat effect being a surface effect rather than a volume effect.
32
• The rate of helium production (atoms/s) varies linearly with excess power (see Fig. 6). • The amount of helium observed in the gas stream is generally within a factor of about 2 less than would be expected for a reaction mechanism consistent with D + D —> 4 He. • Helium is partially retained, and dissolved helium is released only slowly to the gas phase for analysis. Recent work at ENEA Frascati also supports these conclusions. 72 ' 73 Excess heat and helium observations consistent with a D + D —> 4 He + 23.8 MeV (heat) reaction mechanism, in a metal deuteride near room temperature, stands in stark contrast to the d(d,7) 4 He reaction known from nuclear physics.
0
1
2
3 4 5 6 Helium increase (ppmV/V)
7
8, I
Figure 6. Excess energy determined by gradient (boxes) and differential (diamonds) calorimetric methods plotted against the increase in 4 He concentration in a metal-sealed helium leak-tight vessel. The experiment was performed by heating palladium on carbon hydrogenation catalyst materials to ~190°C in ~3 atmospheres of D2 gas pressure (see Appendix B).
3.2. Reaction
Q Value
As the loss of deuterium in association with excess heat is not presently observable, and since there are no commensurate energetic reaction products, the argument in support of reaction mechanisms consistent with D + D —> 4 He is indirect. One can measure energy production, and assay for 4 He in the gas stream or the solid, with uncertainties introduced in the reaction energy Q because all of the helium produced may not be accounted for in the measurement. Experiments are prefered in which a total inventory of the helium is made in order to improve the accuracy
33
of the reaction Q value measurement. To this end, we discuss briefly an experiment in which helium was measured in the gas stream, and an additional effort was made to drive the helium out of the metal. The experiment under consideration was performed at SRI, and the excess heat measured is illustrated in Fig. 5. The experiment was performed in a helium leaktight, all-metal and metal gasketed calorimeter. Samples were transferred in metal gas sample flasks to be analyzed for 4 He by the U.S. Bureau of Mines at Amarillo, Texas. 70 The initial value of 4 He was 0.34 ± 0.007 ppmV/V in the D 2 gas used to charge the cell. Figure 7 traces the history of the cell, M4, from four helium samples taken after excess power was observed. The upper solid line is the expectation for helium concentration presuming: (i) an initial value of 0.34ppmV/V; (ii) that 4 He is produced in a reaction which delivers 23.8 MeV of thermal energy to the calorimeter. The first gas sample taken shortly following the second heat burst of Fig. 5 yielded a value of 1.556 ± 0.007ppmV/V 4 He, which is about 62% of its expected value, and consistent with the earlier observations by Miles, Bush and collaborators, 55 and also Gozzi and coworkers.71 A second sample taken about 6 days after the first showed a measurable increase in 4 He content instead of the decrease that would be expected since, to maintain positive cell pressure, the gas taken for the first sample had been replaced with cylinder D 2 containing a lower level of 4 He (0.34 ppm V/V). These findings support earlier observations that helium is released slowly from the palladium after an initial delay.
• [He] ppm' V/V End
He release
Value expected for 23.8 MeV/He
i
2.5
Q Sampled values
Sample 4
1,
or " CD to 1 /
52.0 E
»
CL CL
d.5
V
_„2.07 077 1H±0. 01
Sample 2 and D 2 make-up
Cathode heating and composition cycling
1 1.661 ±009 1.556 ± 007 * T62%~
M• 69%
Sample 1 and D„ make-up
" 1.0
D„ purge and Sample 3
/
• V
a>0.5
I
Background value of [4He] gf 0.34 ± 0.077
Initial value in D„ 0.0> 450
Jw°/<
550
650
750
850
950
1050
1150
1250
1350
1450
Time (h) Figure 7. Results for 4 He measurements associated with the excess heat results presented in Fig. 5, as discussed in the text. The concentration of helium and gas sampling times are indicated by squares, and the fraction of that expected for a 23.8MeV/ 4 He atom by triangles.
34
After making these measurements, an attempt was made to dislodge near surface He either thermally or by D atom motion by subjecting the cathode to a period of compositional cycling, while still sealed in the calorimeter. Square and sine wave modulations of varying period and amplitude were imposed on the DC (negative) potential at the Pd electrode in an attempt to flux deuterium atoms through the interface and thus act to dislodge near-surface adsorbed or absorbed 4 He atoms. At the end of this period, the potential was reversed to withdraw all deuterium atoms from the Pd bulk. No excess heat was observed during the periods of oscillation although calorimetric uncertainties were large due to the strong departures from the steady state that accompanied the pulsing. Gas samples were taken before this procedure, again after purging the cell and refilling with D 2 from the gas bottle with 0.34 ppmV 4 He, and once more after cycling. The latter sample exhibited the highest concentration of 4 He measured in this cell, specifically 2.077 ± O.OlppmV/V. By making a proper mass balance of the helium lost through sampling and purging, and that gained through make-up from the gas bottle, it is possible to assess with defined uncertainty the results of deuterium fluxing in freeing lightly trapped 4 He. The final integral mass balance yielded a value of 104 ± 10% of the expected value if the excess power in Fig. 5 is due to a reaction of the sort D + D -> 4 He + ~ 23.8 MeV (heat). This value remains the most accurately determined in this field (in the sense that contributions from both the gas stream and the metal are included), but it suffers from the criticisms that the numbers of samples were few, and the largest value of 4 He measured was less than 50% of that in air. We note that 4 He has been produced numerous times in excess heat experiments at levels above that of the concentration in air. One example is shown in Fig. 6. This plot illustrates the real-time correlation between excess heat and the growth of 4 He concentration in a metal-sealed, helium leak-tight vessel. The Q value of 31 ± 13 and 32 ± 13 MeV per 4 He atom measured is also consistent with the reaction D + D —> 4 H e + ~ 23.8 MeV (heat). Because of the importance of this result, it is discussed further in Appendix B. 4
4. Excess Heat Beyond the Basic Fleischmann—Pons Experiment The importance of the basic Fleischmann-Pons experiment, as discussed in the previous section, is primarily scientific in the sense that the research provides strong evidence of a new excess heat effect of nuclear origin. In addition, this basic experiment has provided a focus for a significant research effort, and many important aspects of the experiment have been studied, as discussed above. During the past 15 years, numerous variants of this basic experiment have been proposed and executed. In what follows, we examine a subset of such studies. 4.1. Self-Sustaining
Excess Heat
Effect
Excess heat production in the absence of electrical input was first discussed by Fleischmann and Pons at ICCF4. 74,75 It was found that cathodes continued to
35
produce excess heat in some cases after the termination of the electrochemistry in which heat had been produced earlier during "normal" cell operation. This effect has been reported in other experiments, 22 ' 76 ' 78 ' 79 and is often referred to as "heat after death." These observations suggest a possible difference in the conditions required for the initiation of an excess heat effect as compared to the conditions required for sustaining the effect.
4.2. Excess Heat in Other Metal
Deuterides
Excess heat in electrochemical experiments involving metal deuterides other than PdD has been reported in several modified Fleischmann-Pons experiments. Helium production in association with excess heat was studied in palladium alloys by Miles.80 Excess heat has been reported in TiD with a D2O-H2SO4 electrolyte using thermal imaging. 81 Excess heat and other effects were reported from an electrochemical cell with a Ti cathode by Bernardini and coworkers.76 Excess heat observations with Pt cathodes were reported by Dash 52 and by Storms. 82 Platinum does not form a deuteride, and the excess heat in this case is attributed to a surface layer.82
4.3. Indirect
Gas
Loading
Arata and Zhang introduced an interesting experiment in which palladium black is sealed within the interior of a palladium cathode, and the resulting composite (hollow) cathodes structure is electrolyzed.83 Deuterium gas within the interior of the cathode is in equilibrium with the deuterium in the highly loaded cathode, and the palladium black is loaded indirectly. Evidence for excess heat and helium production has been obtained from this kind of experiment. We discuss this further in Appendix C.
5. Nuclear Emissions The first report of emissions consistent with deuteron-deuteron fusion was made by Jones and coworkers in 1989,2 who claimed that low-level neutrons near 2.45 MeV were emitted from electrochemically loaded titanium deuteride. j Since that time, there have been numerous reports of neutron and charged particle emission generally at low emission rates from metal deuterides, which are consistent with a deuterondeuteron fusion reaction mechanism. In what follows, we will discuss some of this work. We note that there is in addition evidence in support of emissions that are clearly not associated with a deuteron-deuteron fusion reaction mechanism. A subset of these observations will be discussed below.
J
Additionally, present on the titanium surface were Pd, Cu, and Li due to deposition from the electrolyte.
36
5.1. The Jones
Experiment
Much effort has been devoted since 1989 to the Jones effect by Jones and coworkers, 84,85 and also by other groups. 3 2 ' 3 3 ' 8 6 - 9 0 Most of the effort has focused on neutron measurements, but there have been observations of charged particles as well.85 Low-level nuclear emissions typically occur in bursts lasting a few seconds to several days, 84 and at lower current density than that discussed above in connection with the excess heat effect (Jones and coworkers reported neutron emission at 20mA/cm 2 ). A distinct burst effect (see Fig. 8) was reported by Wolf in neutron emission from PdD electrochemical experiments. 91 This is reminiscent of a similar burst effect noted for the excess heat in the Fleischmann-Pons experiment. It was noted in the early 1990s that there were considerable similarities between the electrochemical protocols and palladium cathodes used by Wolf in neutron emission experiments, and those used at SRI in excess heat experiments. In discussions between the two groups, it became apparent that the most significant difference between the two experiments was the current density involved. At SRI, excess heat was observed at elevated current densities, with a current threshold in the range of 200-300 mA/cm 2 . At Texas A&M, Wolf increased the current to about 30mA/cm 2 to initiate neutron emission, but found no neutron emission at significantly higher current densities. 92 The low-high current protocol of Takahashi discussed above scans through both regimes, and is associated with both excess heat and neutron 28
Counts our
emission
.c
130 120 110 100 90 80 70 60 50 40 30 20 10 0
-
•^ •
6 mm cells 3-30-90
H
Neutrons open = 1 - 2 . 6 MeV closed = 1 - 5 . 5 MeV
• -
•
f'i
o
Curent density -
:
„ _ J _ _ _ _ _ _ 4 _ _ _ _
10
1
30
20
,
U _
40
50
Time (h)
Figure 8. Neutron burst from PdD loaded electrolytically from the experiments of Wolf and coworkers.
37
5 . 2 . Stimulation
of Nuclear
Emissions
with
Electrical
Current
Cecil and coworkers reported charged particle emission in experiments where current was run through TiD^ [using Ti(662) alloy]. 9 3 For example, a proton signal centered at 2.45 MeV was presented. 15 Jones and coworkers have recently used this same general approach. 9 4 , 9 0 T h e group evacuated a heated chamber containing 25-250 /mi thick Ti foils, introduced 1 atmosphere of D2 gas and partially loaded the foils, which were then placed in front of a particle detector, or in a neutron counter. A low background nuclear detector system was used. Electrical current was run through the foils during nuclear counting. Background subtracted counts were observed for neutrons at typical rates of 40 counts per hour. Background subtracted counts were observed for charged particles identified as < 3 MeV protons at typical rates of 100 counts per hour (and up to 2000 counts per hour), with emission rates varying strongly over t h e course of a few hour burst event. Results from a particularly strong burst are shown in Fig. 9. T h e signal is centered at 2.4 MeV and the particle identity is determined from a comparison with a similar spectrum obtained with a thin Al absorber foil. 94 Background subtracted coincidences between two particles, consistent with protons and tritium from deuteron-deuteron fusion, occur at a rate of one count per hour in foils with no electrical current running. In this case, there is an additional experimental procedure of LiOD and D2SO4 surface t r e a t m e n t and rinsing prior to nuclear counting. In all cases in the recent Jones experiments, excess nuclear counts diminish with time, positive signals are observed greater t h a n 50% of the time, and no excess nuclear counts are observed when H2 is substituted for D2.
5 . 3 . Neutrons
from
Ti Shards
in Deuterium
Gas
3
Neutron emission consistent with d(d,n) He reactions were reported in 1989 from gas-loaded metal deuteride shards with thermal cycling. 9 5 In these experiments the metal is loaded at high pressure and cycled between liquid nitrogen t e m p e r a t u r e and room t e m p e r a t u r e . Neutron emissions appear occasionally in burst e p s i s o d e s . 9 6 - 1 0 0 High efficiency neutron detectors were employed, 9 8 and some of the measurements were performed under conditions where the background was quite low. 9 6 ' 1 0 1 Research along these lines has not continued in recent years. T h e evidence in support of neutron emission from this kind of experiment is strong, but in such experiments the conditions are not well controlled. This, combined with a low associated emission frequency, made other approaches seem more attractive. 9 6
5.4. Relation
between
Neutron
Emission
and Excess
Heat
Effect
We note t h a t the amount of energy associated with these low-level emissions is not observable calorimetrically. W h e t h e r there is a correlation between nuclear emission effects and excess heat or not has been under discussion since 1989. 1 0 3 k
T h e proton from the d(d,p)t reaction initially has 3 MeV, and perhaps some energy degradation occurs if the proton is born inside the metal deuteride.
38
70'
• Plastic 0 Glass
60 50.
4a o
" 3a 2010-
-jlxi
-*t 11
16
21
26
31
36
41
46
JL 51
56
61
UL •N1* 66 71 J
Light output Figure 9. Proton spectrum near 2.4 MeV from T i D x taken over 21 min using a double scintillation detector, as presented by Jones at ICCF10. The two different signals are from two different scintillators (plastic and glass). The light output scale is related to the proton energy.
There have been several observations of excess heat with simultaneous diagnostics for neutron emission, and for x-ray and gamma emission. 5 ' 71 ' 104 An anticorrelation between excess heat and neutrons was reported by Okamoto and coworkers.105 We have noted that excess heat production in the Fleischmann-Pons experiment has an associated current threshold around 200-300 mA/cm 2 , while neutron emission is associated with lower current densities (around 30 mA/cm 2 in the experiments of Wolf, Jones, and coworkers cited above), suggesting that the different effects have different operating regimes. In experiments that operate with both high and low-current densities, there are reports of both neutron emission and excess heat production. 106 ' 107 There is a study with the low-high current protocol in which a correlation is reported where cathodes producing the largest excess heat effect also show the largest neutron emission.108 5.5. Nuclear Fusion
Emissions
not Attributable
to
Deuteron-Deuteron
There are several reports for weak nuclear emissions, which clearly are not associated with a deuteron-deuteron fusion mechanism. In 1990, Cecil and coworkers noted the presence of very energetic charged particles from thin TiD foils up to and beyond 10MeV 93 (see also the PhD thesis of Liu 109 ). Energetic alphas around 15 MeV have been observed by Lipson and coworkers from PdD. 1 1 0 Both alphas and protons near 14 MeV have been seen in experiments with TiD. 111 The appearance of such signals under conditions that are similar to those associated with excess heat
39
production and low-level deuteron-deuteron fusion is significant, and provides additional information that may be helpful in understanding the underlying physical processes responsible for the new effects. 5.6. Broad Proton
and Alpha Spectrum
from Deuterons
on
TiDx
Kasagi and coworkers have reported anomalous results from beam experiments using TiDj, targets in which product nuclei are observed with a very large energy spread. 112 This group bombarded TiD^ (a; > 1.2) foils with 90-150 keV deuterons and observed protons with energies from 6 to 17MeV and alphas with energies from 4.5 to 6.5 MeV at scattering angles between 135° and 155° at a rate of 10~ 6 of the deuteron-deuteron fusion rate. An aluminum absorber foil in front of the particle detector stopped the elastically scattered beam. The energy spectra for the protons and alphas are consistent with a three-body reaction mechanism d + d + d ->• 4 He + p + n,
Q = 21.62 MeV (three body)
Hubler and coworkers at the Naval Research Laboratory have partially confirmed the existence of this anomaly in that the protons have been observed in some, but not all, of the samples bombarded. A coincidence experiment between the proton and alpha would be required to confirm this reaction. The experiment is important, and thought by some to be related to other experiments that show anomalies in metal deuterides. It could be interpreted as a probe of the probability that two deuterons are close together in the solid when the bombarding deuteron encounters them. There is no viable conventional explanation for the existence of this nuclear signal. 6. Conclusions The research discussed in this paper provides evidence for effects in three categories: (1) The existence of a physical effect that produces heat in metal deuterides. The heat is measured in quantities greatly exceeding all known chemical processes and the results are many times in excess of determined errors using several kinds of apparatus. In addition, the observations have been reproduced, can be reproduced at will when the proper conditions are obtained, and show the same patterns of behavior. Furthermore, many of the reasons for failure to reproduce the heat effect have been discovered. (2) The production of 4 He as an ash associated with this excess heat, in amounts commensurate with a reaction mechanism consistent with D + D -> 4 He + 23.8MeV (heat). (3) A physical effect that results in the emission of: (a) energetic particles consistent with d(d,n) 3 He and d(d,p)t fusion reactions, and (b) energetic alphas and protons with energies in excess of 10 MeV, and other emissions not consistent with deuteron-deuteron reactions.
40
Experimental results for tritium production were noted, and anomalous results from deuteron beam experiments on TiD^ were discussed briefly. In each case, the effects cannot be accounted for by known nuclear or solid-state physics. The underlying processes that produce these results are not manifestly evident from experiment. The scientific questions posed by these experiments are, in the opinion of the authors, both worthy and capable of resolution by a dedicated program of scientific research.
Appendix A: Calorimetric Issues As enumerated by Storms, 30 four questions must be addressed when evaluating the state of heat observations: (1) Was the calorimetric technique used by Fleischmann and Pons sufficiently stable and accurate to see the claimed extra energy? (2) Have others independently replicated the claims using stable and accurate calorimeters? (3) Can prosaic sources of chemical energy or energy storage effects be ruled out? (4) Have reasons for success or failure been discovered? A clear, positive answer to the first question was available in massive detail 114 but only retrospectively. Fleischmann and Pons used an open cell from which energy was lost in a variety of ways, including by infrared radiation, and as chemical energy carried with the evolving gases. The resulting differential equation was awkward and subject to misunderstanding. Fleischmann addressed the mathematical issues to the point where the isoperibolic method used can be seen to have accuracy better than 1% (Fleischmann's estimate is 0.1%). With daily automatic calibration, the Fleischmann-Pons calorimetric method was able to establish and assure stability for the length of time (months) needed to perform their experiments. Because the cell was open to escaping gases, attention was also given to the possibility that an unknown and variable fraction of the evolving D 2 and O2 gas may recombine to D 2 0 within the calorimetric envelope. A reduction of this subtractive term would give rise to the appearance of "excess heat" when in reality it simply had a chemical origin. Quantification of the upper bound of this effect was made by Fleischmann and Pons, 115 by Jones et al.n6 and in final detail by Will. 117 With 15 years of hindsight, it is now clear that the initial heat claims of Fleischmann-Pons must be taken at face value as quantitatively sound and capable of standing alone. Fortunately, this last is not necessary. Hundreds, possibly thousands, of attempts were made to replicate the Fleischmann-Pons effect. Apart from those conducted in 1989, when little was understood about necessary conditions, most researchers who attempted to reproduce the effect claimed success. We do not attempt to evaluate the bulk of these experiments or claims, although readers are invited to do so and could benefit in this regard by starting with the reviews by Storms. 113
41
To address the second question above, we provide an example. Flow calorimetry with closed cells was selected at SRI at the outset in part to avoid ongoing criticisms of the Fleischmann-Pons (Fick's law) method. Electrochemical cells were operated thermodynamically closed, sealed, and immersed in the fluid flow. Rather than measuring heat flow as a temperature difference across a defined (and presumed stable) barrier, the emerging heat in the SRI experiments was measured as the temperature rise in a moving liquid mass that surrounded the cell. In this way, the governing equations become trivial: all considerations of heat source dependence and so-called "recombination" effects can be avoided in simple first principles operation. Where potential sources of error were anticipated or recognized, the calorimetric system was designed to yield conservative estimates. Over 50,000 h of calorimetry to investigate the Fleischmann-Pons effect have been performed to date at SRI, most of it in calorimeters identical or very similar to that shown in Fig. 10. Water
Inlet RTDs
- Hermetic 16-pin connector
Water in
Acrylic top piece Gasket
Gas tube exit to gas-handling manifold
Water outlet containing "veptun migine tube and outlet RTDs
Gas tube containing catheter"
Acrylic flow separator Catalyst RTD
Hermetic 10-pin connector Stainless steel dewar Gasket PTFE plate Quartz cell body - *' PTFE liner -
, Screws Recombination -• catalyst in Pt wire basket - PTFE spray seperator cone PTFE ring
-
— Quartz anode cage
Pd cathode Brass heater support and pins
_,,
Acrylic flow restrictor
-"
Stainless steel outer casing
'
Heater "
Pt wire anode PTFE ring
' * Locating pin
:
Figure 10.
Stand
SRI mass flow calorimeter.
The object in Fig. 10 is immersed in a constant temperature bath (typically held constant and uniform to within 3-mK long term and short term). The bath is situated in a constant temperature room (±1K). Calorimetric fluid is drawn from the environing bath, past two inlet temperature sensors (100 f2 platinum resistance
42
temperature sensor RTDs) through the flow labyrinth and past the cell under interrogation, which is encased in a brass fin structure for better and more uniform communication of heat. The fluid flow is then drawn upwards and constrained by the hemispherical top to flow through a small hole and labyrinth, past and closely proximate to two outlet RTDs. Additional sensors of other types have been used to further assure accurate values of the measured temperature rise. The fluid is then drawn through a heat exchanger to the inlet of a constant volume displacement pump, and then delivered directly to an electronic balance. The balance is polled by computer to determine the fluid mass flow rate as AM/At. In high power experiments requiring higher fluid flow rates, rotameter flow sensors were used in series with the mass flow measurement. Calorimetry at SRI normally employed an electrical Joule heater either inside the cell or wound tightly on the cell circumference, constrained by the radial brass heat fins. This heater is used to calibrate the thermal efficiency of the convective heat flow process, and to allow for constant power operation in the presence of a variable electrochemical heat input. The equation of the calorimeter is thus: Pin = (-fV)Electrochem + (-f^)joule = Constant, /
AM
Pont = [CP^f -* xs = -'out
\ + k)
(Tout - Tin),
*in-
In most experiments and all discussed here, the fluid was air-saturated H 2 0 for which the heat capacity, Cp, is well known. Current, voltage, and temperature sensors, and measurement instrumentation including the mass balance, were calibrated independently of the calorimeter. The only term requiring in situ calibration is the conductive loss term k, which is the coefficient sum of all heat that leaves the calorimeter by means (primarily conductive) other than with the fluid flow. This term is small. By careful insulation, controlled geometry and selection of the fluid flow rate, k was typically less than 1% of C p (AM/At). Since k is defined by geometry, it is also very unlikely to change and was observed to be stable. Using these precautions the calorimetric method developed at SRI was shown by calculation and experiment 27 to have an absolute accuracy between ±0.35% and 0.5% depending on input conditions. It is worth noting that this accuracy is actually worse than that calculated by Fleischmann 114 for the Fleischmann-Pons isoperibolic method when fully implemented. It is important to further note that the calorimetric methods are very different, the absolute accuracies comparable, and the results obtained consistent. Several results have already been presented (Figs. 1-5) to give a sense of the calorimeter signal-to-error ratio in heat-producing experiments. Below we summarize the findings and results from the major SRI effort to confirm (or refute) the existence of the Fleischmann-Pons effect. (1) Sustained excess heat effects were observed from Pd electrodes undergoing
43
(2) (3)
(4) (5) (6)
(7)
(8)
(9)
electrolysis on more than 50 occasions with confidence more than three times the measurement uncertainty (3a). Bursts or episodes of excess heat generation lasted from periods of several hours to more than a week. During a burst, the excess power was typically between 3 and 30% of the total electrical input power, with the largest sustained observation being in excess of 340%. The intensity of this effect was in the range 3-300 W/cm 3 . Sustained heat bursts exhibit an integrated energy at least ten times greater than the sum of all conceivable chemical reactions within the closed cell. When normalized to the number of cathode Pd (or D) atoms, the energy yield is of order 100-1000 eV/atom, with the largest observed yield 2076 eV/Pd atom. Endothermic effects were not observed. Calorimeters maintained a tight thermal balance at times when excess power was not being observed. During these intervals, calibration checks could be performed conveniently and reliably by adjusting the level of the complementary Joule heater to increase and decrease the system total input and output power. Except for the expected transient responses, the calorimeters were never observed to exhibit output heat power lower than input. Excess heat effects were observed to occur with D2O but not H2O electrolytes, under similar or more extreme conditions of loading, input power and current density. After an appreciable initiation or incubation time, heat generation appeared to be correlated to three variables: D/Pd loading above a threshold; electrochemical current stimulus above a threshold; and deuterium flux or other dynamic stimulus.
With these results of a clear enthalpic excess unaccountable by known chemical or physicochemical means, it was determined at SRI and elsewhere to undertake a thorough and systematic evaluation of possible nuclear processes, by careful screening of potential products. 1 At SRI alone, serious efforts were made to interrogate active electrochemical and gas loading cells118 for neutrons, X-rays, 7-rays, charged particles, beta and other charge emission, tritium, 3 He and 4 He. In over a decade of effort, evidence for all of these potential products was observed, except neutrons. Of the products observed, only 3 H, 3 He, and 4 He could in any way be correlated, quantitatively or temporally, with the enthalpy production rates.
This is a matter of considerable importance and perhaps some confusion. Many claims for nuclear reaction products exist in the field now more broadly termed "low-energy nuclear reactions" or LENR.
44
Appendix B: Results for the Case Experiment at SRI In 1998, Case reported results from an experimental technique that offered potential advantages over electrochemical Fleischmann-Pons experiments. 54 He exposed commercial supported platinum group metal (PGM) hydrogenation catalyst materials to hydrogen or deuterium gas at slightly elevated pressure (1-3 atm) and temperature (150-300°C) in sealed metal vessels. In some cases, temperature sensed in a thermowell situated in the catalyst bed was higher by an amount sometimes exceeding 10°C under two different conditions: during heat bursts in D 2 ; and in D 2 relative to H 2 at the same pressure. The difference in thermal conductivity between the gaseous isotopes does not appear to contribute appreciably to the observed temperature difference. The primary heat loss pathway does not significantly involve gas phase conduction. Furthermore, a temperature difference for the same heater power is observed only in unusual circumstances. Having surveyed a very extensive range of supported PGM catalysts, Case concluded that the effect: (1) Could be observed with carbon supported catalysts but not with nonconductive supports. (2) Was exhibited with all PGMs (Pd, Pt, Ir, and Rh) except Ru, which had not been well studied at the time of publication. (3) Occurred optimally in a narrow range of catalyst loading (0.5-1%); at higher and lower loading the magnitude of the effect diminished and disappeared. (4) Occurs in a narrow range of temperature, about 130-300°C, with activity peaking at ~50°C. (5) Was destroyed irreversibly when the catalyst was heated to temperatures much greater than 300° C. Case concluded that his results represented evidence of a nuclear process because the energy production estimated from his calorimetry was much greater than could be accounted for from chemical processes. In addition, one post-test gas sample was reported to contain approximately lOOppm V/V of 4 He in a 1 atm sample of D 2 . The elements of simplicity, small materials inventory, rapid initiation, clear thermal signature and possible quantitative nuclear signature inspired many to attempt replication of what became known as the Case effect. Some succeeded in repeating the isotopic temperature disparity, although it quickly became clear that the experiment was far more demanding than it first seemed.™ An effort was made at SRI to reproduce the Case experiment. Initial attempts to reproduce the effect with catalyst materials supplied by Case and in metal sealed m
O n e study by Clarke 1 1 9 did not measure any significant increase in helium levels in a mass spectrometer where levels much smaller than lOOppmV/V would have been easily recognized. Clarke, however, did not observe the procedures described by Case, 5 4 which were in any case incomplete. Neither was Clarke able to measure any temperature effects and his geometry, which consisted of milligram single samples of "Case-type" catalyst confined with D 2 or H2 in very small sealed P b pipe sections, differed greatly from that used and recommended by Case.
45
vessels somewhat smaller than those employed by Case failed to observe systematic temperature differences between H 2 and D 2 . Samples of gas withdrawn from H 2 and D 2 cells did not show an increase in 4 He when submitted to an on-line, highresolution and high-sensitivity Extrel C-50 Quadrupole Mass Spectrometer. Two clear results of this first phase of activity were: (1) The Case effect, whatever its cause, is not normally or always present in catalyst samples, even those certified by Case as being "active." (2) He is not a natural or normal component of these catalyst materials. Significantly different results were obtained in a second campaign after a visit by Case to SRI to demonstrate his experimental procedures. Experiments were performed in pairs in nominally identical 50 cm 3 Nupro stainless steel sample flasks modified by the e-beam welded addition of a 1/8" stainless steel thermowell and a 1 in. Cajon VCR fitting to permit admission of catalyst. An amount of 10 g samples of catalyst were loaded into the vessels, which were then mounted and supported as shown in Fig. 11.
Figure 11.
Configuration of the Case experiment at SRI.
46
A heating element 1-mm diameter and 117-cm long was wound helically on the circumference of the bottom third of the cells and temperature was maintained by supplying power from a computer controlled DC supply. The two cells were mounted axially in 11, 10 cm inside diameter stainless steel dewars, surrounded by granular insulation to maintain their geometry and impose a consistent thermal environment. A significant change in this second phase of activity was to expose just the top of the sample cells to ensure an axial heat flow; this was found to be important both for calorimetry and to recreate the Case effect. During the course of the experiment, the currents to and voltages across each heating element were monitored together with two thermocouples measuring temperatures in the thermowell of each cell, and an ambient temperature sensor. Typically, experiments were operated in pairs, with one blank and one test cell, with the heater power set to keep the catalyst bed temperatures at nearly equal values. Test cells contained Case-certified 0.4-0.5% Pd on C catalyst in D2. Blank cells contained samples of identical catalyst in H 2 or inactivated or non-catalyst carbon in D 2 . After hydrogen treatments and evacuation to clean the catalyst surfaces, cells were then subjected to an extended period "soak" in H 2 to ensure by measurement that they were 4 He leak-tight and that any labile 4 He sources adsorbed or absorbed on the cell inner surface or catalyst volume had been exhausted. This period was also used to establish a reference temperature. Cells were then charged with D 2 or recharged with H 2 to the reference pressure, and their heat flow and helium levels monitored. Experiments exhibited a range of behaviors. Figure 12 summarizes 6 of 16 results of helium measurements in paired cells; these fall into three classes of behaviors: (1) Cells that show no increase of 4 He over long periods of time (including all cells operated with H 2 ). (2) Cells that exhibit a slow, approximately exponential increase in [4He] with time, following a trajectory very different from that expected for convective or diffusional leakage in from the ambient. (3) Cells that display no measurable increase in [4He] for a period of several days, followed by a rapid, approximately linear rise in [4He] to levels sometimes exceeding that of the ambient background. Using data from temperature sensors situated in the catalyst and gas phases it was possible to make heat flow estimates in one of two ways: (1) Gradient method, based on the relationship between the temperature difference between the catalyst bed and confined gas, and the heater input power. (2) Differential method, based on the temperature differences between active and the reference catalyst bed sensors and room temperature, as a function of the relative input heater powers. The energy estimated in excess of that provided by the heater for these two calori-
47
metric methods is plotted in Fig. 13, together with the measured helium concentration during the time of greatest derivative, d[4He]/dt in experiment SC2. Excess heat and the apparent increase in [4He] seem to be temporally correlated.
Figure 12.
Results of 4 He measurements from the Case experiment at SRI.
In an attempt to establish a quantitative correlation, Fig. 6 plots the two calorimetric estimates of excess heat production interpolated from Fig. 13, vs. the measured increase in [4He] (the value plotted in Fig. 13 minus the 4 He initially present in the D2 gas). Regression lines through these data incorporating the origin have slopes: Q = 31 ± 13 and 32 ± 13 MeV per 4 He atom, respectively, for the gradient and differential calorimetric methods. The Q value of ~23.8 MeV expected for reaction mechanisms consistent with D + D —• 4 He falls with the assigned uncertainties. The apparent shortfall of 4 He may occur for the same reasons observed in electrolytic Fleischmann-Pons studies discussed in Sections 3.1 and 3.2. In that case the residual helium putatively formed in a new nuclear process is released from the metal only slowly to the gas phase for analysis. Another factor must also be considered in accounting for the 4 He mass balance. In Fig. 12 for experiments SC2 and SC4.2 (D 2 on United Catalysts G75D and E, corresponding to 0.4 and 0.5% Pd on C, respectively), the final trajectories of 4 He with time show essentially the same linear decreasing trend. It is apparent the 4 He is either leaving the cell, in which case it may enter if the partial pressure of 4 He is lower inside than the ambient 5.22ppmV/V, or else 4 He is being adsorbed or absorbed onto or into the stainless steel or catalyst solid components, in which case these must be considered as potential sources of the observed increase. The first is unlikely since the cells were demonstrated repeatedly to be helium
48
—«— ppm V SC2 — — 3-Line fit for 4Jde. —o— Differential ---a... Gradient
> Q. CM
5
o E 3
"ai 3 X
40 20 10 Time (days)
Figure 13. at SRI.
0 20
Excess energy and helium production as a function of time from the Case experiment
leak-tight. An experiment performed to test the second hypothesis demonstrated clearly that 4 He adsorbs or absorbs into this class of catalyst material and also into or onto activated charcoal of similar geometry, with a rate consistent with the declining trend in Fig. 12, at similarly elevated temperatures. There is reasonable confidence that the 4 He source of the rising trends in Figs. 12 and 13 is not a release of stored 4 He from the catalyst for the following reasons: (1) A helium storage mechanism is expected to be reversible. A rate such as that shown in Fig. 12 should manifest itself clearly in the 5-day hydrogen pre-soak intended to address this concern (among others) before experiment initiation. (2) The rate of helium sequestration in carbon and carbon catalyst materials, at room temperatures, appears to be negligible. (3) Multiple random samples of catalyst were subjected to direct assay for 4 He by heating to temperatures in excess of 2250 K in the mass spectrometers of Clarke 120 and Arata and Zhang. In all cases these experiments demonstrated that the volume of 4 He contained with Pd on C catalyst materials was less than that in an equivalent volume of air. We conclude, tentatively, that helium is produced in a process that involves deuterium, but not hydrogen, which evolves heat commensurate with a nuclear mechanism consistent with a D + D - t 4 He reaction. Even taking account of the rate of helium re-ad/absorption, the mean value of the 4 He falls below that expected (assuming 23.8 MeV reaction energy) from the measured heat evolution. These observations regarding released 4 He are consistent with those made in studying
49
electrolytic Fleischmann-Pons cells. Calculating the excess power density normalized to the volume of Pd for Cell SC2, we obtain a maximum value of -~50 W/cm 3 , also consistent with the values observed in electrolytic loading of Pd. Further attempts to replicate the Case effect and the above-described results are underway at ENEA Frascati. Appendix C: The Arata and Zhang Effort Arata and Zhang have been major contributors to the research area under discussion. Dr. Arata came from the plasma fusion community. He and his colleague Dr. Yue-Chang Zhang began working as a team on cold fusion in about 1989. Their researches have been carried out in cooperation with other material scientists, including H. Fujita, who gave the Honda Memorial Lecture on atom clusters in 1994. In the early 1990s their researches led them to develop the DS (Double Structure) cathode, which is a Pd bottle whose "outer structure" is the wall of a Pd bottle and whose "inner structure" is filled with Pd-black. In 1994, they published observations of excess heat using open-cell DS-cathodes 83 and water-flow Dewar calorimetry similar to that described in Appendix A. In a continuous 3-month run Arata and Zhang observed excess heat power averaging about 15 W. Data from another run shows a heat balance for about 11 days, followed by 12 days with excess heat power averaging ~80W, with the output heat ~1.8 times input energy. An initiation time with no excess heat effect was seen in these, and in all other experiments with DS cathodes. Two additional 100-day runs exhibiting continuous excess heat of about 10W were published in 1995. 121 Three additional runs showing ~10-20W excess heat were published in 1996. 122 , 123 One of these runs continuously produced excess heat for 6 months. In another run, a mechanical pressure gauge was fitted to the DS cathode and measured the gas pressure inside the Pd bottle. During much of the run, the pressure gauge pinned at 800 bar. Excess heat power was much reduced when the pressure was less than 200 bar. Excess heat studies continued through 2002. An especially important result is presented in a more recent publication. 124 In this run, the inner cathode consisted of metal powder derived from an oxidized ZrgsPdas alloy, showing that powders other than Pd-black can produce excess heat. In 1998, a pair of DS cathodes were run in series, with one DS cathode in D2O electrolyte and the other in H 2 0 electrolyte. The DS cathode in D 2 0 electrolyte showed excess heat rising to 20 W, while the one in H2O electrolyte showed no excess heat. 125
Replication
Effort at SRI
A pair of DS cathodes prepared by Arata and Zhang were operated at SRI under conditions closely similar to those employed in Japan. Two nominally identical cells were exercised cathodically within intentionally similar cells, one in 0.3 M LiOD and the other in 0.3 M LiOH. Calorimetric accuracy was less than that normally present in the SRI Mass Flow Calorimeters because of the need to operate at very high input
50
power levels to exceed the threshold current density on large area cathodes. It was also not possible to submerge the Arata-Zhang cell completely in the constant temperature bath. Nevertheless, the results obtained at SRI 118 confirm the excess heat results published earlier by Arata and Zhang. In the same range of input powers, the heavy water cell clearly yielded more output heat than the light water cell when operated simultaneously and monitored with the same instruments. The maximum excess power observed in D 2 0 was 9.9 ± 1.3% of the measured power input, with the average value being approximately half the maximum. The measured excess power exceeded the experimental uncertainty (1-2% depending on conditions) for a period of ~86 days to produce an integrated energy excess of 64 ± 6 MJ for the D 2 0 cell. For the H 2 0 cell in the same period of time, the measured energy excess was - 1 ± 6 M J . At the conclusion of the experiment, both cathodes were removed and placed successively in a sealed chamber where they were punctured mechanically, and the gas contents of the cathode void volumes extracted for analysis. The Pd black powders also were removed and the Pd metal walls of the hollow cathodes were sectioned for 3 He and 4 He analysis. Significant amounts of tritium and 3 He (from the decay of tritium) were found inside the interior of the DS cathode electrolyzed in heavy water. Small amounts of 4 He were attributed to atmospheric contamination. Detailed results and conclusions from this work 126 and the results of later analyses are summarized here:
(1) Production of tritium was between 2 and 5 xlO 1 5 atoms. (2) Assuming that the 3 He is from tritium decay, independent determinations of both quantities allows for a determination of when the tritium was generated. Modeled as a single event, the generation of tritium computed from the measured yields occurred during the period of cathodic electrolysis. (3) There is definite evidence of excess 3 He from tritium decay in all samples of gas, Pd bulk metal and Pd black from the D 2 0 experiment. (4) Samples of Pd taken from a similar and contemporaneous electrode run with H 2 0 show low 3 He levels consistent with blank Pd. (5) Measurements of the 3 He gradient through the 3.5 mm wall of the D 2 0 cathode show that the 3 He is the decay product of tritium, which diffused from a source inside the electrode void volume (see Fig. 14). (6) A ~30% increase in tritium levels in the D 2 0 electrolyte measured by liquid scintillation methods is quantitatively consistent with the integral flux of tritium departing the cathode void and registered in the cathode walls. (7) The total inventory of tritium in the initial electrolyte and its increase, while substantial, represents only 0.05% of the total tritium mass balance following the experiment. (8) No evidence was found for 4 He in the interior gas (in the hollow within the cathode) or in the metal that was quantitatively consistent with the measured excess heat.
51
0.4 0.5 Radial position (cm) Figure 14. The 3 H e profile as a function of radius observed in an Arata-type, double structured cathode experiment at SRI.
The results of gas, metal and electrolyte phase 3 He and tritium analyses compel the conclusion that tritium was sourced in, on or adjacent to the Pd black in the void of the D2O double-structure cathode. While neither sought nor expected, this result provides sufficient evidence of the formation of a wholly nuclear product in an essentially electrochemical experiment to merit further study. Of concern, however, is the apparent absence of 4 He. Excess Heat and
Helium
Having convinced themselves that non-chemical heat production within DS cathodes is a real phenomenon, Arata and Zhang sought to identify helium nuclear products using quadrupole mass spectroscopy. They constructed a welded stainless steel manifold vacuum system evacuated with clean turbo pumps. They also built a small furnace system for outgassing metal powder test samples, and later developed a protocol using a Ti getter pump for removing chemically reactive gases from test volumes of desorbed gas. The manifold system included two dedicated mass spectrometers: one normally used to repeatedly scan the mass-4 peak structure, and the other to repeatedly scan the mass-3 peak structure. The initial analysis program was restricted to a study of desorbed gases from furnace-heated, as received and post-run Pd-black. The quadrupole instruments were very clean and had moderate mass resolution. Arata and Zhang routinely observed the 4 H e + peak resolved from the D^" peak. 123 The gas desorption studies 127 provided compositional analysis of both strongly bound gases (released at T > 1000° C) and less strongly bound gases (released at T < 800° C). They repeatedly demonstrated that post-run Pd powder al-
52
ways showed easily measurable 4 He+ peaks, whereas as-received Pd powder showed no detectable 4 H e + peaks. In 1998, they detected 3 He+ within a resolved mass3 peak structure. They found that they could often measure 3 He even when the mass-3 peak was not resolved. The 3 He + fraction could be distinguished from the HD + fraction by measuring the peak height as a function of ion source voltage. 128 The helium signal always made its appearance at a higher voltage due to its higher ionization potential. In 1999, following the experiment at SRI 118 and post-test sampling 126 described above, Arata and Zhang expanded their studies to include analysis of intergranular and ullage gas from the interior volume of one of their DS cathodes. They added an aliquot sampling volume to their manifold and built an assembly for piercing the DS cathode and for collecting gas samples. They used their system to collect both prompt release gas samples from the room temperature DS-cathode and slow release gas samples from the moderately heated DS-cathode. The helium signals were strong and clean. Measurements corresponded to a total 4 He production ~0.05% of that required to explain the run-integrated excess heat measured for the test cathode. 129 Whether 0.05% as observed in Osaka or 0.00% observed in similar experiments performed at SRI, the discrepancy relative to the integrated excess heat is large, and this difference has not been resolved. Possible explanations are: (1) The measurement of heat in both laboratories was substantially in error and no 4 He should be expected. The heat associated with the generation of tritium (measured as 3 He by Arata and Zhang) would be unmeasurable in either calorimeter. (2) Heat was produced in the cathode void by nuclear reaction of D, but the bulk of product helium was lost before sample collection due to micro-fractures, which occur in surface-stressed Pd, as described by Farkas. 130 (3) Heat was produced as in Fleischmann and Pons electrolytic cells at the cathode outer surface where loading, deuterium chemical potential, and stimulation are the greatest. The helium produced was only tenuously attached to the Pd surface and vented to the atmosphere in the Arata Zhang electrolytic cells, which are helium permeable." In this case, one must ascribe a secondary, not primary purpose for the cathode void and its enclosed Pd black, which conflicts with the hypothesis of Arata and Zhang. This is an important question that will be resolved as a result of continued experimentation underway at Osaka University, SRI, and ENEA Frascati.
References 1. M. Fleischmann, S. P o n s , a n d M. Hawkins, J. Electroanal. Chem. 2 0 1 , 301 (1989); Errata 2 6 3 , 187 (1990). See also M. Fleischmann, S. P o n s , M . W . Anderson, L.J. Li, n
I n other words, helium from the outer surface is not collected and measured in these experiments.
53 and M. Hawkins, J. Electroanal. Chem. 287, 293 (1990). 2. S.E. Jones, E.P. Palmer, J.B. Czirr, D.L. Decker, G.L. Jensen, J.M. Thorne, S.F. Taylor, and J. Rafelski, Observation of cold nuclear fusion in condensed matter, Nature 338, 737 (1989). 3. E. Storms, Calorimetry 101 for cold fusion: methods, problems and errors, http://www.lenr-canr.org/acrobat/StormsEcalorimetr.pdf 4. S. Pons and M. Fleischmann, in Proceedings of the ICCF1, 1990, p. 1. 5. D. Gozzi, P.L. Cignini, M. Tomellini, S. Frullani, F. Garibaldi, F. Ghio, M. Jodice, and G.M. Urciuoli, in Proceedings of the ICCF2, 1991, p. 21. 6. M.C.H. McKubre, R. Rocha-Filho, S.I. Smedley, F.L. Tanzella, S. Crouch-Baker, T.O. Passell, and J. Santucci, in Proceedings of the ICCF2, 1991, p. 419. 7. D. Macdonald, M.C.H. McKubre, A.C. Scott, and P.R. Wentrcek, I EC Fundam. 20, 290 (1981). 8. M.C.H. McKubre, R.C. Rocha-Filho, S.I. Smedley, and F.L. Tanzella, Calorimetry and electrochemistry in the D / P d System, in Proceedings of the ICCF1, 1990, p. 20. 9. K. Kunimatsu, N. Hasegawa, A. Kabota, N. Imai, N. Ishikawa, H. Akita, and Y. Tsuchida, Deuterium loading ratio and excess heat generation during electrolysis of heavy water by a palladium cathode in a closed cell using a partially immersed fuel cell anode, in Proceedings of the ICCF3, p. 31 (1992). 10. N. Hasegawa, N. Hayakawa, Y. Tsuchida, Y. Yamamoto, and K. Kunimatsu, Proc. ICCF4 1, 3-1 (1993). 11. M.C.H. McKubre and F. Tanzella, inProceedings of the ICCF7, p. 230 (1998). 12. L. Bertalot, L. Bettinali, F. DeMarco, V. Violante, P. De Logu, T. Dikonimos Makris, and A. La Barbera, inProceedings of the ICCF2, p. 3 (1991). 13. S.E. Koonin and M. Nauenberg, Cold fusion in isotopic hydrogen molecules, Nature 339, 690 (1989). 14. J.O'.M. Bockris and A.K.N. Reddy, Modern electrochemistry; an introduction to an interdisciplinary area, New York, Plenum Press (1970). 15. S. Pons, M. Fleischmann, C.T. Walling, J.P. Simons, international PCT Patent Application PCT/US90/01328, International Patent number WO 90/10935 (1990). 16. L. Bertalot, A. DeNinno, F. DeMarco, A. La Barber, F. Scaramuzzi, V. Violante, Excess power production in electrolysis experiments and ENEA Frascati, inProceedings of the ICCF5, p. 34 (1995). 17. E. Storms, inProceedings of the ICCF6, p. 105 (1996). 18. E. Storms, Relationship between open-circuit-voltage and heat production in a PonsFleischmann cell, inProceedings of the ICCF7, p. 356 (1998). 19. M. Swartz and G. Verner, Excess heat from low-electrical conductivity heavy water spiral-wound P d / D 2 0 / P t and Pd/D20-PdCl2/Pt Devices, inProceedings of the ICCF10, (2004). 20. S. Pons and M. Fleischmann, inProceedings of the ICGF2, p. 349 (1991). 21. M. Fleischmann, inProceedings of the ICCF5, p. 152 (1995). 22. M.H. Miles, S. Szpak, P.A. Mosier-Boss, and M. Fleischmann, inProceedings of the ICCF9, p. 250 (2002). 23. inProceedings of the ICCF4, 2, 18-1 (1993). 24. E. Storms, Some characteristics of heat production using the cold fusion effect, Proc. ICCF4 2, 4-1 (1993). 25. L. Case, in his oral presentation at ICCF10. 26. M.C.H. McKubre, S. Crouch-Baker, A.M. Riley, S.I. Smedley, and F.L. Tanzella, Excess power observations in electrochemical studies of the D / P d system; the influence of loading inProceedings of the ICCF3, p. 5 (1992). 27. M.C.H. McKubre, S. Crouch-Baker, F.L. Tanzella, S.I. Smedley, M. Williams, S.
54
28. 29. 30.
31. 32. 33.
34.
35. 36. 37. 38.
39. 40. 41. 42.
43.
44. 45. 46. 47.
48. 49. 50. 51.
Wing, M. Maly-Schreiber, R.C. Rocha-Filho, P.C. Searson, J.G. Pronko, and D.A. Koehler, Development of Advanced Concepts for Nuclear Processes in Deuterated Metals, EPRI Report TR-104195, August 1994. A. Takahashi, A. Mega, T. Takeuchi, H. Miyamura, and T. Iida, inProceedings of the ICCF3, p. 79 (1992). T. Aoki, Y. Kurata, E. Ebihara, N. Yoshikawa, Proc. ICCF4 2, 23-1 (1993). E.K. Storms, A study of those properties of palladium that influence excess energy production by the Pons-Fleischmann effect, (1996) http://www.lenrcanr.org/acrobat/StormsEastudyofth.pdf F. De Marco, A. De Ninno, A. Frattolillo, A. La Barbera, F. Scaramuzzi, and V. Violante, inProceedings of the ICCF6, p. 145 (1996). A. Takahashi, T. Takeuchi, T. Iida, and M. Watanbe, Neutron spectra from D 2 0 - P d cells with pulse electrolysis, inProceedings of the Provo meeting, p. 323 (1990). A. Takahashi, T. Iida, T. Takeuchi, A. Mega, S. Yoshida, and M. Watanabe, Neutron spectra anc control lability by PdD/Electrolysis cell with low-high current pulse operation, inProceedings of the ICCF2, p. 93 (1991). J.O'.M Bockris, D. Hodko, and Z. Minevski, The mechanism of deuterium evolution on palladium: Relation to heat bursts provoked by fluxing deuterium across the interface, inProceedings of the ICCF2, p. 337 (1991). E. Yamaguchi and T. Nishioka, Direct evidence for nuclear fusion reactions in deuterated palladium, inProceedings of the ICCF3, p. 179 (1992). H. Sugiura and E. Yamaguchi, inProceedings of the ICCF7, p. 366 (1998). E. Yamaguchi and H. Sugiura, inProceedings of the ICCF7, p. 420 (1998). C. Bartolomeo, M. Fleischmann, G. Larramona, S. Pons, J. Roulette, H. Sugiura, and G. Preparata, Alfred Coehn and after: The a, /3, 7 of the palladium-hydrogen system, Proc. ICCF4 1, 19-1 (1993). F. Celani, A. Spallone, P. Tripodi, A. Petrocchi, D. DiGioacchino, P. Marini, V. DiStefano, S. Pace, and A. Mancini, inProceedings of the ICCF5, p. 57 (1995). F. Celani, A. Spallone, P. Tripodi, D. DiGioacchino, P. Maini, V. DiStefan, A. Mancini, and S. Pace, inProceedings of the ICCF6, p. 93 (1996). G. Preparata, inProceedings of the ICCF6, p. 136 (1996). M.C.H. McKubre, S. Crouch-Baker, A.K. Hauser, S.I. Smedley, F.L. Tanzella, M.S. Williams, and S.S. Wing, Concerning reproducibility of excess power production, inProceedings of the ICCF5, p. 17 (1995). J. Tian, X.Z. Li, W.Z. Yu, D.X. Cao, R. Zhou, Z.W. Yu, Z.F. Jiang, Y. Liu, J.T. He, and R.X. Zhou, Anomalous heat flow and its correlation with deuterium flux in a gas-loading deuterium-palladium system, inProceedings of the ICCF9, p. 353 (2002). J.O'.M. Bockris, et al., Proc. ICCF4 2, 1-1 (1993). X.Z. Li, B. Liu, N.N. Cai, Q.M. Wei, J. Tian, and D.X. Cao, inProceedings of the ICCF10, (2004). Y. Iwamura, M. Sakano, and T. Itoh, Jpn. J. Appl. Phys. 41 4642 (2002). Y. Iwamura, T. Itoh, M. Sakano, S. Sakai, and S. Kuribayashi, Low energy nuclear transmutation in condensed matter induced by D2 gas permeation through Pd complexes: Correlation between deuterium flux and nuclear products, inProceedings of the ICCF10, (2004). D. Letts and D. Cravens, Laser stimulation of deuterated palladium: Past and present, inProceedings of the ICCF10, (2004). D. Cravens and D. Letts, Practical techniques in CF research: Triggering methods, inProceedings of the ICCF10, (2004). T.O. Passell, inProceedings of the ICCF5, p. 603 (1995). T.O. Passell, inProceedings of the ICCF9, p. 299 (2002).
55 52. J. Dash, inProceedings of the ICCF6, p. 477 (1996). 53. T. Bressani, Nuclear products in cold fusion experiments, comments and remarks after ICCF-6, inProceedings of the ICCF6, p. 703 (1996). 54. L.C. Case, Catalytic fusion of deuterium into helium-4inProceedm<7s of the ICCF7, p. 48 (1998). 55. M.H. Miles and B. Bush, Search for anomalous effects during D2O Electrolysis Using Palladium C&thodesinProceedings of the ICCF3, p. 189 (1992). See also: M.H. Miles, B. Bush, and J.J. Lagowski, Anomalous effects involving excess power, radiation, and helium production during D2O electrolysis using palladium cathodes, Fusion Technol. 25, 478, 1994. B.F. Bush, J.J. Lagowski, M.H. Miles, and G.S. Ostrom, Helium production during the electrolysis of D2O in cold fusion, J. Electroanal. Chem. 304 (1991) 271. M.H. Miles, R.A. Hollins, B.F. Bush, J.J. Logowski, and R.E. Miles, Correlation of excess power and helium production during D2O and H2O electrolysis using palladium cathodes, J. Electroanal. Chem. 346 (1993) 99. 56. B. Bush and J.J. Lagowski, Methods of generating excess heat with the Pons and Fleischmann effect: Rigorous and cost effective calorimetry, nuclear products analysis of the cathode and helium analysis, inProceedings of the ICCF7, p. 38 (1998). 57. E. Botta, R. Bracco, T. Bressani, D. Calvo, V. Cela, C. Fanara, U. Ferracin, and F. Iazzi, Search for He production from Pd/D2 systems in gas phase, inProceedings of the ICCF5, p. 233 (1995). 58. E. Botta, T. Bressani, D. Calvo, C. Fanara, and F. Iazzi, Measurements of He production from D2 gas- loaded Pd sample, inProceedings of the ICCF6, p. 29 (1996). 59. G.S. Qiao, X.L. Han, L.C. Kong, S.X. Zheng, H.F. Huang, Y.J. Yan, Q.L. Wu, Y. Deng, S.L. Lei, and X.Z. Li, Nuclear products in a gas-loading D/Pd and H / P d system, inProceedings of the ICCF7, p. 314 (1998). 60. D. Gozzi, R. Caputo, P.L. Cignini, M. Tomellini, G. Gigli, G. Balducci, E. Cisban, S. Frullani, F. Garibaldi, M. Jodice, G.M. Urciuoli, Excess heat and nuclear product measurements in cold fusion electrochemical cells, inProceedings of the ICCF4 1,2-1 (1993). 61. J. O'M. Bockris, C. Chien, D. Hodko, and Z Minevski, Tritium and Helium Production of Palladium Electrodes and the Fugacity of Deuterium Therein, inProceedings of the ICCF3, p. 231 (1992). C-C Chien, D. Hodko, Z. Minevski, and J. O'M. Bockris, On an electrode producing massive quantities of tritium and helium, J. Electroanal. Chem. 338 (1992) 189. 62. B.Y. Liaw, P.-L. Tao, and B.E. Liebert, Recent progress on cold fusion research using molten salt tech niques, inProceedings of the ICCF2, p. 92 (1991). 63. H. Sakaguchi, G. Adachi, and K. Nagao, Helium Isotopes from Deuterium Absorbed in LaNi5, inProceedings of the ICCF3, p. 527 (1992). 64. J.R. Morrey, M.W. Caffee, H. Farrar, IV, N.J. Hoffman, G.B. Hudson, R.H. Jones, M.D. Kurz, J. Lupton, B.M. Oliver, B.V. Ruiz, J.F. Wacker, and A. Van Veen, Measurements of helium in electrolyzed palladium, Fusion Technol. 18 (1990) 659. 65. Y. Arata and Y.-C. Zhang, Helium ( 4 He, 3 He) within deuterated Pd-black, inProceedings of the Japan Acad. 73B (1997) 1. 66. Y. Arata and Y.-C. Zhang, Achievement of solid-state plasma fusion (cold fusion), inProceedings of the Japan Acad. 71 Ser. B (1995) 304. 67. A.G. Lipson, A.S. Roussetski, G.H. Miley, and E.I. Saunin, inProceedings of the ICCF8, p. 231 (2000). 68. A.G. Lipson, A.S. Roussetski, G.H. Miley, and C H . Castano, inProceedings of the ICCF9, p. 218 (2002). 69. M.H. Miles, Correlation of excess enthalpy and helium-4 production: A review, inProceedings of the ICCF10, (2004).
56 70. M.C.H. McKubre, et al., Energy Production Processes in Deuterated Metals, EPRI Report TR-107843-V1 (1998). 71. F. Cellucci, P.L. Cignini, G. Gigli, D. Gozzi, M. Tomellini, E. Cisbani, S. Frullani, F. Garibaldi, M. Jodice, and G.M. Urciuoli, inProceedings of the ICCF6, p. 3 (1996). 72. A. De Ninno, A. Frattolillo, A. Rizzo, and E. Del Giudice, inProceedings of the ICCF9, p. 82 (2002). 73. A. De Ninno, A. Frattolillo, A. Rizzo, and E. Del Giudice, He detection in a cold fusion experiment, inProceedings of the ICCF10, (2004). 74. S. Pons and M. Fleischmann, Heat after death, Proc. ICCF4 2, 8-1 (1993). 75. M. Fleischmann and S. Pons, Phys. Lett. A 176 118 (1993). 76. M. Bernardini, C. Manduchi, G. Mengoli, and G. Zannoni, Anomalous effects induced by D2O electrolysis at titanium, inProceedings of the ICCF8, p. 39 (2000). 77. M.H. Miles, M.A. Imam, and M. Fleischmann, inProceedings of the ICCF8, p. 105 (2000). 78. M. Fleischmann, inProceedings of the ICCF9, p. Ill (2002). 79. I. Dardik, H. Branover, A. El-Boher, D. Gazit, E. Golbreich, E. Greenspan, A. Kapusta, B. Khachatorov, V. Krakov, S. Lesin, B. Michailovitch, G. Shani*, and T. Zilov, inProceedings of the ICCF10, (2004). 80. M.H. Miles, K.B. Johnson, and M.A. Imam, Heat and helium measurements using palladium alloys in heavy water, inProceedings of the ICCF6, p. 20 (1996). 81. M.F. Klopfenstein and J. Dash, Thermal imaging during electrolysis of heavy water with a Ti cathode, inProceedings of the ICCF7, p. 98 (1998). 82. E. Storms, Excess power production from platinum cathodes using the PonsFleischmann effect, inProceedings of the ICCF8, p. 55 (2000). 83. Y. Arata and Y.-C. Zhang, inProceedings of the Japan Acad., 70(B), 106 (1994). 84. S.E. Jones, D. Bennion, D. Buehler, J.B. Czirr, D.L. Decker, J. Harb, R. Hunter, G.L. Jensen, E.P. Palmer, W. Pitt, S. Taylor, J. Thorne, D. Tolley, and J.C. Wang, inProceedings of the Provo meeting, p. 206 (1990). 85. S.E. Jones, T.K. Bartlett, D.B. Buehler, J.B. Czirr, G.L. Jensen, and J.C. Wang, inProceedings of the Provo meeting, p. 397 (1990). 86. F. Celani, A. Spallone, L. Liberatori, B. Stella, F. Ferrarotto, M. Corradi, P. Marini, S. Fortunati, and M. Tului, inProceedings of the Provo meeting, p. 62 (1990). 87. P.I. Golubnichyi, A.D. Philonenko, A.A. Tsaric, E.P. Kovalchuk, G.L Merzon, and V.A. Tsarev, Obser vation of nuclear particles and their correlation with acoustic and electromagnetic emission from palladium targets loaded with deuterium, inProceedings of the Provo meeting, p. 146 (1990). 88. P.L Golubnichyi, A.D. Philonenko, A.A. Tsaric, V.V. Kuzminov, B.V. Pritchenko, G.L Merzon, and V.A. Tsarev, Recording of neutron and acoustic emissions from palladium target in a low background underground experiment, inProceedings of the Provo meeting, p. 151 (1990). 89. M. Okamoto, Y. Yoshinaga, M. Aida, and T. Kusunoki, Proc. ICCF4 2, 3-1 (1993). 90. S.E. Jones, J.E. Ellsworth, and M.R. Scott, F.W. Keeney, A.C. Johnson, D.B. Buehler, F.E. Cecil, G. Hubler, and P.L. Hagelstein, Neutron emissions from metal deuterides, inProceedings of the ICCF10, (2004). 91. K.L. Wolf, Nuclear reactions in deuterated metals, EPRI Progress Report, March 1992. 92. K.L. Wolf, private communication, 1993. 93. F.E. Cecil, H. Liu, D. Beddingfield, and C.S. Galovich, inProceedings of the Provo meeting, p. 375 (1990). 94. S.E. Jones, F.W. Keeney, A.C. Johnson, D.B. Buehler, F.E. Cecil, G. Hubler, P.L. Hagelstein, J.E. Ellsworth, and M.R. Scott, Charged particle emissions from metal
57 deuterides, inProceedings of the ICCF10, (2004). 95. A. De Ninno, A. Frattolillo, G. Lollobattista, L. Martinis, M. Martone, L. Mori, S. Podda, F. Scaramuzzi, Europhys. Lett. 9 221 (1989). 96. A. De Ninno, F. Scaramuzzi, A. Frattolillo, S. Migliori, F. Lanza, S. Scaglione, P. Zeppa, and C. Pontorieri, The production of neutrons and tritium in the deuterium gas-titanium interaction, inProceedings of the ICCF2, p. 129 (1991). 97. H.O. Menlove, M.A. Paciotti, T.N. Claytor, H.R. Maltrud, O.M. Rivers, D.G. Tuggle, and S.E. Jones, Reproducible neutron emission measurements from Ti metal in pressurized D2 gas, inProceedings of the Provo meeting, p. 287 (1990). 98. H.O. Menlove, M.A. Paciotti, T.N. Claytor, and D.G. Tuggle, Low-background measurements of neutron emission from Ti metal in pressurized deuterium gas, inProceedings of the ICCF2, p. 385 (1991). 99. T. Bressani, D. Calvo, A. Feliciello, C. Lamberti, F. Iazzi, B. Minetti, R. Cherubini, A.M.I. Haque, and R.A. Ricci, A study of the neutron emission from Ti loaded with D in gas phase by means of a time-of-flight spectrometer, inProceedings of the ICCF2, p. 105 (1991). 100. M. Agnello, E. Botta, T. Bressani, D. Calvo, A. Feliciello, P. Gianotti, F. Iazzi, C. Lamberti, B. Minetti, and A. Zecchina, Measurement of 2.4 MeV neutrons from Ti/D and P d / D systems, inProceedings of the ICCF3, p. 433 (1992). 101. A. De Ninno, F. Scaramuzzi, C. Pontorieri, and P. Zeppa, Emission of neutron bursts from a titanium- deuterium gas system in a high-efficiency low-background experimental setup, inProceedings of the Provo meeting, p. 122 (1990). 102. F. Scaramuzzi, Survey of gas loading experiments, inProceedings of the ICCF2, p. 445 (1991). 103. M. Fleischmann, An overview of cold fusion phenomena, inProceedings of the ICCF1, p. 344 (1990). 104. D. Gozzi, P.L. Cignini, R. Caputo, M. Tomellini, G. Balducci, G. Gigli, E. Cisbani, S. Frullani, F. Garibaldi, M. Jodice, and G.M. Urciuoli, Experiments with global detection of cold fusion byproducts, inProceedings of the ICCF3, p. 155 (1992). 105. H. Ogawa, S. Yoshida, Y. Yoshinaga, M. Aida, and M. Okamoto, Excess heat and neutron emission in Pd-Li-D electrolysis, inProceedings of the ICCF5, p. 116 (1995). 106. A. Takahashi, T. Inokuchi, Y. Chimi, I. Ikegawa, N. Kaji, Y. Nitta, K. Kobayashi, and M. Tanaguchi, Experimental correlation between heat and nuclear products, inProceedings of the ICCF5, p. 69 (1995). 107. A. Takahashi, Results of experimental studies on excess heat vs. nuclear products correlation and conceiv able reaction model, inProceedings of the ICCF7, p. 378 (1998). 108. Y. Oya, H. Ogawa, M. Aida, K. Iinuma, and M. Okamoto, Material conditions to replicate the generation of excess energy and the emission of excess neutrons, inProceedings of the ICCF7, p. 285 (1998). 109. H. Liu, Studies of nuclear reactions D-D, D-6Li, and D-10B at low energies and charged particle emission from deuterium-metal systems, PhD Thesis, Colorado School of Mines, 1992. 110. A.G. Lipson, A.S. Roussetski, G.H. Miley, and E.I. Saunin, inProceedings of the ICCF8, p. 231 (2000). A.G. Lipson, A.S. Roussetski, G.H. Miley, and C.H. Castano, inProceedings of the ICCF9, p. 218 (2002). 111. A.G. Lipson, A.S. Roussetski, G.H. Miley, and E.I. Saunin, Phenomenon of an energetic charged particle emission from hydrogen/deuterium loaded metals, inProceedings of the ICCF10, (2004). 112. J. Kasagi, T. Ohtsuki, K. Ishu, and M. Hiraga, Phys. Soc. Japan 64, 777 (1995). 113. E.K. Storms, A critical evaluation of the Pons-Fleischmann effect, http://www.lenr-
58 canr.org/acrobat/StormsEacriticale.pdf 114. M. Fleischmann, Thermal and nuclear aspects of the P d / D 2 0 system; Volume 2, SPAWAR System Center Report TR-1862 (2002). 115. S. Pons and M. Fleischmann, Calorimetric measurements of the palladium/deuterium system: Fact and fiction, Fusion Technol. 17 (1990) 669. 116. S.E. Jones, L.D. Hansen, S.E. Jones, D.S. Shelton, and J.M. Thorne, Faradaic efficiencies less than 100% during electrolysis of water can account for reports of excess heat in cold fusion cells, J. Phys. Chem. 99 (1995) 6973. 117. F.G. Will Hydrogen + oxygen recombination and related heat generation in undivided electrolysis cells, J. Electroanal. Chem. 426 (1997) 177. 118. M.C.H. McKubre, F.L. Tanzella, P. Tripodi, and P.L. Hagelstein, The emergence of a coherent explanation for anomalies observed in D / P d and H / P d systems: Evidence for He and He production, inProceedings of the ICCF8, p. 3 (2000). 119. W.B. Clarke, Fusion Science and Technology, Production of He in D2-loaded palladium-carbon catalyst I, 43 (1) 122 (2003). 120. W.B. Clarke, W.J. Jenkins, and Z. Top, Determination of tritium by mass spectrometric measurement of He, i n j . Appl. Radiat. Isot. 27, p. 515 (1976). 121. Y. Arata and Y.-C. Zhang, inProceedings of the Japan Acad., 71(B), 98 (1995). 122. Y. Arata and Y.-C. Zhang, inProceedings of the ICCF6, p. 129 (1996). 123. Y. Arata and Y.-C. Zhang, J. High Temperature Society, 23, 1 (1997). 124. Y. Arata and Y.-C. Zhang, inProceedings of the Japan Acad. 78(B), 57 (2002). 125. Y. Arata and Y.-C. Zhang, Anomalous difference between reaction energies generated within D 2 0-Cell and H 2 0-cell, Jpn. J. Appl. Phys. 37, L1274 (1998). 126. W.B. Clarke, B.M. Oliver, M.C.H. McKubre, F.L. Tanzella, and P. Tripodi, Search for He and He in Arata-style palladium cathodes II; Evidence for tritium production, Fusion Science and Technology, 40 (2) (2001). 127. Y. Arata and Y.-C. Zhang, Deuterium nuclear reaction process within solid, inProceedings of the Japan Acad. 72(B), 179 (1996). 128. Y. Arata and Y.-C. Zhang, Presence of Helium (He, 3He) confirmed in deuterated Pd-black by the 'vi- effect' in a 'closed QMS' environment, Proc. Jpn. Acad. 73B, 62 (1997). 129. Y. Arata and Y.-C. Zhang, Anomalous production of gaseous He at the inside of 'DS-cathode' during D 2 0-electrolysis, Proc. Jpn. Acad. 75B, 281 (1999). 130. A. Farkas, On the electrolytic separation of the hydrogen isotopes on a palladium eathode, Trans. Faraday Soc. 33, 552 (1937).
The Conference Proceedings Cited in This Bibliography (1) Proc. Provo meeting (1990): Anomalous Nuclear Effects in Deuterium/Solid Systems (Provo, UT, 1990); S.E Jones, F. Scaramuzzi, and D.H. Worledge (eds.), American Institute of Physics: Conference Proceedings, Vol. 228. (2) Proc. ICCF1 (1990): F. Will (ed.), Proceedings of the First International Conference on Cold Fusion, March 1990 (Salt Lake City, UT). (3) Proc. ICCF2 (1991): T. Bressani, E. Del Giudice, and G. Preparata (eds.), The Science of Cold Fusion, Proceedings of the Second Annual Conference on Cold Fusion, Vol. 33 (Societa Italiana di Fisica, Como, Italy, June 29-July 4, 1991).
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(4) Proc. ICCF3 (1993): Frontiers of Cold Fusion, Proceedings of the Third International Conference on Cold Fusion (Nagoya, Japan, October 1992) edited by H. Ikegami, Universal Academy Press, Tokyo. (5) Proc. ICCF4 (1993): T.O. Passell and M.C.H. McKubre (eds.), Proceedings of the Fourth International Conference on Cold Fusion (Maui, Hawaii, December 1993) (6) Proc. ICCF5 (1995): Proceedings of the Fifth International Conference on Cold Fusion (Monte Carlo, Monaco, April 9-13, 1995; IMRA, Europe, Sophia Antipolis Cedex, France, 1995). (7) Proc. ICCF6(1996): M. Okamoto (ed.), Proceedings of the Sixth International Conference on Cold Fusion (Hokkaido, Japan, October 1996). (8) Proc. ICCF7 (1998): Proceedings of The Seventh International Conference on Cold Fusion (Vancouver, Canada, April 19-24, 1998; ENECO Inc., Salt Lake City, UT; 1998). (9) Proc. ICCF8 (2000): Proceedings of the Eighth International Conference on Cold Fusion (Lerici, La Spezia, Italy, May 2000) edited by F. Scaramuzzi. (10) Proc. ICCF9 (2002): X.Z. Li (ed.), Proceedings of the Ninth International Conference on Cold Fusion (Beijing, China, May 2002) (11) Proc. ICCF10 (2003): Proceedings of the Tenth International Conference on Cold Fusion Cambridge, MA, August 2003) edited by P.L. Hagelstein and S.R. Chubb, World Scientific, to appear.
REPRODUCIBILITY, CONTROLLABILITY, A N D OPTIMIZATION OF LENR E X P E R I M E N T S
DAVID J. NAGEL The George Washington University, Washington, DC 20052, USA Low-energy nuclear reaction (LENR) measurements are significantly and increasingly reproducible. Practical control of the production of energy or materials by LENR has yet to be demonstrated. Minimization of costly inputs and maximization of desired outputs of LENR remain for future developments.
1. Introduction Experimental evidence for low-energy nuclear reaction (LENR) is robust. There is what many consider to be an irrefutable collection of laboratory data, which says that nuclear reactions can be induced at low temperatures (energies). Of the 3000+ papers in the field, many contain data by experienced investigators, with good equipment, who used careful procedures (including calibrations and controls) and got high signal-to-noise ratios for anomalous effects in repeated experiments. Part of such data was reviewed recently.1 The understanding of nuclear reactions in condensed matter at low energies is very incomplete, but that does not detract from the reliability of much of the experimental data. If one takes the view that nuclear reactions can occur at low energies in solid and liquid systems, then it can be asked what might come out of this new field of science, now termed condensed matter nuclear science. When understood, will the new knowledge prove to be of no use whatsoever, merely an intellectual curiosity? Or, might LENR be the basis of some technology, that is, some demonstrable capability, but have no commercial applications? Possibly, LENR will turn out to be economically, and may be even socially important. The questions of technical and commercial viability can be addressed in coming years. Currently, concerns about reproducibility, controllability, and optimization of LENR experiments are very germane. These topics are the subject of this paper. The emphasis here is on reproducibility of LENR experiments, which is one of the most important and contentious topics in the field. Concerns about reproducibility are nothing new to science. However, they are very different for the various kinds of scientific functions, which are listed in the next section. Then, the possible combinations of scientific activities and results will be noted. Factors germane to LENR experiments are described next. The question of how the reproducibility of experiments can be quantified will be addressed. The following section presents some of the intra- and inter-laboratory data on the reproducibility of LENR experiments. 60
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Then, the controllability and optimization of the results of LENR experiments are considered, these topics being fundamental to the ultimate utility of LENR. The concluding section summarizes the current status of reproducibility, controllability and optimization of LENR experiments. 2. Scientific Functions There are five types of scientific research activities. They have histories of widely varying duration: • Scientific observations. Human observations certainly predate the development of the scientific method. They remain central in some fields, astronomy being a good example. It is important that, even though scientists cannot influence what they are observing, they can choose the apparatus to use, for example, optical telescopes, or radio receivers. • Experimental science. Developing and testing things also has an ancient history, with the production of rudimentary tools, such as flints, providing an early example. When people have control over what is being tried, then varying measures of reproducibility and controllability are expected, especially in modern times. • Development of theories. Having ideas that will either explain past observations or predict the results of new experiments is central to science. Without such understanding, optimization of processes, and the concomitant commercial impact, are difficult to achieve. This scientific function is old and can be done with simple tools, essentially writing instruments and paper. • Computational science. In the last several decades, the development of facile computers has enormously accelerated both the size and number of calculations that can be done to either understand available data or guide pending experiments. The reduction of complex theoretical formulations to numbers in diverse simulations has also significantly improved commercial engineering. The impact of computations even extends to fundamental research in mathematics. • Data analysis. The synthesis of data from observations and experiments is an old activity. Here again, computers have had dramatic recent effects. They can compile, compare, and mine data, whatever its source, and provide insights that could not be obtained or supported otherwise. Scientific experimentation controls the input activities that produce some results. It is common for the same set of activities to produce the same set of results, even in arenas in which understanding is imperfect or lacking. This is a basic reason why so many people were critical of "cold fusion" in the early years after it burst on the world stage. Lack of reproducibility, and the great disagreement in nuclear reaction rates between observations in LENR experiments and understood theory were both fundamental to the field being dismissed by most people as wrong or worse.
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In the next section, we briefly list and examine the possible combinations of input activities and output results for scientific experiments. It is a prelude to more specific consideration of factors relevant to LENR in the following section. 3. Experimental Activities and Results In general, people desire and expect the same experimental activities to produce the same results. However, this is not always the case. Further, sometimes the activities can be varied without significantly changing the results. In that case, the results are relatively insensitive to one or more of the experimental variables. The point is that, for most experiments, there are several critical variables. The identity of all of these must be known, and controlled to within some tolerance, if an experiment is to give the same results and be deemed to be reproducible. This is usually the case in established areas of science and technology. However, it is often not the case early in a field, when all the salient variables are not known, let alone their values for reproduction of certain results. In general terms, the multi-dimensional space formed by all the relevant experimental variables has a "sweet spot" that includes the important values of each of the variables. The range of permissible values will generally be different (in absolute or relative terms) for the various variables. If the input experimental conditions are within that hyper-volume of acceptable values for all the variables, then the outcome of the experiment will be the same to some tolerance. Early in a field, some scientists may happen to perform experiments that fall within the "sweet spot" of variables that will produce unexpected (anomalous) results. However, if they do not achieve similar conditions in later experiments, due to ignorance or lack of control of salient variables, they will not have a reproducible experiment. Table 1. The combinations of possible activities and results in LENR and other experimental research.
Activities Results
Same
Different
AS RS
AD RD
The variety of input and outcome possibilities can be considered with the aid of Table 1. The four combinations have the following characteristics. • AS-RS. This is the common case, which many people expect, or even demand, of laboratory research. All of the relevant variables and their acceptable ranges are known and controlled. • AS-RD. Here, there might be some uncontrolled (hidden) variable that has a significant influence on the outcome of an experiment. That is, one or more of the critical variables is not even recognized, let alone controlled. • AD-RS. In this case, one of the input variables is not very important to
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the outcome. This means that, while the variable may be significant, the results are not very sensitive to its value. • AD-RD. This, also, is a common case. Then, the input to the experiment is outside the "sweet spot" for one or more of the critical variables. 4. Factors in LENR Experiments The discussion in the last section is very general. It does not specify the important types of activities, functions, or factors that go into the design of an experiment, the so-called inputs. They are the subjects of this section. There are five fundamental input factors that determine both the execution and outcome of an LENR experiment, and are, therefore, relevant to the issue of reproducibility. • Materials. The composition of materials, including both the major, minor and impurity elements, and the lattice and defect structures of materials, are usually critical in condensed matter experiments. The role of alloying elements, such as boron, has been discussed in the literature on LENR. • Apparatus. The materials out of which the experimental equipment is constructed, and its geometry, are generally very influential. The base material, usually glass or plastic, and the presence or absence of coatings on the interiors of electrochemical cells, are thought to be significant in LENR experiments. • Protocols. What is done and in what order almost always determines the results of experiments, whatever the subject. Many different means, including heated containers, electrochemical cells, plasmas, and beams in a vacuum, have been employed in LENR experiments to bring together the nuclear reactants. In electrochemical cells, the magnitude of the electrical current used to charge Pd with deuterons, and the way in which it is varied with time, have gotten much attention in experiments aimed at producing excess energy by LENR. • Experimenter. The experience, skills, and predilections of the experimenter, generally determined by education and past work, are important, especially for very inter-disciplinary subjects like LENR. Given that physics, chemistry, materials and other sciences, and multiple engineering disciplines, are all germane to LENR experiments, and that few scientists have significant hands-on experience in all these fields, some parts of LENR experiments get more attention than others in the hands of people with different backgrounds. • Organization. The organization within which experiments are conducted certainly influences their course because of the importance of available infrastructure, and the actual or psychological support of managers and colleagues. The LENR experiments in a home shop can produce worthwhile results and information, but they generally lack the ready access to diverse and expensive analytical and other equipment, and experts in many fields, which are both available in large laboratories.
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5. Quantification of Reproducibility Science depends on numerical measures of its functions. A quantitative measure of the reproducibility of experiments could take into account both the input to and output from an experiment. However, no such measure has been found in the literature. In most fields of research, only the output of experiments has been used as a measure of reproducibility. This is understandable because of the primacy of results and the fact that they are usually quantitative. However, in most experiments there are multiple outputs that can be measured, so it is worth discussing which of them will serve as the measure of reproducibility. In the case of LENR experiments, either the output of energy or of new materials could serve as a fiducial for reproducibility. Focussing on energy, specific measures can be the observation of instantaneous or average excess power, or excess energy, the integral of the excess power over the duration of an experiment. In early and in many current experiments, the basic question has been whether or not any excess power is observed. There is no unanimity on which of the various measures of power should be the arbiter of a successful experiment. Absolute power (W) or power density (W per surface area, volume, mass, or atoms) could all serve that function. Even if there were an agreed upon factor, there remains a need to set a threshold above which an experiment is deemed a success. There has been little discussion of either the factors or the thresholds for quantification of reproducibility for LENR. The most common approach has been to form a ratio of the number of experiments that were thought by the person who conducted them to exhibit anomalous effects to the number of experiments that were run. That is commonly done without specification of the threshold for determining that an experiment gave unusual results and was successful at replicating one or more of the anomalies reported in the field. This approach, while flawed logically and practically, is all that is available, and will be used here. 6. Reproducibility of LENR Experiments The most fundamental ability is for an experimenter to be able to reproduce conditions and results within their own laboratory. The ability of different researchers in their own separate laboratories to reproduce each other's experiments is also critical. Both of these are important in condensed matter nuclear science. 6.1. Intra-Laboratory
Reproducibility
McKubre and his colleagues at SRI International have performed over 100,000 h of precision calorimetry since the Fleischmann-Pons announcement in 1989. A graphical summary of their experiments, which achieved high degrees of loading, is given in Fig. I. 2 The data show that the appearance of excess power in D-Pd electrochemical experiments is reproducible, if a high ratio of D to Pd atoms is achieved in the experiments. The degree of reproducibility is flawed because the amount of excess power and energy varies even amongst experiments that do give a power and energy gain.
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|
| No excess observed I "\i-i"N«t power observed
1 100%
E s Z
38%
i 100% I
<0.90
1.00 0.95 Maximum loading obtai ed (D/Pd)
1.05
Figure 1. Observations at SRI International of excess heat as a function of the loading ratio of deuterons (D) to Pd atoms in cathodes in electrochemical experiments.
The reproducibility fraction within one laboratory in certainly not constant over time, even for a given experimenter. In general, reproducibility increases with time. A survey of intra-laboratory reproducibility was conducted in 2003 by Krivit. 3 He polled 43 researchers in the field and asked them, among other things, about their rate of experimental reproducibility both 5 years before and in the last year. Seven researchers provided data on their older rate and 10 on their more recent experience. The average of the rates for 1998 was 45% and the average for 2003 was 83%. While these are small samples, both statistically and relative to the number of experimenters in the field, the increase may be indicative of a real improvement in the reproducibility of LENR experiments over those years. There are many other reports of intra-laboratory reproducibility of anomalies by different investigators using a variety of techniques. Miles conducted numerous electrochemical experiments, usually with rod-shaped cathodes, and measured both heat and helium production. In a review, he reported that "30 out of 33 experiments agree with the hypothesis that the excess enthalpy produced in cold fusion studies is correlated with helium-4 production" . 4 Szpak and his colleagues used electrochemical co-deposition of D and Pd, and measured a wide variety of anomalies, including heat and tritium production, and X-ray and infrared emissions. Experiments for over one decade exhibited "anomalous events virtually 100% of the time" . 5 Other reports of reproducibility are scattered throughout the literature on LENR. A complete study of intra-laboratory reproducibility could be done by getting time-dependent, say annual, reproducibility rates from several of the researchers in the field, who have conducted continual experiments. It could also be based on the spotty reports of reproducibility scattered throughout the literature on LENR. Both of these approaches are beyond the scope of this paper. However, it seems clear, and is widely accepted within the field, that reproducibility within some laboratories is
66
now significantly better than in the early years of the field. It is still short of what is desired, and many researchers are seeking a recipe that will work consistently both in their laboratories and in the hands of researchers at other locations. See, for example, the guidance on reproducibility provided by Storms. 6
6.2. Inter-Laboratory
Reproducibility
There have been relatively few attempts to transfer experiments from one laboratory to another. Nine efforts to reproduce experiments first done in various other laboratories were made at SRI International by McKubre et al.7 They involved the initial investigators. A three-step protocol was used in these cases: (1) One or more of the original experimenters was given space in the SRI International laboratories to set up and operate their experiment without involvement by SRI personnel, other than providing support. No changes in the experiment were made by SRI personnel. (2) At the appropriate time, the guest experimenter(s) taught their procedures and explained their performance characteristics to SRI personnel, enabling them to operate the existing setup. (3) The SRI scientists operated the experiment either without changes in the setup or protocols, or with new procedures and, often, with the addition of improved or new diagnostics. The experiments involved precision calorimetry and other high-quality diagnostics. The originating investigators, the years of their reports, the character of their experiments and the outcome of the reproducibility attempts at SRI International are summarized in Table 2. Table 2. The scientists, years of their work, type of experiments and results of replication attempts at SRI international (EC = electrochemical). Experimenters (years)
Nature of experiment
Outcome @ SRI International
M. Miles and B. Bush (1993) M. Srinivasan (1994)
EC loading: D - P d EC loading: H-Ni
J. Patterson and D. Cravens (1995) R. Stringham and R. George (1996) X. Arata and X. Zhang (1996-1997) F. Celani et al. (1998) R. Stringham (1999) L. Case (1998-2002)
EC loading: H/D-Ni
Low levels of He observed No excess power; chemical effect No excess power
Cavitation loading: D-metals
No excess power
EC double structure cathode: D-Pd EC loading fine wires Cavitation loading: D-metals Heat and Pressure: D2 + Pd catalyst EC Loading + Laser Stimulation
80% excess energy and He increase No excess power No excess power Correlated heat and He production 28 W / c m 3 and 25 kJ excess observed
D. Letts (2003)
and
D. Cravens
67
Table 2 shows that excess power and energy, sometimes with significant amounts of He, were produced in three of the nine replication attempts. The reasons for the failed replication attempts are not clear, in general. 7. Controllability and Optimization of LENR Experiments The ability to reproduce LENR or other experiments can be viewed as a form of control. That is, the experimenter has sufficient control over the relevant variables to make the results come out within some bounds for run after run. However, further degrees of control are needed if LENR are to be practical sources of energy or materials. Consider an automobile. It is useful only because of the several controls that are built into it, including the ability to turn on the motor, to accelerate, to brake, and to turn-off the car. Without any one of these, a car would not be practical. The same considerations apply to processes for the production of energy or materials. Means to turn them on, to speed or slow them, and to turn them off are needed, if they are to be useful. Significant progress on the ability to influence, and even to control LENR experiments has been demonstrated. It is widely accepted for electrochemical experiments that high loading of D into Pd (as illustrated in Fig. 1), surface current densities above a thresholds of 100-500 mA/cm 2 and some disequilibrium are needed for the production of excess heat. 1 Conditions required for control of other types of LENR experiments involving heat, high pressures, plasmas or beams, which are needed for production of energy or materials, are much less well determined. If an LENR experiment is truly controllable, and hence reproducible, it might still be far from optimum. Optimization generally has two facets, minimization of the amounts and costs of the input energy and materials, and maximization of the output of energy or desired materials (and profits). If LENR proves to be useful for remediation of nuclear waste by transforming it into harmless materials, then optimization would involve processing the greatest amount of the undesired input material for the minimum expenditure of energy and money on equipment, and ancillary materials. Many LENR experiments have shown increases in heat or material production with some parameters, but peaks in output are rarely found. There has been almost no work on the practical optimization of LENR experiments. Such work can be done entirely on an empirical basis, the so-called "Edisonian" approach. However, it is most efficient and productive if there is theoretical understanding of the input factors that are relevant and the nature of the mechanisms involved in LENR. 8. Conclusion It is now clear that demands for reproducible experiments in the early years of LENR experiments were premature. In fact, one can argue that irreproducibility should be expected for early experiments in a complex new field. As emphasized in Table 3, and, as often happened in the history of science, experimental and theoretical progress can take years and even decades. For example, the understanding
68 of superconductivity took about four decades, even though reproducible experiments were possible for most of t h a t period. It is now taking another few decades for significant commercial exploitation of superconductivity. T h e historical flow in m a n y important scientific fields is from initial observations, which are often irreproducible, to reproducible observations, which might not be controlled, to controlled experiments t h a t might not be optimized, and finally, to controlled and optimized processes, which might be commercially viable.
Table 3. The evolution of reproducibility, controllability, and optimization in LENR experiments, as a function of time and increasing understanding. Time in years or decades Reproducibility Controllability Optimization Understanding
No No No
—>
Yes Yes Yes No Yes Yes No No Yes Increases with time
Reproducibility is only the first of these three sequential factors t h a t are crucial, if L E N R is t o prove t o b e as useful for production of energy and materials as many people hope. It has improved significantly since the early days of the field, and further advances can be expected, although the rate of progress is difficult to predict accurately. Controllability and optimization are technologically important. Now, controllability of L E N R experiments is limited and insufficient for practical exploitation of the mechanisms at work in those experiments. Optimization will be a practical (economic) necessity, but has hardly been explored, even empirically. It is likely t o b e m a n y years before investments in L E N R experiments will yield significant returns, even for successful research programs. However, it is clear t h a t a fundamental understanding of the anomalous effects observed in numerous experiments will significantly increase reproducibility, improve controllability, enable optimization of processes, and accelerate t h e economic viability of L E N R . References 1. P. L. Hagelstein, M. C. H. McKubre, D. J. Nagel, T. A. Chubb, and R. J. Hekman, New Physical Effects in Metal Deuterides, http://www.newenergytimes.com/DOE/2004DOE-Summary-Paper.pdf. 2. M. C. H. McKubre, Review of experimental measurements involving DD reactions, short course, 10th international conference on cold fusion (Cambridge, MA, USA, 25 August 2003). 3. S. Krivit, Cold fusion reproducibility, www.newenergytimes.com, 2004. 4. M. Miles, Correlation of excess enthalpy and helium-4 production: a review, 10th international conference on cold fusion (Cambridge, MA, USA, 25 August 2003).
69
5. F. E. Gordon, Private communication. See also S. Szpak, P. A. Mosier-Boss and F. E. Gordon, Precursors and the fusion reactions in polarized P d / P d - D 2 0 system: effect of an external electric field, these proceedings and references therein. 6. E. Storms, How to produce the Pons-Fleischmann effect, Fusion Technol. 29, 261 (1996). 7. M. C. H. McKubre, and F. Tanzella, Studies of reproducibility in the field of condensed matter nuclear science, in Proceedings of the 11th international conference of cold fusion (Marseilles, France, 2 November 2004).
E V I D E N C E OF ELECTROMAGNETIC RADIATION FROM N i - H SYSTEMS
S. F O C A R D I Department
of Physics,
Centro IMO,
University
of Bologna,
Bologna,
Italy
V. G A B B A N I , V. M O N T A L B A N O , F . P I A N T E L L I , A N D S. V E R O N E S I Department
of Physics,
Centro IMO,
University
of Siena,
Siena,
Italy
S. V E R O N E S I INFM,
UdR Siena,
Siena,
Italy
We report evidence of photon emission in three experiments with hydrogen loading of Ni slabs, during the degassing phase, when hydrogen was introduced into the cell, and during thermal cycling. In the first experiment we obtained excess power of about 20 W, while in the second experiment photon emission was observed instead of power production. In the third experiment, a Ni sample in hydrogen underwent thermal excitation and showed an increasing photon emission for a few hours.
1. Introduction In this paper, we present experimental results of photon emission observed during a preliminary preparation step of a Ni-H system. This step is performed to obtain heat production. The emission was detected in three successive experiments in a temperature range between 350 and 750 K. During previous experiments in which anomalous energy was produced from Ni samples in H atmosphere, 1 " 3 evidence was obtained of nuclear phenomena occurring in the samples4 and of ionising radiation coming from the experimental cell. 3 ' 5 Other authors reported similar evidence with electrolytic systems. 6,7 The purpose of the experiments described here was to obtain detailed information and confirmation of gamma emission3 and to perform a calorimetric evaluation of the cell energy balance using samples whose geometry was different from the one considered elsewhere.1 ~3 2. Experimental Setup 2.1. Experimental
Cell
The cell vessel consists of a stainless steel tube (AISI 304) having at the extremities two standard CF35 flanges. In the cell there are three Ni samples (99.5% purity) with slab geometry (200 mm x 12 mm x 1mm), prepared in a hydrogen 70
71
environment. 2 The heater consists of four plate coils, each made from a small NiCr slab of analogous dimensions, connected in series and held in a ceramic cylinder with the Ni samples in alternating positions (see Fig. 1).
Figure 1. (a) The experimental cell for three planar samples alternate with four planar heaters. The T[ indicates thermocouples, (b) The ceramic holder with a heater inside and a sample on the right.
All measurements (temperature, pressure, and power) are performed with the Labview data acquisition system as reported in Refs. 1 and 2. The experimental setup is shown in Fig. 2.
Nal(TI) detect or 2 n d and 3 r d exp
Pressure sensors
EXP. CELL
fcomi Compute Nal(TI) Detector 1 s t exp
I1(». coii.-ikT
&
M
Vacuum turbo-pump Neutron shield
\ Polyethylene Figure 2.
2.2. Neutron
Powdered boric acid
A schematic layout of the experimental setup.
Shield
In previous experiments we detected neutron emissions. 3 ' 5 Thus, for safety reasons, the cell was placed within a neutron shield (see Fig. 3). The shield is cube 100 cm on each side with walls 10-cm thick. The walls are made of polyethylene with an interstice of powdered boric acid (width 3.5 cm).
72
2.3. Photon
Detection
The measurement was obtained with a Nal(Tl) 4 in. x 4 in. detector and acquisition software (EG&G Ortec, Maestro II). Later on, to obtain a more accurate photon energy measurement, we used an HPGe detector having 7% efficiency and Silena EMCA PLUS acquisition software. Figure 2 shows the detector positions in all experiments. 3. Photon Emission The measurements were performed automatically, each recording having a fixed live time, usually 12,000 or 18,000 s. In the first experiment, the Nal detector was in front, as shown in Fig. 2. During a degassing phase 2 5 days after the start, when the sample temperature was about 420 K, the Nal detector was turned on. The 7 spectrum showed a structure different from the background. Figure 3 shows the measured 7 spectrum, the background spectrum, and the spectrum given by the difference between the two. In the difference spectrum the presence of three peaks superimposed on a continuous low-energy spectrum can be observed.
I 800 - i |
*: 600 -
1 /*•"
j .
,
E(keV) Measured spectrum « Background spectrum « Difference
ft?1000 E(keV)
Figure 3. First experiment: background and measured spectra, at the beginning of gamma measurements, obtained with the Nal(Tl) detector placed frontal in position. The background spectrum is a mean of 90 acquisition (live time 12,000 s) while the measured one is a mean of six acquisitions. The lower curve is the difference between measured and background spectrum.
Five days later we observed a sudden variation in photon spectrum with a lowering of the intensity of the three peaks as shown in Fig. 4. Peak intensity did not show detectable variation with gas admission, which was performed 19 days after the start of degassing. This emission lasted on the whole about 45 days. After this time period the spectrum went abruptly to the background
73 800
600-
% 400-
200
Measured spectrum Background spectrum Difference
'\et. *\ •-pv^
0 p"
500
1000
1/\ -?=»=*»•
JWEN^MafwMMWMlMwtMf
1500
2500
E(keV) Figure 4. First experiment: background and measured spectra 45 days after the beginning of gamma measurements, the measured spectrum is a mean of 18 acquisitions. The lower curve is the difference between measured and background spectra.
one. Later on the cell produced excess power (maximum 25 W measured with the method reported in Ref. 2) for about 35 days, after which the cell was shut down, in order t o repeat the experiment. In the second experiment new samples were used and the H P G e was added to att e m p t a quantitative measurement of photon energy. 8 In this experiment, the H P G e detector was in a lateral position while the N a l detector was placed as shown in Fig. 2. During the degassing period, the very first acquisition revealed a spectrum (Fig. 5) dramatically different from the background one. During some acquisition sequences sample t e m p e r a t u r e was changed in the range from 350 to 750 K without any detectable variation in the 7 spectrum. Samples were kept 52 days under vacu u m before hydrogen admission in order to study extensively the photon emission. After this too prolonged treatment, the system did not produce energy. It may be t h a t the two phenomena, extended photon emission and energy production, are alternative, and mutually exclusive. T h e behavior over time of these spectra was similar to the one observed in the first experiment; 26 days after the hydrogen introduction the 7 spectrum returned to the background level. During this time period the spectra acquired with the H P G e detector only allowed the determination of the energy of the most intense peak due to the low efficiency of the detector and to the bad geometry imposed by t h e presence of t h e neutron shield. Figure 6 shows one of the acquired spectra, relative to the energy range of interest. T h e detector was calibrated by using n a t u r a l background peaks, and the energy measurement of the observed peak is 661.5 ± 0.8 keV. It can be observed in the insert of Fig. 5 t h a t the C o m p t o n shoulder is in the
74
1500
1000
vw 500
1000
1500
2000
2500
£(keV)
500
A
Measured spectrum Background spectrum
V**^-*^ 500
1500
1000
2000
2500
E(KeV) Figure 5. Second experiment: background and measured spectra, at the beginning of gamma measurements. The background spectrum is a mean of 20 acquisitions (live time 18,000 s) and the measured one is a mean of 30 acquisitions. The curve in the small picture is the difference between measured and background spectrum.
70
First measure Mean on 30 measures one week later Mean on 100 measures one month later
60 50
B 40 c 20 «»***•»••*.*
••.»f.:
>*.*»«*.»*•'•* I**V*!***.*»t.U*
10-1
0 650
660
670
680
690
700
E(keV) Figure 6. Second experiment: three measured spectra obtained with the HPGe detector. The first spectrum is a single acquisition (live time 12,000s), taken at the beginning of gamma measurements.
expected position (487 keV) and the energy of the left peak corresponds to the back-scattered one (184keV). The experimental results show in an unambiguous way the existence of processes involving photon emission, obtained in experimental conditions for which such processes are unexpected and unexplainable within the frame of present physical theories. In fact the observed Nal and HPGe spectra are different from those produced by neutrons impinging on the detectors. 9 ' 10 We maintain that the phenomenon is imputable to Ni (and not to the cell walls
75
and to the heater) because it is not observed without a suitable Ni sample. An accurate determination of energy was obtained only for the lower energy peak. For this reason, a search on two database (Lawrence Berkeley National Laboratory - GAMQUEST program and Brookhaven National Laboratory - National Nuclear Data Center - NUDAT program) has been performed in the energy range 660.0-663.0 keV in order to find a possible nucleus responsible for the emission. In this region, we have found only heavy radioactive nuclei (from 67 Ge to 243 Am) whose presence is difficult to justify. The only exception is 50 Mn whose strongest lines are at 1098.0 and 783.3 keV, which were not observed. Moreover, a possible nuclear excitation of a Ni isotope has been considered. A unique coincidence was found: 59 Ni from an highly excited emitting level (level energy 7164 keV and Jpi = 19/2, 21/2-) which is very hard to justify, because the cascade gamma emission to the ground level was not observed. Finally, in a third experiment with new Ni samples there was no difference in radiation emission during the degassing period and the H atmosphere, as shown in Fig. 7, almost all the time.
600
V*. 200-
V 1000
\
1500 E(keV)
2000
2500
500
1000
1500 £(keV)
2000
2500
Figure 7. Third experiment: (a) a spectrum during the degassing and (b) a spectrum in the hydrogen atmosphere.
After the admission of hydrogen, differences in photon emission are revealed only in two very different cases. The first alteration in radiation emission happened in a condition of closed cell (matter cannot be exchanged with the outside). In this condition, a small thermal excitation was made (the electrical power was turned off for a few minutes) causing a photon emission that persisted for less than 10 h. The spectra during this period, in the region of energy of interest, are shown in Fig. 8. Figure 9 shows the differences between these spectra and the previous one. Some weeks later, spontaneous excitation occurred and it persisted unaltered during admission of hydrogen. Again the photon emission increased, this time for a long period of about 3 weeks.
76
!S*A c 3 O
.A
>**>
W^ \
O
\
400-
\ 500 £(keV) Figure 8.
Third experiment: five spectra zoomed in the region of the increasing of emission.
1400 \ ^ 1200^ 1000 400'600 800 1000 12001400 1600 1800 2000 2200 2400 2600 2800
acq!
£(keV)
Figure 9. Third experiment: (a) Differences between spectra during the excitation and far from it. (b) Temporal evolution is shown.
The spectra of this excitation are shown in Figs. 10 and 11. In all these experiments, despite the very different ways and times of emission, the main emitted photon shows a peak at the same energy.
4. Discussion a n d Conclusion We have presented experimental results for photon emission observed in three different experiments performed during a preliminary preparation step of a Ni H heat production system. In this section, we briefly reconsider the main phenomena detected in all these experiments.
77 Mean
i«W
Mearv
2500
Figure 10. Third experiment: spectra are acquisitions of 12,000 s during the excitation and after, a mean over a week is performed.
lStw
-
mean
no -i
Difference m e a n ^
too -
Dilference m e a n ^ 2 „ a w - m e a n ^
wav
Dilference m e a n ^
3rdw
- mean M o v
DiHerence m e a n ^
4lhw
- mean prev
90 • 80 70 60 50 40 30 20 10 "
0
LJLJLV^
,'iM
. I. U„^uiL*^,. ,^'i
600
800
1000
1200 1400 1600
1800 2000
2200 2400
2600 2800
E(keV) Figure 11.
Third experiment: differences between spectra shown in Fig. 10 and a previous weekly
4.1. First
Experiment
A fast loading of hydrogen was observed (a typical loading is shown in Fig. 12) which involved large gas quantities. Radiation was emitted in an early time with peaks that showed low intensities for few days and extremely low intensity for 40 days. It disappeared before the beginning of energy production. No neutron emission was detected during this experiment. Moreover, excess heat was observed 11 " 13 that persisted for 22 days with a energy production of about 35M.I. After the experiment, nickel samples were analyzed with a scanning electron microscope (SEM) to investigate morphological and elemental difference from a blank sample. The measurements were performed by using an
78
Time (h)
Figure 12. 1.8 h.
First experiment: a fast loading, large decrease of pressure with characteristic time of
energy dispersive X-ray system for elemental analysis. The most interesting result is shown in Fig. 13: new elements (Cr and Mn) were detected in a wide region of a sample.
200 x 200 urn 2
Sample 1B
Cr„, 150
Mn k ,
•
*
*
*
*
*
;
\
Fek,
/
,
*s>^* <
"'
E(keV) Figure 13. First experiment: surface analysis of a nickel sample performed by using SEM X microprobe (electron gun at 20 kV) on 200/xm 2 X 200 /an 2 windows. Empty circles indicate an analysis of an unaltered surface on the nickel sample, which is indistinguishable from analysis on a blank sample. Full squares indicate an analysis on a wide altered region. The large peak on the right comes from nickel.
79
4.2. Second
Experiment
A slow loading of hydrogen was observed (a typical loading is shown in Fig. 14) which involved small gas quantities. Radiation was emitted early in the run with peaks that showed high intensities for many days, they decreased slowly and persisted for 78days (26 in H atmosphere). No neutron emission or excess heat production were detected during this experiment. No quantitative changes were detected in surface analysis. Pressure 'sample
415-.
«*
770 760
410-
750 405-
740
- 730 - 720 - 710 - 700
l, 400O.
|
395390-
'
1
6
Figure 14. of days.
§ °-
690
385380-
~ CO
•"
'
' 1 --""
-'-'
—
r
7 8 Time (days)
'
—,—,
»"
9
680
670 10
Second experiment: a slow loading, small decrease of pressure with characteristic time
4.3. Third
Experiment
A very slow loading of hydrogen was observed which involved very small gas quantities (few 10s of mbar, characteristic time of weeks). Radiation was always present with peaks that showed low intensities. A thermal excitation provoked a transient increasing in radiation emitted. A spontaneous increasing persisted for weeks. No neutron emission or excess heat production was detected during this experiment. In our opinion, these experiments show the complexity of phenomena involved in the physics of the Ni-H system. Further investigations are needed in order to throw light on these phenomena. Acknowledgments We are grateful to the current and the past director of the Siena physics department L. Moi and A. Scribano for their support. We wish to thank P.G. Bergamini, L. Daddi and P.G. Sona for helpful suggestions and discussions. The technical support of C. Stanghini was crucial for the realisation of the experimental apparatus.
80
References 1. S. Focardi, R. Habel, and F. Piantelli, Nuovc Cimento A 107, 163 (1994). 2. S. Focardi, V. Gabbani, V. Montalbano, F. Piantelli, and S. Veronesi, Nuovo Cimento A 111, 1233 (1998). 3. S. Focardi, V. Gabbani, R. Habel, V. Montalbano, F. Piantelli, G. Salvetti, E. Tombari, and S. Veronesi, Status of cold fusion in Italy, in B. Stella (ed.), IV Proceedings of Siena workshop (Siena, 24-25 March 1995). 4. S. Focardi, V. Gabbani, V. Montalbano, F. Piantelli, and S. Veronesi, Atti Accad. Fisioc. Serie XV, Tomo XV, 109-115 (1996). 5. A. Battaglia, L. Daddi, S. Focardi, V. Gabbani, V. Montalbano, F. Piantelli, P.G. Sona, and S. Veronesi, Nuovo Cimento A 112, 921 (1999). 6. A.B. Garg, R.K. Rout, M. Srinisavan, T.K. Sankarnarayanan, A. Shyam, and L.V. Kulkarni, in Proceedings of the ICCF-5 (Monte-Carlo, Monaco, 9-13 April 1995), and references therein. 7. A. Shyam, M. Srinisavan, T.C. Kaushik, and L.V. Kulkarni, in Proceedings of the ICCF-5 (Monte-Carlo, Monaco, 9-13 April 1995), and references therein. 8. S. Focardi, V. Gabbani, V. Montalbano, F. Piantelli, and S. Veronesi, Atti Accad. Fisioc. Serie XV, X V I I I 109 (1999). 9. O. Hausser, M.A. Lone, T.K. Alexander, S.A. Kushneriuk, and J. Gascon, Nucl. Inst. Meth. 14, 115 (1961). 10. J.P. Hirvonen and R. Lappalainen, in J.R. Tesmer and M. Nastasi (eds.), Handbook of modern ion beam material analysis (Material Research Society, PA, USA), p. 609 11. E.G. Campari, S. Focardi, V. Gabbani, V. Montalbano, F. Piantelli, E. Porcu, E. Tosti, and S. Veronesi, in F. Scaramuzzi (ed.), Proceedings of the ICCF8 Conference, Vol. 70, 2000, p. 69 12. E.G. Campari, S. Focardi, V. Gabbani, V. Montalbano, F. Piantelli, and S. Veronesi, in A. Lorusso and V. Nassisi (eds.), Proceedings of the Workshop TESMI (Lecce, 2002), p. 35. 13. E.G. Campari, G. Fasano, S. Focardi, V. Gabbani, S. Lorusso, V. Montalbano, F. Piantelli, C. Stanghini, and S. Veronesi, in J. Biberian (ed.), ICCF11, to appear on Conference Proceedings, 2004.
SUPERWAVE REALITY*
IRVING DARDIK Here I present the elegant reality that is the natural universe. All existence is waves - only waves. This entirely new understanding of waves - what I call SuperWaves - is the single universality that generates the entire natural universe of motion, of order and of matter, space, and time. SuperWaves is not a theoretical model or mathematical law about nature; nor is it a hidden reality within nature; it is the simple reality that is nature. 1 - 4 1. Motion is SuperWaves All motions and all changes are only waves. To create complex features in an existence that is comprised only of waves, waves must wave. All changes are changing. Waves do not move in straight lines. Waves move only within waves and contain waves, as an inherent continuum of wave motion in wave motion. This new understanding of waves as SuperWaves is an entirely new understanding of motion. Constant uniform, or linear, motion does not and cannot exist. Waves, which are in motion on one scale, are in motion, moving up and down on another scale. This is an innate continuum of nested scales within scales, unbroken fractals within fractals. Linear frequencies, linear amplitudes, and linear interference patterns of superposition do not exist because nature is SuperWaves. Rather, in SuperWaves, smaller waves repeat in non-linear frequencies, climbing up and down the trajectory of the larger wave. In turn, the larger wave is moving with its own progressively changing frequencies and amplitudes within a yet larger wave - ad infinitum. Frequencies and amplitudes can now be recognized as existing as a seamless continuum, generating in all directions within and across scales.
2. SuperWaving Motion is Order The order of nature exists because of the unbroken fractal order of SuperWaves. Towards the peak of the carrier wave, spiraling waves are accelerating and are most concentrated. The peak contains the highest super waving frequencies and amplitudes of inner waves, whose stability is maintained at a maximum by the peak of the carrier wave. The reverse occurs toward the trough of the carrier wave: the frequencies and amplitudes of the inner waves decrease; they spread out and disperse in all directions as change and become relatively unstable, susceptible "Irving I. Dardik June 10, 2005. 81
82
to perturbation. As SuperWaves are the stuff of nature; and as SuperWaves are intrinsically self-similar; we can now understand why nature is fractal in form, at all scales. Nature exhibits only relative degrees of order; absolute chaos does not exist. The puzzle of action at a distance, or non-locality, is explained by the Super Wave order of nature. A change in the form of a carrier wave will cause changes in the form of inner waves, simultaneously within and across scales. The reverse occurs as well. Changes of inner waves can simultaneously change the form of the carrier wave, depending on the degree of stability of the inner waves. I call this simulcausality. Science has looked for absolute causality, or determinism, but has failed to find it. Redefining action at a distance as simulcausality explains this failure. The reason is that waves waving are always changing, never being precisely circular or linear; as they are constantly influencing each other, they cause further change. Nature exhibits no invariance or absolute constancy. This explains why all linear measurements are inexact and approximate, and ultimately exhibit non-linear complexity. Science separates frequencies and amplitudes as linear dimensions, and then superimposes them to explain interference patterns. From the perspective of SuperWaves, interference patterns are explained by the (non-linear) continuum of amplitude and frequency, which is the same phenomenon as action at a distance and causality, which is simulcausality. This unbroken fractal motion of SuperWaves generates the order of nature. 3. The Order of Superwaving Motion is Matter, Space, and Time The compression of waves in the peaks of SuperWaves exhibit confined stability which manifests as matter, at all scales. At the smallest scale, matter is the confined compressed wave packet, termed a particle. At higher and higher scales of SuperWaves, the compression of clusters creates the stability that is an atom, a molecule, an organism, an ecosystem, Earth, the Solar System, our galaxy, galaxy clusters, to the whole universe itself. At each scale, SuperWaves organize and bring relative coherence to the inner waves, in seamless fractally nested jumps - this is relative order. Conversely, the gaps between particles or object masses that we presently perceive as space are regions of SuperWave dispersion - this is relative disorder. Matter and space are therefore different manifestations of the same SuperWave continuum; this applies to matter and space on all scales. The forces of nature - the weak and strong forces, electromagnetism, and gravity - are also manifestations of SuperWaves. Gravity and the strong force are the attractor peaks of carrier waves, or matter, with gravity being at a higher scale than the strong force, fractals of each other. The weak force and electromagnetism are also fractals of each other, being the repulsion or dispersal of waves which is space. The understanding of SuperWaves gives a new understanding of how organization comes about in nature. Matter is described above as the relatively stable compression of waves at the peak of a SuperWave. The process of waves waving within waves, moving toward the peak in continuous scalar jumps, is what science calls the emergence and evolution of organizational order. The process of
83
dispersal and flattening of Super Waves, also occurring as inherent continuous jumps, manifests as Cartesian order of parts and what science calls thermodynamic entropy. Just as evolution and entropy are processes of change as a result of moving towards and away from the peak, so too is time the outcome of waves waving. Waves waving is change, the irreversible process that is time. Time is perceived differently, depending locally on the scale of waves waving. SuperWaves is matter, space, and time. 4. Conclusion Science has perceived nature to be a universe of matter in motion, governed by mathematical laws of order. In reality, nature is SuperWaves, whose motion is the order of the universe that is matter, space, and time. The recognition of the SuperWave universe allows for the investigation and understanding of the individual parts in the true context of their indivisible collective wholeness. The scientific, mathematical laws of nature are in fact partial abstractions to a linear ideal of the SuperWaving order present in different scales of the universe. SuperWaves provides a new understanding of how to go about understanding the universe. The received understanding of the universe is that it is too complicated to understand all at once. Therefore, the scientific method is forced to try to understand nature piece by piece. In other words, science treats nature as if it were discontinuous. Investigating nature from this perspective means that inherent continuity cannot be identified. However, from the perspective of SuperWaves, the universe is recognized as being seamlessly and exclusively a wave universe in which everything is connected to, and affects, everything else all at once while everything is changing. This order, the inherently continuous pattern of motion, is the true indivisibility (a-tomos) of nature. The universe is the manifestation of this order, neither random nor uncertain. The recognition of the SuperWave universe allows for the investigation and understanding of the individual parts in the true context of their indivisible collective wholeness. The universe is ultimately not a material universe. In reality the universe is a motion universe, where matter is a consequence of wave motion. How the universe works is what the universe is made of. What remains to be understood is a new recognition of all accumulated and future knowledge in light of SuperWaves. So I begin here by going back to the beginning of all our thinking, all our understanding about the nature of the universe. The universe is simply SuperWaves. References 1. 2. 3. 4.
I. Dardik, Superesonant wavenergy theory, Monograph 1-21 (1989). I. Dardik, The great law of the universe, Cycles, 44, 265-277 (1994). I. Dardik, The law of waves, Cycles 45, 49-60 (1995). I. Dardik, The origin of disease and health, heart waves: the single solution to heart rate variability and ischemic preconditioning, Frontier Perspectives 6, 18-32 (1997).
EXCESS HEAT IN ELECTROLYSIS E X P E R I M E N T S AT ENERGETICS TECHNOLOGIES
I. D A R D I K , T . ZILOV, H. B R A N O V E R , A. E L - B O H E R , E. G R E E N S P A N , B . K H A C H A T U R O V , V. K R A K O V , S. LESIN, A N D M. T S I R L I N Energetics
Technologies,
P. O. Box 3026, Omer Industrial E-mail:
[email protected]. co
Park,
Omer,
Israel
Using electrolytic cells driven with Dardik's modified Superwaves, significant amounts of excess heat were obtained in a number of experiments using Pd foil cathodes that were prepared by by Dr. Vittorio Violante of ENEA in Frascati, Italy. The most successful of these experiments generated excess heat a couple of times: (1) Approximately 5 h into the first loading of deuterium into the Pd cathode - giving an average power gain of ~2500% during 17 h. The average current density was 7 m A / c m 2 . (2) The same foil was deloaded after the excess heat generation stopped for no apparent reason and than loaded again. After 16 h of loading excess heat was generated again at an average level of ~1500% for 80 h. The average current density was 8.4 m A / c m 2 . At the end of the two experiments the effective tritium concentration in the electrolyte was ~750% of its pre-experiment level. The total amount of excess energy generated is approximately 1.1 and 3.5 MJ in, respectively, the first and second experiments. This amount of excess energy corresponds to, respectively, ~4.8 or ~15.3keV per Pd atom. The corresponding average specific power is 71 or 48 W per gram Pd. For comparison, the average specific power in commercial nuclear fission reactors is between 20 and 40 W per gram uranium. The cathodes were investigated before and after the electrolysis using a number of probing techniques, including AES, SEM-EDS, TEM, and SIMS. Significant amount of low Z contaminants were found on its surface, extending to a depth of 100s of Angstrom. Their origin appears to be the lubricant used for rolling the foil in the pretreatment process. Their presence prohibited detecting nuclear reaction products with acceptable certainty on and near the surface. No transmutation products were found at deeper layers. However, no measurement of He inventory was attempted.
1. Introduction In ICCF-10, Energetics Technologies (ET) described four approaches it is experimenting with for generation of LENR: 1 electrolysis (EC), glow-discharge (GD), gas loading in catalyst cells (CC) and a combination of ultrasonic wave excitation with electrolysis. All these experiments involve use of so-called "waves-waving-waves" or Superwaves for driving the processes. The idea of Superwaves for enhancing the probability of LENR was first proposed by Dr. Irving I. Dardik based on his vision of nature described in the accompanying paper. 2 The purpose of the present paper is to describe recently performed electrolysis experiments that resulted in significant excess heat generation. 84
85
Starting from a brief description of the Superwaves used in the electrolysis experiments (Section 2), we'll describe the electrolytic cells used for the experiments (Section 3), the Superwave effect on deuterium loading in the P d cathodes (Section 4), the results of the three most successful excess heat generating experiments (Section 5), results of tritium measurements (Section 6), and results obtained from material analysis of the P d foils before and after the electrolysis (Section 7). Section 8 summarizes the obtained results.
2.
Superwaves
Figure 1 illustrates the principles of Superwaves used for the electrolytic cell experiments. Three levels of modulation were used for these experiments. T h e figure shows a t o t a l of four levels of modulation. T h e amplitude, A\, and frequency, u>[, of each of the super-imposed waves are adjustable.
3. Electrolytic Cells Figure 2 shows the overall layout of the electrolytic cells designed and constructed by E T . T h e cathode is 8-cm long ( 6 c m in effective length), 0.7-cm wide and 50 or 100-/xm thick P d foil. Two platinum foils of similar dimensions - 2 0 m m x 80 m m x 0.1mm, are used for the anode. They are located 5 m m from each side of the cathode. T h e c a t h o d e - a n o d e assembly is immersed in an electrolyte made of 0 . 1 1 M LiOD in D2O. T h e electrolyte and the c a t h o d e - a n o d e are inside a cell made from two concentric aluminum cylinders with alumina powder thermal insulation in between the cylinders (Fig. 2). T h e cell is immersed in a constant t e m p e r a t u r e water b a t h usually set at 2.5 ± 0.25°C. Three sensors monitor the t e m p e r a t u r e in different locations in the cell. The cell has an external recombiner. Presently, there are six electrolytic cells working in parallel; three cells per water b a t h . Each dedicated computer drives three cells. T h e same computer also collects, stores and analyzes the experimental data. Temperatures readings are done at a rate of 25scans/s, whereas voltage and current readings are taken at a rate of 50,000 scans/s. T h e cathode resistance is measured to infer the level of deuterium loading. A Labview program was developed to perform all these functions. A typical Superwave generated by this computer control system is given in Fig. 1. More t h a n one hundred of P d foils have been used in our experiments so far. Dr. Vittorio Violante of the Frascatti research center in Italy provided a significant number of the foils. T h e foils received from Dr. Violante were degreased and annealed at 870° C for 1 h. Then they were etched first with nitric acid of 65-67% for l m i n and then for 1 min in Aqua Regia 1:1 water solution. Following t h a t the foils were rinsed four times in heavy water, twice in 95% ethanol, and once in ethanol absolute. Finally the foils were dried in vacuum at ambient t e m p e r a t u r e for 24 h.
86 F0(f) = A0smz Hi
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Figure 1.
Principles of Superwave formation.
87
Figure 2.
Schematic layout (left) and a photo (right) of the ET electrolytic cells.
Excess heat is measured using an isoperibolic calorimeter. Each electrolytic cell was calibrated using an electrical heater. A typical calibration curve is given in Fig. 3. The "AT" of Fig. 3 is T4 — T5, where the temperatures are measured in the locations shown in Fig. 2. The accuracy of this calorimeter is estimated to be 1-2%.
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Figure 3.
A typical calibration plot of the calorimeter of the electrolytic cells.
4 . S u p e r w a v e Effect o n D e u t e r i u m L o a d i n g in P a l l a d i u m C a t h o d e s
A set of experiments was performed to investigate the effect of current modulation on the rate of deuterium loading into the Pd. Figure 4 shows the three levels of
88
wave modulation considered, while Figs. 5-7 show loading rate dependence of foil No. 56 on the modulation level. A clear and reproducible correlation is observed; the higher the level of modulation, the faster is the deuterium-loading rate.
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5. Excess Heat Generation Significant amount of excess heat was generated by two of the foils: foil Nos. 56 and 64. Both of these foils were prepared by Dr. Violante. The rest of this paper will focus on describing these two successful experiments. Figures 8 and 9 show the Superwaves used in these experiments. The excess heat in foil No. 56 was generated in the fourth loading. It started after 80 h of loading and lasted for approximately 300 h. Figure 10 shows the evolution of input and output power during this period and the excess power generated. The average input, output and excess power generated during the period are estimated to be, respectively, 3.9, 6.6, and 2.7 W. The total excess energy generated is estimated to be 3.1 MJ.
90
1 2 3 3 2 1 1 2 3 3 2 1 2 3 2 1 2 3 3 Level of modulation
Figure 7.
Resistance ratio dependence on modulation level and current density (foil No. 56).
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Foil No. 64 started generating excess heat approximately 5 h into the first loading of deuterium into the Pd cathode - giving an average power gain of ~2500% during 17h. The average current density was 7mA/cm 2 . The evolution of input and output power during this part of the experiment is given in Fig. 11 The average input power was ~0.74W while the average output power was ~20W; the peak power reached ~34W. The total energy invested in this cell up to the termination of excess heat generation was 33 kj while the excess energy accumulated was 1.1 MJ; that is a gain of ~33. The temperature evolution during the excess heat generation, as measured at different points in the system, is shown in Fig. 12. As the outer wall temperature,
91
Figure 9.
ETE-64 first event; average current 50mA; Peak - 116 mA (13.8mA/cm 2 ).
Figure 10. Evolution of net input power (Pi n e t), output power (P o u t) and excess power (P x ) in experiment with foil No. 56.
T5, is nearly constant, the temperatures at inner locations evolve with time in a similar shape to the output power. The time evolution of the cell voltage and current during the excess heat generation is shown in Fig. 13. The cell current is pretty stable; it has the pattern of the Superwave shown in Fig. 9. The cell voltage, on the other hand, exhibits a significant increase and significant random fluctuations during the period of excess heat generation. Also very fluctuating during this period is the Pd cathode resistance ratio, R/RQ, shown in Fig. 14. The average deuterium loading during this excess heat generation was only ~ 0.8 D per Pd atom. The same foil was deloaded after the excess heat generation stopped for no apparent reason and than loaded again. After 16 h of loading, excess heat was initiated again and lasted for ~80h. The evolution of input and output power during this part of the experiment is given in Fig. 15. The average input power
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was ~0.72\V while the average output power was ~12\V giving an average power gain of 1500%. Figure l(i shows the rale of accumulation of excess energy in this experiment. The total excess energy accumulated was 4.6 MJ, not including the energy generated between ~28 and ~33 h since this experiment was started. In this period there was an anomalous jump in the cell voltage and an anomalous behavior of the current, as illustrated in Fig. 17. The reason for the anomalous current behavior is not understood. Coinciding with the ramp up of the cell voltage there was a ramp up
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of the in-cell temperatures, as illustrated in the upper plot of Fig. 17. Figure 18 shows that the R/RQ ratio strongly oscillated also during the second session of excess heat generation by foil No. 64. After termination of the excess heat generation we tried deloading and reloading foil No. 64 a couple of more times but did not succeed in generating additional excess heat. The R/Ro evolution during these extra trials is shown in Fig. 19.
Figure 15. Evolution of net input power (Pi„ot) and output power (Pout) in the second loading experiment with foil No. 64.
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Figure 16. Evolution of input energy, output energy and excess energy in the second session of heat generation from foil No. 64.
6. Tritium Measurement At the end of the experiments with foil No. 64 the tritium concentration in the electrolyte was measured in ENEA by Dr. Violante using Packard Liquid Scintillation Analyzer model 2560 TR/XL. The measured tritium level was ~250% of background level. Taking into account that ~625cm 3 of D 2 0 has been added to the electrolytic cell during the experiments with foil No. 64 to make-up for evaporation, that the initial inventory of D2O was 230cm 3 , and assuming a T D O / D 2 0 evaporation rate of ~1.0, we are estimating that the effective tritium concentration
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is ~750% of background. This amount of tritium corresponds to < 1 J - negligible as compared with the 5.7 MJ of total excess energy generated with foil No. 64.
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7. Cathode Material Analysis The following analytical procedures were used to examine the Pd foils before and after the electrolysis: • Auger Electron Spectrometry (AES), • Time Of Flight Secondary Ion Mass Spectrometry (TOF-SIMS), • Scanning Electron Microscopy X-Rays Energy Dispersive Spectrometry (SEM-EDS), • Transmission Electron Microscopy (TEM). A characteristic feature of all samples of Pd foil analyzed after rolling and vacuum annealing is the presence of black spots on their surface. For example, Figure 20 shows the surface of Pd foil Nos. 63 and 64 after rolling and annealing at 870°C. Both foils were obtained from the same Pd batch and same rolling and other pretreatment procedures; foil No. 64 gave excess heat while foil No. 63 did not. The concentration of these spots varies from sample to sample; their sizes and structures are different. Elemental analysis of this spot is given in the table and spectrum of Fig. 21. The principal component is carbon. Sulfur and oxygen are also present. Very probably, their source is the lubricant used for Pd rolling. We guess that the observed spots are products of high-temperature pyrolysis of the lubricant. At present, there is no information on the phase composition of these spots and on their effect on the process of palladium deuteration. In addition to the above-mentioned microspots, there is always a thin adsorption layer on the Pd surface containing carbon, oxygen, and chlorine, as illustrated in Fig.
97
Figure 20.
SEM-EDS analysis of foil Nos. 63 (right) and 64 (left) after rolling and annealing.
22. The thickness of this layer does not exceed 60 A and its composition is rather sensitive to the kind of air contaminants, such as sulfur-containing compounds. Rolled and annealed Pd foils are characterized by a high dislocation density (as illustrated in Fig. 23) 3 x 1010 and 6 x 1010 dislocations per cm 2 in, respectively, foil Nos. 63 and 64. An attempt was made to detect isotopic shifts in the nuclei of elements present in the Pd cathodes by performing a layer-by-layer SIMS analysis. We analyzed
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AES profile of selected elements as a function of depth in foil Nos. 63 and 64.
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TEM images of dislocation density in foil Nos. 63 (right) and 64 (left).
the previously described foil No. 64, virgin foils as well as foils that underwent electrolysis but did not generate excess heat. It was found that: (1) there is a 500-600 A deep zone on the surface of all investigated samples that contains numerous impurities including impurities of organic origin, as illustrated in Fig. 24. These impurities, making unknown composite ions, interfere with the analysis of isotopic shift in this near-surface region. (2) During the foil exposure to air, an exchange of D by H occurs in the absorption zone. Several days after the electrolysis - when the SIMS analysis is performed, the D/H ratio on the foil surface is typically smaller than 1:10.
99
In Fig. 24 the H/D ratio is ~100. The form of the H + ions concentration versus depth is typical of diffusion from a fixed source into a semi-infinite body. (3) No significant isotopic shift was detected at Pd layers deeper than 500-600 A. We have analyzed more than 20 positive and negative ions. It should be mentioned, nevertheless, that we were not set to detect helium.
0
100
200
300
400
500
600
Depth A Figure 24.
AES profile of selected elements as a function of depth in foil Nos. 63 and 64.
The character of elements distribution over the Pd foil surface shown in Fig. 25 testifies to the preferential adsorption and, hence, absorption of most elements along grain boundaries. Only platinum, whose maximal concentration was found within the grain body, is an exception.
Figure 25. SIMS images of foil No. 64. Scanning for concentration of (a) D, (b) isotopes, and (d) 1 2 5 P t . Scale bar is 10 fan.
32
S , (c) all
100
Figure 26 illustrates the plastic deformation of the Pd foil as a result of the absorption of deuterium that causes a considerable increase in the lattice volume. Since the (111) plane is the principal slip plane during plastic deformation of Pd, the disorientation of slip planes in adjacent grains allows us to evaluate the disorientation of Pd grains. As Fig. 26 shows, the disorientation of Pd grains is rather significant.
*
Figure 26. Plastic deformation of Pd foil No. 64 caused by deuterium absorption. Left: planes of sliding (111) are visible. Right: Enlargement of area shown by arrow.
8. Summary Dardik's modified Superwaves were found to significantly accelerate the loading of deuterium into the palladium cathode of electrolytic cells. Significant amounts of excess heat were obtained in a number of experiments using a couple of Pd foil cathodes that were prepared by by Dr. Vittorio Violante of ENEA in Frascati, Italy. The most successful of these experiments, done using foil No. 64, generated excess heat a couple of times: (1) Approximately 5h into the first loading of deuterium into the Pd cathode - giving an average power gain of ~2500% during 17 h. The average current density was 7mA/cm 2 . (2) The same foil was deloaded after the excess heat generation stopped for no apparent reason and than loaded again. After 16 h of loading excess heat was generated again at an average level of ~1500% for 80 h. The average current density was 8.4 mA/cm 2 . At the end of the two experiments the tritium concentration in the electrolyte is estimated to be ~750% of its pre-experiment level. The total amount of excess energy generated is approximately 1.1 and 3.5 MJ in, respectively, the first and second experiments. This amount of excess energy corresponds to, respectively, ^4.8 or ~15.3keV per Pd atom. The corresponding average specific power is 71 or 48 W per gram Pd. For comparison, the average specific power in commercial nuclear fission reactors is between 20 and 40 W per gram uranium.
101
Excess heat was also generated during the fourth loading of foil No. 56. It started ~ 8 0 h following loading initiation and lasted for approximately 300 h. T h e average input, o u t p u t and excess power generated during t h e period are estimated t o be, respectively, 3.9, 6.6, and 2.7 W. T h e total excess energy generated is estimated to be 3.1 M J . Table 1 summarizes the description of the three most successful experiments and the obtained results. Table 1.
Summary of the most successful electrolysis experiments.
Experiment number Loading cycle number Loading time (s) Excess heat generated (%) Duration of excess heat generation (h) Excess energy generated (MJ) Specific excess heat ( W / g Pd) Specific excess energy (keV/Pd atom)
56 4 80 80 300 3.1 11 13.5
64a 1 5 2500 17 1.1 71 4.8
64b 2 16 1500 80 4.6 62 20 (24.8)
After the experiments the cathodes were investigated using a number of probing techniques, including AES, SEM-EDS, T E M , and SIMS. Significant amount of low-Z contaminants were found on their surface, extending to a depth of dozens of Angstrom. One origin of the contaminants appears to be the lubricant used for rolling the foil in the pretreatment process. T h e second origin appears to be adsorption of air constituents by the P d surface. T h e lubricant stains are of various sizes and configurations and are present on the surface of all foils b o t h before and after the electrolysis. Annealing at 850°C does not fully remove the lubricant's components from the P d surface. T h e density of dislocations and the average size of grains in foil No. 64 are approximately twice those in foil No. 63. It is not clear whether or not these differences contributed to the difference in excess heat generation. Nuclear reaction products were not detected, with sufficient certainty, on and near the surface of the foils t h a t generated excess heat. Contributing to this uncertainty is the high concentration of contaminants. However, no He measurement has been a t t e m p t e d . Acknowledgment This work was fully funded by Mr. Sidney Kimmel. References 1. I. Dardik, H. Branover, A. El-Boher, D. Gazit, E. Golbreich, E. Greenspan, A. Kapusta, B. Khachaturov, V. Krakov, S. Lesin, B. Michailovitch, G. Shani And T. Zilov, Intensification of low energy nuclear reactions using superwave excitation, in Proceedings of the 10th International Conference on Cold Fusion ICCF-10 (Cambridge, MA, August 2003). 2. I. Dardik, Superwave reality, These Proceedings.
"EXCESS HEAT" D U R I N G ELECTROLYSIS IN P L A T I N I U M / K 2 C 0 3 / N I C K E L LIGHT WATER S Y S T E M
J. T I A N , L. H. J I N , Z. K. W E N G , B . S O N G , X. L. Z H A O , Z. J. X I A O , G. C H E N , A N D B. Q. D U Changchun
University
of Science and Technology, No. 7989, Weixing Road, Jilin 130022, People's Republic of China Tel/Fax: +86-431-5337696(o)/+86-431-537304 7(1) E-mail:
[email protected];
[email protected]
Changchun,
The characteristic variation of heating coefficients (k = AT/AP°C/W) of Pt(H)-Ni electrolytic system with K2CO3 and Na2CC>3 solutions was studied in both situations of electric and electrolytic heating, respectively. The results in equilibrium revealed that there was an obvious difference of k in electrolytic-heating (Ak m 30°C/W, k^2co3 > ^Na 2 C0 3 ) between these two systems, whereas there was a little difference of k in electric heating (Ak « 2 ° C / W , /CK 2 CO 3 < fcNa2C03 between them. "Excess heat" of about 2.5 x 10 4 J was produced during electrolysis of K2CO3 solution over l d a y of electrolysis. The differences of K2CO3 solution after electrolysis in the potential of hydrogen value (ApH = 0.15) and in absorbency (AA = 0.108) implied that some new Ca 2 + might have formed in the electrolytic system.
Key words: Pt(H)-Ni System; Light water electrolysis; Excess heat; pH value; Absorbency
1. Introduction In "Cold Fusion" or "Condensed Matter Nuclear Science" research, light water has often been referred as a control for excess heat, meaning it is assumed that light water will not produce heat. Is there really no abnormal behavior in light water electrolysis? One possible negative answer was from V.C. Noninski, when he did experiments on electrolysis with a nickel cathode in K2CO3 solution. 1 By comparing with the difference of heating coefficients, k, which is defined as the temperature rise over the unit input power, between two different systems (K2CO3 and Na2C03) and two different heating manners. Noninski concluded that there exists some "excess heat" in K2CO3 electrolysis; the power ratio (output/input) was more than 160% when the ke = 50°C/W (electrolysis heating) and kT = 30°C/W (resistance heating). 102
103
2. Experimental 2.1. Apparatus
and
Materials
Components include: DC power supplies (WYJ-302, Shanghai Apple Instrument Ltd., PRC); constant temperature magnetic stirrer (85-2, Shanghai Nanhui Electrical Apparatus, PRC); platinum thermometer (PtlOO, Beijing Glassware Instrument, PRC); pH meter (PHS-25B, Shanghai Dapu Instrument Ltd., PRC); spectrophotometer (722s Shanghai Lingguang Technique Company, PRC); data acquisition system (2700, Keithley Instruments Inc., USA); K 2 C 0 3 and N a 2 C 0 3 for electrolyte (99.95%, Beijing Chemicals Factory, PRC); Electrodes: Pt anode {<j> 0.3mm, I = 20 mm), Ni cathode (I = 254 mm, w = 6.09 mm, d = 0.09 mm, Beijing Nonferrous Metals Factory, PRC).
2.2. Experimental
Setup
Figure 1 is a schematic of our experiment. The electrodes, electrolyte, resistance heater, Pt 100 thermometer and the magnetic stirrer are exactly the same in both experimental and control cells. The parameters in experiment such as electrolytic current, the stirrer speed are basically the same as in Noninski's experiment. However, some improvements were made in our experiment: The Ni cathode was covered by a section of glass tube (about 11 cm in length) to prevent the hydrogen released from cathode from meeting the oxygen from the anode; Some thermal blocking materials were wrapped up surrounding the system to prevent the effect of ambient temperature on the system thermal qualities.
Figure 1. Schematic of our device for observing the variation of heating coefficient. 1 and 2, test tube; 3, resistor heater; 4, vacuum-jacketed dewar; 5, magnetic stirring rod; 6, magnetic stirrer; 7, leading wire; 8, heat-barrier material; 9, nickel cathode; 10 and 12, thermometer; 11, palladium anode; 13, rubber stopper; 14, DC power supplier; 15, data acquisition system.
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2.3. Experimental
Process
2.3.1. Electrode Cleaning Anode: In order to get rid of impurities on the surface, the Pt anode was dipped into dilute nitrate (0.2mol/l) for 10 h. It was then washed the surface with distilled water. Cathode: using an Ni anode, Pt cathode, electrolysis was performed at / = 0.08 A for 1 h. The cathode was also washed with distilled water. 2.3.2. K2CO3 and Na^COs Heated by Resistance and Electrolysis The aim of this step is to see how the system temperature changes when the system was heated electrically in the control cell and electrolytically in the test cell. The volume of K2CO3 and Na2CC>3 was 200 ml in both cells; the concentration 0.6mol/l. Five parameters were recorded every lOmin. For resistance heating, the resistance heater circuit was turned on for 24 h. The final stable currents were kept on 447 mA (Na2C03) and 623 mA (K2CO3). For electrolysis, the electrolyte circuit was turned on for same period of time, and the same kind of data was taken at the same intervals. Finally, the constant current power supplies were both kept at 78 mA. 2.3.3. Variations of H+, Ca2+ Concentrations in K2CO3 Solution before and after Electrolysis The purpose of this phase of the experiment was to test whether there might be a new element formed during the electrolysis. Our goal was to assay the elements with ordinary chemical methods, rather than using very expensive instruments such as SEM or SIMS. For the H+, a common pH meter (resolution ± 0.01) and for Ca 2 + , an ordinary spectrophotometer were tentatively used. 2.4. Analysis
of
Results
2.4.1. There were Variations in the Heating Coefficients (k) in both Electrolytic and Electrical Heating Within Different Solutions Figure 2 shows the variations of k in both K2CO3 and Na2CC>3 solutions, respectively. With regard to the Na2C03 experiment, it can be seen that the heating coefficient was always higher in resistance heating than that in electrolyte heating. There is A A; = kr — ke = 2.1°C/W when the system reached equilibrium. The result may become from the heat loss due to the escape of H 2 and O2 during the electrolysis. On the contrary, when the K2CO3 was taken into account, its heating coefficient was always higher in electrolyte heating than that in resistance heating. There is Ak = kT - ke = - 3 0 ° C / W when the system reached equilibrium. According to the same reason as in the consideration of N a 2 C 0 3 solution heating, the behavior of k should be lower in resistance heating than that in electrolysis heating because of the heat loss from the escape of effluent gas. So one possible reason or explanation
105
1 2 3
—
0
200
400
600
800
1000
1200
4
1400
1600
Time (min) Figure 2. The variation of heating coefficients in heating Na2CC>3 and K2C03Solutions (1, K2CO3 heated by electrolysis; 2, Na2C03 heated by a resistor heating; 3, Na2CC>3 heated by electrolysis; 4, K2CO3 heated by a resistor heating).
should be that there might be "anomalous heat" or "excess heat" in the system. When fcr = 15.8°C/W, ke = 45.2°C/W. The result obtained here is 1.5 times higher than in Noninski's experiment. When the total electrical input energy was 1.4 x 104 J, the measured heat output were 3.9 x 104, the ratio of output/input was about 280%. Taking only ke into account, it could be found that the heating coefficient was always higher in K2CO3 electrolysis than that in Na2C03. This implies that maybe K + has an unusual behavior in the experiment.
2.4.2. Comparison of H+, Ca2+ Concentrations in K2CO3 before and after Electrolysis H + : Before electrolysis, the pH of the original solution was 11.33. Near the end of electrolysis, pH reached to 11.48, showing an obvious drift of ApH = 0.15 during the electrolysis. There may be two possible explanations. One is the continuous decomposition of water makes the pH higher, and the other is that H+ was consumed to form another new element. By calculation, the variation of pH caused by water decomposition should be less than 0.01. So the increase of pH value may be due to the latter reason. Ca 2 + : Table 1 shows the absorbency variation of Ca 2 + in K2CO3 solution by spectrophotometry before/after the electrolyzing: Table 1. The absorbency variation of Ca2"1" in K2CO3 solution before/after the electrolyzing. Absorbency Data
Blank (Al) 1.399
Before electrolysis (A2) 1.477
After electrolysis (A3) 1.585
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take Al, A2, and A3 into the standard linear equation: AA = 0.0671C +0.0162.
(1)
We get C0 = 1.1490 x H P 5 mol/1,
Ce = 3.1570 x 10~5 mol/1.
Because there is a trace of Ca 2 + in both the K2CO3 and in the solvent (distilled water), the absorbency of the K2CO3 solution is higher before electrolysis than in the blank value. But this is not the important thing we intend to indicate here. The most important thing in this work is that we got an absorbency increase (AA = 0.108) in K2CO3 after electrolysis. To explanations may be offered. The first is that this is due to the water decomposition, and the second some new Ca 2 + formed in the solution. If the increase of Ca 2 + is from water decomposition, the concentration can be calculated by the following formula: Co x V0 = CY x Vu
(2)
where Co, and VQ are the original concentration of Ca 2 + and the original volume of the solution, respectively; C\ and V\ are the concentration of Ca 2 + and the volume of the solution after electrolysis, respectively. So we can get d = 1.192 x 10" 5 mol/1. But the concentration of Ca 2 + is 3.157 x 10~ 5 mol/1 by actual measurement, which is nearly three times higher than calculated. This phenomenon implied that some new Ca 2 + formed in the solution during the electrolysis. According to the theory proposed by Mills,2 the following possible reactions may exist in the system: ^ K + ^ ^ ^ C a + S.SSMeV
or
fiK + J P -> ^ C a + 10.3MeV.
3. Conclusions "Excess heat" can be repeatedly obtained through the electrolysis in Pt/K^COs/Ni light water system. Comparing the heating coefficients, ke is always smaller than kT in Na2C03 electrolysis; On the contrary the ke is always higher than fcr in K2CO3 electrolysis. Taking the whole experiment into consideration, the ke is always higher in K2CO3 electrolysis than ke in Na2C03 electrolysis. The thermal output energy is 280% more than electrical input energy when the current was 0.078 A. The "excess heat" is about 2.5 x 104 J over 24 h. After electrolysis, the increases of pH value and absorbency in K2CO3 solution (which are, respectively, by ApH = 0.15 and AA = 0.108) implied that some H+ combined with K + to form Ca 2 + .
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References 1. V. Noninski, Excess heat during the electrolysis of a light water solution of K2CO3 with a nickel cathode, Fusion Technol. 2 1 , 163-167 (1992). 2. R. Mills and W.R. Good, Fractional quantum energy levels of hydrogen. Fusion Technol. 28, 1697-1706 (1995).
INNOVATIVE P R O C E D U R E FOR THE, IN SITU, M E A S U R E M E N T OF T H E RESISTIVE T H E R M A L COEFFICIENT OF H ( D ) / P d D U R I N G ELECTROLYSIS; C R O S S - C O M P A R I S O N OF N E W ELEMENTS D E T E C T E D IN THE T h - H g - P d - D ( H ) ELECTROLYTIC CELLS
F R A N C E S C O C E L A N I , A. S P A L L O N E , E . R I G H I , G. T R E N T A , C. C A T E N A , G. D ' A G O S T A R O , P. Q U E R C I A , A N D V. A N D R E A S S I INFN-LNF
Via E. Fermi 40, 00044 Frascati, Rome, E-mail:
[email protected]
Italy
P. M A R I N I , V. DI S T E F A N O , A N D M. N A K A M U R A EURESYS,
Via hero 30, 00129 Rome,
Italy
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F . F O N T A N A , L. G A M B E R A L E , A N D D . G A R B E L L I Pirelli Labs SpA,
Viale Sarca 222, 20126 Milan,
Italy
E . C E L I A , F . F A L C I O N I , M. M A R C H E S I N I , A N D E. N O V A R O CSM SpA,
Via di Castel Romano
100, 00129 Rome,
Italy
U. M A S T R O M A T T E O ST Microelectronics
SpA,
Via Tolomeo
1, 20010 Cornaredo,
Milan,
Italy
In the framework of cold fusion studies one of the most important parameters is the deuterium (D) to palladium (Pd) ratio, D / P d . It is well known that the value of this parameter is related to the normalised resistivity (R/RQ)
of the D - P d system. When at high D / P d ratios (i.e. at low R/RQ
values) some excess heat occurs, the Pd wire temperature increase and, as a consequence, the apparent R/Ro value also increases. This effect might give raise to ambiguous data interpretation: similar results are in fact expected in case of a Pd wire degassing (i.e. decreasing of D / P d ratio). To solve this problem, we developed an innovative procedure and a suitable experimental set-up for the in situ measurement of the Resistive Temperature Coefficient (which is affected only by the real D / P d ratio) during electrolysis. We will report the results on the hydrogen and deuterium loading of thin (50 urn), and long (60cm) Pd wires, immersed in a solution of C 2 H 5 O D (or C2H5OH) and 108
109 D2O (or H2O), with addition of thorium (Th) and mercury (Hg) salts at micromolar concentrations. Evidence of "transmutations" of some elements occasionally present on the Pd surface, and sometimes also in the electrolytic solution, have often been claimed in cold fusion experiments. In the present work, unexpected elements have been detected by high-resolution ICP-MS analysis. Some of these elements have also an isotopic composition different from the natural one.
1. Introduction: Reasons to Measure, In Situ, the Resistive Thermal Coefficient of the Pd Cathode To detect excess heat in cold fusion experiments one of the most important parameters is the deuterium (D) over palladium (Pd) ratio, D/Pd. It is well known that the value of the D/Pd ratio is related to the normalised resistivity (R/Ro) of the D-Pd system: e.g. its maximum value, 2.0, is equivalent (at room temperature) to a D/Pd ratio of about 0.75. By further increasing the D/Pd ratio, the R/RQ starts to decrease. If at high D/Pd ratios (^> about 0.90) there is some excess heat, the Pd temperature increases; as a consequence, the apparent R/RQ value also increases, which is the same result that would be obtained if degassing occurred (a decrease of D/Pd ratio). This effect might give raise to ambiguous data interpretation and fruitless discussions. To try to solve such a problem, we developed an innovative experimental set-up and a specific procedure for the in situ measurement of the Resistive Temperature Coefficient. As such a parameter is affected only by the real D/Pd ratio, any ambiguous interpretation in case of sudden variations of the D/Pd ratio will be avoided. We will show, and discuss in some detail, a test that lasted about 2 days, made during a typical loading-unloading experiment. The results were obtained on deuterium loading of thin (50 ^m), and long (~60cm) Pd wire, immersed in a solution of ultrapure, vacuum distilled and ultrafiltered C2H5OD and D2O with addition of thorium (Th) and mercury (Hg) salts at micromolar concentrations. 2. The Unconventional Frascati-INFN Procedures for Electrolytes, Electrolysis and Cathode Shape and Preparation Here are some of key points regarding the Frascati-INFN electrolysis procedure. The aims of experiments were essentially: (a) To develop innovative and reproducible electrolytic techniques capable to maximise the values of hydrogen (H) and deuterium (D) concentrations in palladium (Pd) (i.e. the so-called "overloading": H(D)/Pd 3> 0.90 as mean value). (b) To shorten the time from beginning of experiment to reach overloading (<50h). (c) To maintain the stability of the overloading for a long time (>4h).
110
Table 1. Summary of the composition of the nine experiments performed, date and some comments about results Comments on results OVL = overloading (D/Pd > 0.9) S/N — signal/noise Pr = 1 count = 6E10 atoms
Experiments
Date: begin —> end (dd/mm/yy; 1
Electrolyte composition (mol)
1
20/12/02 -> 16/01/03
CsNOa (5E-5) SrCl2 (1E-5) LiOD (1.5E-5) H 2 S 0 4 (5E-6) NH3OH (1E-4)
Almost no OVL Anode = Pd wire 250 fim Pr = 80 =* S/N = 2
2
17/01/03 -> 14/02/03
CaCl 2 (21E-5) SrCl 2 (1E-4) HgCl2 (2E-4) H2SO4 (1E-5)
Two times OVL Residual Cs? Pr = 170 =>• S/N = 4
3
18/02/03 - • 05/03/03
CaCl 2 (1E-5) SrCl2 (1E-4) HgCl2 (2E-4) H2SO4 (1E-5) Th(N0 3 )4 (8E-6)
Three times OVL R/Ro = 1-706 Pr = 370 =s- S/N = 9
4
04/04/03 -» 14/04/03
HgCl2 (1E-5) Hg 2 S0 4 (E-4) Th(N0 3 )4 (21E-6)
No OVL
5
15/04/03 - • 19/05/03
T h ( N 0 3 ) 4 (34E-6)
Several times OVL; excess heat Pr = 300 =>• S/N = 6
Hg 2 S0 4 (2E-6) 6
29/05/03 - • 31/07/03
T h ( N 0 3 ) 4 (65E-6) Hg 2 S0 4 (5E-6)
7
31/10/03 -> 08/12/03
T h ( N 0 3 ) 4 (21E-6) Hg 2 S0 4 (3E-6)
8
29/01/04 - • 15/03/04
C 2 H 5 Od = 740 cm 3 3
D 2 0 = 61cm Th(N0 3 ) 4 (30E-6) Hg 2 S0 4 (8E-6) 9
15/03/04 -» 21/05/04
C 2 H 5 OH = 710 cm 3 H2O = 37cm
3
D2O = 12cm 3 T h ( N 0 3 ) 4 (21E-6) Hg 2 S0 4 (7E-6)
Several times OVL; excess heat Pr = 1.4E3 => S/N = 21 208 Pb anomaly; ™3^Tl = 4.6E3 and 209 Bi = 9E3 Few times OVL: Na contamination Pt deposit on Pd Q = 40E+3C Few times D overloading (R/Ro < 1.8) Na contamination Pt deposit on Pd Almost "light" experiment - • BLANK Large current adopted for long time (Q = 125E+3C) Few times H overloading (R/Ro < 1.45) Pt deposit on Pd
Ill
2.1. Electrolytes
and Electrolysis
Procedures
We decided first to employ hydro-alcoholic electrolytic solutions. The reasons for this unconventional choice were described in detail in our previous papers of ICCF series (Refs. 7 and 8). In short, we used, and are still now using, a solution of 90-95% heavy ethyl alcohol (C2H5OD) and 10-5% heavy water (D2O). The main dissolved cations were strontium (as SrCLj) and mercury (as H g C y ions, at some micromolar concentrations (10-100/xM and 1-10 fjM, respectively). The pH was kept at about 4 (acidic) by addition (if needed) of few drops of concentrated HNO3. For the sake of comparison, most of the electrolytic "cold fusion" experiments carried out in other laboratories use 0.1-1 M LiOD/D20 solutions, i.e. strong basic solutions (pH around 13/14), and a cathode current density between 60 and 600mA/cm 2 . Such procedure follows the pioneer teachings and long experimental work of Fleischmann and Pons 9 (Univ. Utah, USA), since 1989. We emphasise that in our experiments, because of the mildly acidic electrolyte (pH ~4) and the very low current density (only 5-20mA/cm 2 at the cathode surface and five times less at the anode) it is possible to reduce, to a large extent, the corrosion of components inside the electrolytic cell, borosilicate glass beaker included. Corrosion effects are typical of "conventional" electrolytic experiments: they are usually operated at high current for long time at strong basic pH. We anticipate that despite our efforts, problems coming from Pt dissolution on the anode are still not solved in a reliable way. 2.2. Elemental
Analysis
As a consequence of our procedure, at the end of the experiment it is possible to make accurate elemental analysis by inductively coupled plasma-mass spectroscopy (ICP-MS); inductively coupled plasma-optical emission spectroscopy (ICP-OES); scanning electron microscopy (SEM) with micro-analysis. The following were analysed: the residual powder filtered off from the electrolyte (by vacuum distillation), and the components of the Pd wire itself. The deleterious "matrix effect" in ICP-MS analysis is strongly reduced. After proper (long) background subtractions and inter-calibrations just after each ICPMS measurements, the results were quite accurate and reliable. The results were "safe" because they did not call for special, sophisticated (and always dangerous) mathematical elaboration. Refs. 5-7 give a detailed overview and a general discussion on the interpretation of ICP-MS results. As a historical note, because of obvious economic considerations, we developed our experimental procedure with hydrogen overloading using low cost light hydroalcoholic electrolytes at different concentrations. In the next step, we tried to adapt, and transfer, the most successful methods to the heavy water and heavy alcoholic solutions, which are about 400 times more expensive. In our deuterium-based experiments, we were looking for anomalous production of excess heat, tritium and particularly "transmutations". Very recently in fact,
112
"transmutation" phenomena received a significant acceptance in the scientific community mainly because of the reproducible experiments carried out at Mitsubishi Heavy Industries Laboratories (Yokohama, Japan). 1 - 4 We would like to remark that some of the Mitsubishi Group results (headed by Yasuhiro Iwamura) were independently confirmed also by our experimental group at INFN Frascati National Laboratories, by using with respect to that of Iwamura a complementary methodology: wet electrolytic environment instead of dry gaseous one. A detailed description and comments on the results can be found in Refs. 5-7. 2.3. Cathode Shape and
Preparation
Based on suggestions made by Giuliano Preparata and Emilio Del Giudice (University and INFN Milan, 1994), in our loading tests we use Pd cathodes consisting of wires 50-100 cm long with diameter as thin as 0.05 mm. Generally, researchers use rods (following the example of Fleischmann and Pons) or plates (25 x 25 x 1 mm, following Akito Takahashi, Osaka University, Japan, 1992). Before use, the Pd wires were carefully cleaned by dipping them in sequence in organic solvent, water, nitric acid, and water. Afterwards, by means of a specific protocol of joule heating and subsequent slow cooling down to room temperature, the wires are stress relieve annealed and, at the same time, properly oxidised as to form a thin film of Palladium oxide on the wire surface. Such a complex protocol for treating wires was developed and continuously improved by our group since 1996. By the way, we note that since 1993, we have exploited the peculiar characteristic of PdO at surface of palladium plates. The plates (Takahashi type geometry) were air oxidized at about 700° C, with a butane gas flame in a proper alumina crucible. Results from fast deuterium loading were presented at the ICCF4 and ICCF5 conferences. At that time the understanding of phenomena, although quite intriguing and reproducible, was not deep enough to justify further research. 2.4. Effects of Electrolysis
Procedure
on
Results
As reported in our papers presented at previous ICCF conference, JCF Meetings and Asti Workshops, we performed a series of experiments with hydro-alcoholic solutions containing small amounts of Sr and Hg salts. We found excess heat (see Ref. 8) and tritium (see Ref. 10) well above background. We also found that in the hydro-alcoholic ambient, during the anodic phases (that is for some hours every 13 days) of our loading cycles, the Pd electrode was partially eroded, producing small solid debris. Significant amounts of very small Pd particles are found at the bottom of the cell at the end of the experiments. In such black coloured powder ICP-MS analysis showed the presence of Pd together with some unexpected elements (see Ref. 5). Moreover, after several electrolytic loading-unloading cycles, we could observe a very unusual phenomenon: the eroded (and therefore very active?) surface of the
113
Pd wire was able to rapidly absorb the small amount of the deuterium gas dissolved into the solution without applying any electrolytic current. In our cell the maximum overpressure is only 50 mbar. Such spontaneous absorption was remarkable: a D/Pd ratio up to 0.75 was often reached. The observed D self-loading of the Pd wire up to a value equivalent to a gas pressure of over 10 bar, is obviously connected to our new and specific electrolysis procedure. Because the observation of such experimental effect, we designed a new electronic circuit able to manage, at will, the cathodic —> anodic —> cathodic cycles, in a continuous way. Such circuitry worked well and is under consideration for a patent application. Coming back to the Pd cathode, we observed by SEM analysis that the surface after electrolysis, was deeply modified; many small bubbles and holes were sprayed over the surface, suggesting the formation of a nanostructural and/or fractal geometry. See Ref. 11 for further comments about the importance of nano-structure in cold fusion experiments as pointed out by Yoshiaki Arata (Osaka University, Japan). Based on Arata's views, we are also convinced that the formation of nanostructural and/or fractal geometry at Pd surface plays a key role in the production of all the anomalous effects detected in cold fusion experiments. 3. Analysis of N e w E l e m e n t s Another important result in cold fusion studies is the experimental evidence of "transmutations" of some elements present on the cathode surface (Th and/or Hg in the present work), along with the Pd itself. In our experiments, we used both light and heavy water electrolytic solutions. In some experiments, characterised by high deuterium loading over long periods (days) and repeated loading-unloading cycles, unexpected elements (sometimes in quite large amounts) have been detected by high resolution ICP-MS analysis. Some of these elements have also an isotopic composition different from natural one. We would like to recall that in 2001, Iwamura et al. 1 was the first to show, in a very elegant experiment, that strontium (Sr) is apparently transmuted into molybdenum (Mo), or cesium (Cs) into the rare earth praseodymium (Pr) when: (a) D2 gas is forced to flow for enough long time (several hundreds of hours), (b) the D 2 gas flow is at a high enough rate (>2sccm), (c) the D 2 gas flow through a proper multilayer of Pd/Pd-CaO/Sr or Cs. We recall that proper multilayer was fully developed by Iwamura's team at Mitsubishi Heavy Industries (Yokohama Laboratories, Japan), starting in 2000, and later patented at International level. We tried to check whether such a "transmutation" can also occur after repeated D-Pd loading/unloading/loading cycles in our experimental set-up. In July 2002, we were ready to perform an independent variant of the Iwamura experiment.
114
Before starting we performed ICP-MS analysis of all the components present in the cell (C 2 H 5 OD, D z O, SrCl 2 , DC1, HgCl 2 , and Pd), and pieces of the two Pt wires (anode and reference electrodes, taken from the same batch). At the end of the D-Pd loading/unloading experiment, the electrolytic solution was vacuum dried, the residue was collected and again analysed by ICP-MS together with the Pd cathode, all dissolved in hot-concentrated aqua regia. Excess Mo was found in amounts far above any conceivable contamination. The isotopic composition of the Mo was different from the natural one (see Ref. 5). It appears that the phenomena previously discovered by Iwamura in a flowing deuterium gas system also occur in our electrolytic cell, operating for a time length of 500-1000 h, according to our loading-unloading-loading procedure.
3.1. Thorium
Salts as
Electrolyte
In January 2003, we decided to substitute the strontium salts, previously used as electrolytes, with thorium salts. The two main reasons for such the change were as follows: (a) Some results published also by our group in 1997-1998, seemed to show Th "transmutations" during high-electric power, at high temperatures and pressure, with AC (50 Hz) electrolysis with massive zirconium electrodes (both anode and cathode, see Ref. 12). Accordingly, we decided to test whether something similar could happen in our new experimental apparatus based on thin Pd wires and a very strict control of impurities. (b) Th ions (like Sr 2 + ), because of the local alkalization produced by the passage of the electrolytic current, can precipitate on the cathode surface as Th(OH) 4 (solubility product Ks = lO" 5 0 ). Th ions (like Sr 2 + ) should not be galvanically deposited on the cathode because of the high negative value of their standard potential (EQ = —1.899 V). In any case, as we want Th to be present on the Pd surface, even though this element could be co-deposited as Th deuteride (instead of as Th hydroxide) through some unknown process, no incompatibility with the aim of our specific experiment should occur. Taking into account that very low values of current density are required to deposit the proper Th(OD)4 and/or ThD s layer(s) on the cathode surface, the occurrence of some anomalous excess heat, should be easily detected. Operating with Th containing electrolytes, we intended to assay the following: (a) the occurrence of anomalous excess heat; (b) the presence of foreign elements: at the Pd cathode surface and/or into the bulk, into the liquid solutions, in the insoluble agglomerates generally present at the end of the experiment in the electrolytic cell.
115
4. Short Description of Experimental Set-up: Electrolytic Cell and Flow Calorimeter In order to understand the resistive thermal coefficient (RTC) measurement procedure (see Chapter 5) and experimental results obtained, we report some of key points of our electrolytic cell. The configuration of the cell was shown in Fig. 1 of Ref. 6. The sample holder, a PTFE tube, is placed in a 1000 ml borosilicate glass (type 3.3, brand FORTUNA) cylinder (diameter 67 mm and height 460 mm). The cathode and anode are both "U"-shaped and are located on the opposite walls of the holder, facing each other. The cathode is a thin (diameter 0.050 mm) long (60 cm) Pd wire (total surface about 1 cm 2 ). In the lower part of the Pd "U"-shaped cathode, at its centre, a small weight (6g PTFE cylinder) keeps the wire tense during the loading so as to compensate its 4-6% elongation. The anode is a Pt wire: diameter 0.250 mm, length 60 cm, purity >99.99% (Aldrich Chemicals, Germany; provided with an analysis certificate made with the ICP-MS method). A second Pt wire (length 30cm, same type of previous one) is put exactly in the middle of the "U" -shaped cathode for purposes of electrolytic tests. To measure cathode resistance, an AC current (16 mA, 10 kHz, square wave, equivalent to a current density along the wire as high as 800 A/cm 2 ) is superimposed by an array of metallic polyester capacitors to the low intensity electrolysis DC current (2-20 mA). The AC resistance value, resulting from AC voltage drop measurements (about every 10 s), is computed and acquired by a computer. The square-wave AC current, with a low current of about 15 mA, is kept constant by a proper array of fast (ns response) constant current diodes, kept at constant temperature to minimise their strong thermal dependence. A high quality LM135H thermometer (sensitivity 0.05°C), inserted in a PTFE tube, is placed in the middle of the cell, perpendicular to the cathode and anode. A Joule heater (maximum 20 W), used to calibrate the calorimeter, is located between the electrodes in a peripheral position. It is inserted in a PTFE tube (diameter 8 mm and length 30 cm). The cell is slightly pressurised (50mbar at maximum) and thermally insulated. The electrolysis gases and vapours are allowed to flow through both twin cold-traps and silicon oil bubblier before reaching the atmosphere. Corrections for these losses of energy are not yet applied, consequently all the data for excess heat are slightly under-estimated. The heat exchanger within the cell consists in a 500 cm long PTFE pipe, outer/inner diameter 4/2 mm, wound around the PTFE holder through which the cooling water flows. The temperature of the distilled water flowing in the pipe is continuously measured at the inlet and outlet of the heat exchanger with two LM135H thermometers. A computerised peristaltic pump (Masterflex 7550-62) provides a constant flow of distilled water (0.200 ml/s, with day-to-day stability of ± 1 % , routinely measured every 12 h). Since November 2003, the water is pumped from a 4-1 temperature-stabilised bath (brand Thermo NELSAB, model RTE 201), through thermally isolated tubes, kept usually at 24±0.1°C, to which it returns from the cell.
116 18 February 2004.row
0.0045
0.001 1.4x105 1.6x105 1.8x105 2x105 2.2x105 2.4x105 2.6x105 2.8x105 3x105 Time (s)
Figure 1.
Row data. R/Ro and Resistive Temperature Coefficient, versus time (s).
Cell and pump are placed in a small volume temperature stabilised chamber (kept at 24±0.15°C) to further improve the accuracy and reliability of the calorimetric measurements.
4.1. Composition
of the Electrolyte
and Cleaning
Procedure
A mixture, typical 93% volume of heavy ethyl alcohol (C2H5OD) and 7% water (D 2 0), with a total volume of 750ml, was used as electrolyte. The ethyl alcohol (Aldrich) was previously vacuum distilled at 30-35° C with a vacuum distillation system (Buchi, Model 134, Switzerland) to eliminate mainly sodium and iron. It was also ultrafiltered on line using a 100 nm, Millipore PTFE filter. The distillation system was significantly modified in our Frascati Laboratory in order to keep vacuum conditions in a static state. The density was routinely measured by densimeter (Mettler Toledo, Model DA-110M, Japan) before and after distillation, to confirm that no significant H 2 0 contamination occurred during the distillation operations. Heavy water (99.97%) isotopic purity, reactor grade (Ontario-Hydro, Canada)
117
was distilled at 40-45° C in vacuum and ultrafiltered before use, in a procedure similar to t h a t used with the alcohol. Density was measured before and after distillation. T h ( N 0 3 ) 4 (5/15 mg) was added to the electrolyte and the pH of the resulting hydro-alcoholic solution was adjusted to a value of about 3 by adding few drops of (highly concentrated, 14.5 M) HNO3 (diluted in pure D 2 0 ) , in order to avoid uncontrolled precipitation of Th(OD)4. T h e cell was cleaned after each experiment using repeated cycles of water/organic solvents/water/nitric acid/water in an ultrasonic b a t h . After experiment # 2 (February 14, 2003; see Table 1 in Ref. 6), we increased the duration of the immersion of the cell in concentrated (65%) warm (60°C) HNO3 from 2 m i n to 14 h (all night) because we suspected t h a t residual traces of Cs might remain t r a p p e d around the strictly connected spires of the cooling serpentine. 5. R T C M e a s u r e m e n t : P r i n c i p l e s of O p e r a t i o n T h e innovative procedure developed for the, in situ, measurement of the R T C , is based on a regular (every 60-200 s) changing of the intensity of AC current (at 10 kHz) along the wire, from the "low intensity" (15 mA) normally used to measure the R/RQ values, to the "high intensity" (about 120 m A ) . T h e change of current intensity affects the power dissipated in the wire (i.e. from about 7-15 m W at low intensity regime, to about 800 m W at high-intensity regime). Obviously, the dissipated power depends on the wire resistance variation, due to H / D absorption. W h e n the "high intensity" is on, the wire increases its t e m p e r a t u r e . T h e variation is large enough (although the wire is immersed in a good thermally conductive solution, like alcohol-water) to be detected, with accuracy of the order of some percent by our R/RQ measuring system. It is reasonable to assume t h a t during the "high intensity" cycle the actual loading ratio D / P d remains substantially unaffected. It is also reasonable to assume t h a t the relationship: W = hS(Tw-Ta),
(1)
where W is the dissipated power, h the thermal exchange coefficient, S the wire surface, and Tw — Ts is the t e m p e r a t u r e difference between wire and solution, remains substantially unaffected when the wire resistance changes because of the H / D loading. T h e value of the R T C is known for pure P d ( a = 3.8 x 10~ 3 ). It is, therefore, possible to calculate the (1) values at H ( D ) / P d = 0 by applying t h e low-high current intensity: Riow
= Ro(l + aTs),
(2)
^high = .Ro(l + &TW), Rio^/Rhigh
= (1 + aTs)/(l
+
(3) aTw).
(4)
118
In (4) the only unknown is Tw: such a quantity can be calculated as a function of W (Tw = f(W)) and can be determined at any moment of the experiment (in fact, the actual dissipated power at high level of current intensity is always known; consequently, Tw is always known; the only unknown is therefore the value, function of the loading ratio, of the resistive coefficient a). Taking into account that the change of a as a function of loading ratio is very large (>200%, i.e. from 0.38%/°C at D/Pd = 0 to 0.18%/°C at D/Pd = 0.75) the assumed approximations can be largely accepted. 6. Experimental Results on RTC Measurements from experiments # 8 (deuterium experiment) and # 9 (hydrogen experiment) are compared here because the experimental set-up was exactly the same, making cross-comparisons easy. 6.1. Exp. 8 (File 18 February
2004)
Deuterium
In Fig. 1, the R/RQ ratio (vertical left axis, from 0.95 to 2.05), shows over time (from 140,000 to 310,000s), and the Resistive Temperature Coefficient (vertical right axis, from 0.001 to 0.004). The data clearly show the twin values of R/RQ due to the cycles of low power (about 7-15 mW) and high power (700-800 mW) because AC (electromigration) currents injected along the Pd wire. In Fig. 2, the same data of Fig. 1 are shown after off line filtering. This procedure, up to now, has been made selecting the data one-to-one, and is very long time consuming and tedious. Figure 3 is just a magnification of Fig. 2 around the unloading-loading area. In short, the cell was kept in cathodic condition up to time 196,000 {R/RQ = 1.82). At that time the electrolytic current was disconnected and the R/RQ value, after a small decrease, started to increase again because unloading. About RTC, it was at 0.0020-0.0021 during loading condition and decreased to 0.0015 at the point where it reached the maximum of R/RQ. At time 194,000 unloading was forced by anodic current (2 mA). The maximum of R/RQ was 1.94 and not 2.0 as expected because the anodic stripping was quite strong and the unloading was not homogeneous along the wire. At time 204,000 the anodic current was ended and the R/RQ reached the minimum value of about 1.015. This value is little bit larger then 1.00 because some stress, due to previous loading, was induced into the wire. The RTC reached a value of about 0.0037, close to the value reported in the literature (0.0038 at 293 K). From about time 204,000 to time 206,000 the wire was in floating condition and absorbed some deuterium dissolved in the alcohol-water solution. At time 206,000 was given again cathodic current, and it started usual loading. At time 213,500 the R/RQ reached the maximum value, about 2.015, larger than 2.00 because previous residual stress. The RTC reached it minimum value,
119 18 February 2004_corr 0.004
—,—
ll1
V V — —
0.0035
-L
»Ro_d |
5
'
—
7 * ytf
mi
»
™
-TcN_L->H
|
0.002
'xypv" 1
]
-
[JJPPH
0.001
1.4x105 1.6x105 1.8x105 2x105 2.2x105 2.4x105 2.6x105 2.8x105 3x105 Time (s) Figure 2.
Same as Fig. 1, except the data are filtered for clarity.
about 0.0014. The value of 0.0014 is clearly different from previous 0.0015 (at time 198,000) found in our experiment because of forced, rapid inhomogeneous unloading. Such values are lower then that reported in the literature (0.0018). We think that our measurement conditions (electrolysis) are quite different from that reported in the literature (clean gas environment) and can explain the differences. Moreover, we think that the value of heat exchange constant, measured at the beginning of the experiment, increased because of better thermal conductivity. This effect reduced the amount of signal detected. Obviously, more sophisticated analysis and experimental procedures will be needed in the future. At time 290,000 the R/RQ value reached the same value of time 145,000, i.e. 1.90. We can observe that the value of RTC was lower at time 290,000 compared to time 145,000. A possible explanation is that at time 145,000 some excess heat occurred that increased the value of R/RQ of the wire. The effect of excess heat can be seen in Fig. 4. The value was over 200 mW.
120 18 February 2004.cor 0045
0.001 1.9x105
1.95x105
2x10 5
2.05x105
2.1x105
2.15x105
2.2x105
Time (s) Figure 3.
Magnification around maximum-minimum of
R/RQ.
In conclusion, the combined observation of R/RQ and RTC can help strongly to judge if there is some excess heat, especially at low level of power.
6.2. Exp. 9 (File 25 March 2004)-
Hydrogen
Experiment
In Figs. 5 and 6, similar to Figs. 2 and 3, are shown the behaviour over time (in s) of R/RQ (vertical left axis, from 0.95 to 1.85) and RTC (vertical right axis, from 0.001 to 0.0045). The electrolytic current was as low as 5 mA. The wire was previously almost overloaded because of the combined effects of Th and Hg, apart from cathodic current. At time 930,000 it was almost steady at R/R0 = 1.43 from several hours and RTC had a value of about 0.0024. At time 933,000 electrolysis was discontinued, and the wire immediately started to deload. At time 93,340, because the loading was not very fast, we applied anodic current (2 mA).
121 18 February 2004_row 0035
0.004
0.0035
0.003
H
v
0.0025
X
0.002
0.0015
0.001
1.4x105 1.6x105 1.8x105 2x105 2.2x105 2.4x105 2.6x105 2.8x105 3x105 Time (s) Figure 4. Row data. Evidence of excess heat, at time 150,000, in respect to time 290,000. In fact, the R/Ro values were the same but RTC were different.
At time 934,000 the R/RQ value reached it maximum (1.80) and RTC its minimum value (0.0013). The value of RTC was 0.0013 lower than the expected value, 0.0018. As discussed in the previous deuterium experiment 6.1, the differences of values about RTC can be understood if we accept that the heat exchange coefficient of wire with the solution increased a large amount in respect to "time zero" of the experiment, when we calibrate (keeping the value for data elaboration). At time 940,500 the R/RQ reached its minimum value (1.05) and RTC its maximum (about 0.0033): we disconnected the anodic current. We did not wait long in anodic conditions because we were afraid the wire might break from the anodic corrosion effect. The minimum of R/RQ was larger than 1.00. At time 941,500, after observing weak self-loading, we restarted the cathodic current at 5 mA. At time 951,000 the R/RQ reached it maximum value of 1.62 and RTC its minimum of about 0.0017. Both values are different from expected. We think that large differences are due to inhomogeneous loading of the wire.
122 25MAR04 corr 0.0045 1.8 0.004 -
RIR0_d 1.6
if 5
0.0035
1I
1.4
0.003
£& Ifali r
0 0025
f ffl
0.002
1.2 I
I
jpPfrpi w™# IF*"* "H" 0 0015 J„L->H |
1
1 9.3x105
9.4x106
9.5x105
9.6x105
9.7x105
0.001
9.8x105
Time (s) Figure 5.
Filtered data. Hydrogen loading. Overview of 1 day of experiment.
At time 985,000 the loading was still improving (R/Ro about 1.53) and after about other 30,000s reached the value of 1.42, similar to the value that we observed at time 935,000 (the beginning of unloading —> loading cycle). In other words, the mild unloading —> loading cycle did not damage the surface of Palladium wire. 7. Experimental Results with ICP-MS Experimental conditions and ICP-MS analysis results about the nine experiments, up to now performed that included ICP-MS analysis, are reported in Tables 1 and 2. 7.1. Summary of Experiment about 5 X 1 0 1 0 atoms)
#7 (Analysis
by ICP-MS,
1 count
Date: Oct 31, 2003-Dec. 08, 2003. Current: Usually 10mA, up to 50mA along 5 days (Q = 40 x 10 3 C). Overall results: Only few times overloading.
123 25MAR04_corr
0.001 9.3x105
9.35x105
9.4x105
9.45x105
9.5x105 9.55x105
9.6x105
Time (s) Figure 6. Filtered data. Hydrogen loading. Magnification around: minimum (relative) —» maximum (absolute) —> minimum (absolute) —> maximum (relative) of R/RQ.
Reasons: Large 23 Na in C2H5OD (poor vacuum distillation); excessive Pt deposition from anode. Electrolytes (750cm 3 solution: C 2 H 5 OD 93%, D 2 0 7%): • Th(N0 3 ) 4 = 21.5 x 10~ 6 mol (-> 2.6 x 108 counts) recovered 70%. • Hg 2 S0 4 = 3 x 10" 6 mol (-• 3.6 x 107 counts) recovered 3%. Main elements detected by ICP-MS: • • • • • •
Cu = 3.9 xlO 6 ; 6 3 Cu/ 6 5 Cu = 2.0; Cu from Hg? Zn = 3.6 xlO 6 ; Cu/Zn = 1.08. Rb = 2 xlO 4 . Cs = 2 xlO 4 . Pb = 1.25 xlO 6 ; Pb from Hg and/or Th? Bi = 8 xlO 3 .
124 Table 2.
Summary of some of most frequent elements found by IGP-MS in the nine experiments 64
K (93.3)
C u (69.2) 65 C u (30.8) 63/65 = 2.25
Zn Zn 67 Zn 68 Zn
63
39
66
(48.6) (27.9) (4.1) (18.8)
206
P b (24.1) P b (22.1) 208 P b (52.4) 206/208 = 0.46 207
133
Cs (100)
Experiments
31
1
7E3
2.2E6
2.4E6
2.7E6
>3E8
1E4
2
0
0
2.1E6 63/65 = 1.94
1.8E6
6E5
4E5
3
4E5
2.7E6
6.1E6 63/65 = 1.93
1.7E6
1E6
9.5E5
4
2.5E4
1.4E6
2.9E6 63/65 =: 2.05
7.5E3
1.94E5 6.9E5
5
1.8E6
2.3E6
2.4E7 63/65 = 2.07
1.2E7
9E4
1.5E6
6
2.72E7
6.4E6
9.3E8 63/65 = 2.08
5.1E8
2.2E5
2E8 206/208 == 0.39
7
0
0
3.9E6 63/65 =: 2.0
3.6E6
2E4
1.25E6
8
2.5E5
1.6E8
2.7E6 63/65 =: 2.14
1.77E7
3E5
7.1E5 206/208 == 0.49
9
0
0 (found 6.6E6 from C2HsOH)
2.3E6
6.2E6
0
4.5E5
P (100)
63/65 =: 2.12 Background subtracted.
7.2. Summary
of Experiment
#9
Date: March 15, 2004-May 21, 2004. Current: Usually 20mA, up to 50 mA along 15 days (Q = 125 x 103 C). Overall results: Only few times H overloading (R/RQ < 1.45). Reason: Excessive Pt deposition from anode. Electrolytes: (1) 760 cm 3 solution: C 2 H 5 OH = 712 cm 3 , H 2 0 = 36 cm 3 i.e. commercial 95% concentration, ethyl alcohol; D2O = 12cm 3 ; (2) Th(N0 3 ) 4 = 21.5 x 10- 6 mol (-> 2.6 x 108 counts) recovered 60%; (3) Hg 2 S0 4 = 7 x 10- 6 mol (-> 8.4 x 107 counts) recovered 58%. Main elements detected by ICP-MS: • Cu = 2.3 xlO 6 ; 6 3 Cu/ 6 5 Cu = 2.12; Cu from Hg? • Zn = 6.2 XlO6; Cu/Zn = 0.37; Zn from Pd? • Rb = 0.
125
• Cs = 0. • Pb = 44.5 xlO 5 ; Pb from Th and/or Hg? • Bi = 0. 8. Key Parameters and Comments After a lot of tests in different experimental conditions we have identified the following key parameters and experimental conditions to be fulfilled: (a) Deuterium, must be carefully purified, especially if it comes from a liquid compound. (b) Large overloading, for long time (days) and flux of deuterium through the Pd surface. At present the stability of the D overloading in our experiment is not yet completely satisfactory. (c) Presence of "nanostructures" on the Pd surface (Pd + Th + Hg + "impurities" ). (d) Pt dissolution should be avoided. Pt ions are galvanically collected on the Pd surface and inhibit the loading process (a drop in the cathodic overvoltage): at present this important item is not fully controlled in our experiments. (e) Cleaning the Pd surface during the loading process by means of short periods of anodic stripping. 9. Comments on Transmutations • Pb seems to be related to Th: enhanced decay of Th by deuterium? (also according to Cincinnati Group preliminary experiments, by Zr-H, in 1997); • Cu seems to be related to Th, Hg and Pd: fission, according to Takahashi model and, very recent, specific results using Y. Iwamura multilayer device (test on D-Hg-Pd, Japan-Italy joint Collaboration, this Conference); • Zn seems to be related to Pd: fission, according to Takahashi model; • It is necessary to increase, in a large amount, the equivalent cross section. At present, it is about 1 barn on Iwamura Cs to Pr (ion beam deposition) gas experiments, reproducible; up to 600 barn in our electrolytic (Th-Pb, experiments # 6 reported in Tables 1 and 2) but not fully reproducible. 9.1. Comments
about Th-Hg
Addition
• The Th-Hg solutions, at micromolar concentration, give transmutations results "better" than Sr-Hg solutions. • The main drawback is the criticality of Th addition because, quite frequently, it form a thick layer at Pd surface that decrease largely the H (or D) absorption into Pd, at least at room temperature. • The main advantage is the increased mechanical properties of Pd wire: our historic problems of thin wire ruptures disappeared.
126
• T h e combined effect t h e previous two points can be very useful in t h e case of technological application of cold fusion effect: high t e m p e r a t u r e and over-all reliability are needed.
10.
Conclusions
By comparing the results of nine experiments, it can be argued t h a t are real and not an instrumental artefact. In fact, t h e appearance of new elements depend on:
transmutations
(a) deuterium presence (not hydrogen) in t h e P d lattice; (b) deuterium overloading for a long time together with inward-outward deuterium flux trough t h e P d surface; (c) elements added to the electrolyte t h a t are capable of being fixed a n d / o r absorbed at the Pd-electrolyte interface. Work is in progress at I N F N - L N F to build a special calorimeter and electrolytic cell transparent to I R radiation. Such radiation will be detected from a I R thermocamera, model TH7102MX (from N E C , J a p a n ) , provided also with a special optical instrument (Nikon) able t o detect our thin wire (50 /xm) u p to 2 cm of distance. Our goal is to get a "full movie" of t h e "excess heat" coming out from the P d surface, along the experiment, starting from t h e beginning when no excess heat exists, u p to its eventual occurrence. Further work is necessary in order t o reduce t h e dissolution of P t at t h e anode in our cell.
Acknowledgments We are deeply indebted with Prof. Akito Takahashi (Osaka University, J a p a n ) and Dr. Yasuhiro Iwamura (Mitsubishi Heavy Industries, Yokohama, J a p a n ) , for very useful suggestions a n d critical comments about b o t h ICP-MS measurements and discussion about models t h a t can help to explain t h e experimental results. We cannot forget t h e patience, a n d encouragements given t o us from Prof. Jean Paul Biberian, chairman of ICCF11 at Marseille. He waited our paper for really long time, without complaining us too much. At I N F N Frascati National Laboratory we cannot forget the enthusiastic support given to our experimental activity, in all aspects, by Dr. Sergio Bertolucci (Main Director of the Laboratory) and Dr. Lucia Votano (Director of Research D e p a r t m e n t ) . At I N F N t h e F R E E T H A I experiment was performed with a grant from G V National Group.
References 1. 2. 3. 4.
Y. Y. Y. Y.
Iwamura, Iwamura, Iwamura, Iwamura,
et et et et
al, al, al, al,
Jpn. J. Appl. Phys. 4 1 , 4642-4648 (2002). Proceedings of the ICCF10, 24-29 August 2003. The 5th Meeting of Japan CF-Research Society (JCF5). Proceedings of the ICCF11, 2004.
127 5. F. Celani, et al, The Ith Meeting of Japan CF-Research Society (JCF4), October 17-18, 2002, Iwate University, Japan, pp. 17-21. 6. F. Celani, et al, Proceedings of the ICCF10, 24-29 August 2003. 7. F. Celani, et al, The 5th Meeting of Japan CF-Research Society (JCF5). 8. F. Celani, et al, Condensed matter nuclear science, in Proceedings of the ICCF9, 19-25 May 2002, Beijing, China, pp. 29-35; ISBN 7-302-06489-X. 9. M. Fleischmann, S. Pons, and M. Hawkins, J. Electroanal Chem. 261, 301-308 (1989). 10. F. Celani, et al, Condensed matter nuclear science, in Proceedings of the ICCF9, 19-25 May 2002, Beijing, China, pp. 36-41; ISBN 7-302-06489-X. 11. Y. Arata and Yue Chang Zhang, Proceedings of the ICCF10, 24-29 August 2003. 12. F. Celani, P.G. Sona, and A. Mancini, Proceedings of the ICCF7, April 19-24, 1998, Vancouver, Canada, pp. 56-61.
E M E R G E N C E OF A H I G H - T E M P E R A T U R E S U P E R C O N D U C T I V I T Y IN H Y D R O G E N CYCLED P d C O M P O U N D S AS A N E V I D E N C E FOR S U P E R S T O I H I O M E T R I C H / D SITES
ANDREI LIPSON, CARLOS CASTANO, AND G E O R G E MILEY University
of Illinois
at Urbana-Champaign,
IL,
USA
ANDREI LIPSON AND BORIS LYAKHOV Insititute
of Physical
Chemistry,
RAS,
Moscow,
Russia
ALEXANDER MITIN P. Kapitza
Institute
for Physical
Problems,
RAS,
Moscow,
Russia
Transport and magnetic properties of hydrogen cycled PdHz and P d / P d O H ^ (x ~ (4/6) X 10 —4 ) nano-composite consisting of a Pd matrix with hydrogen trapped inside dislocation cores have been studied. The results suggest emergence of a high-temperature superconductivity state of a condensed hydrogen phase confined inside deep dislocation cores in the Pd matrix. The possible role of hydrogen/deuterium filled dislocation nano-tubes is discussed. These dislocation cores could be considered as active centers of LENR triggering due to (i) short D-D separation distance (~Bohr radius); (ii) high-local D-loading in the Pd and the corresponding effective lattice compression; (iii) a large optic phonon energy resulting in a most effective lattice-nuclei energy transfer.
1. Introduction The study of the trapping and interaction of hydrogen atoms inside metallic nano-structures (dislocation cores or "nanotubes") is important in order to shed light on the possible origin of LENR in highly loaded palladium hydrides/deuterides. Recently, Ashcroft presented a strong argument that hydrogen dominant metallic alloys, might demonstrate high-temperature superconductivity (HTS) even in a modest external pressure range. 1 According to Ashcroft's reasoning, HTS of highly loaded metal hydrides would be due to the overlapping of metal-hydrogen bands. The high-electron concentration and optical phonon energy result in a strong electron-phonon coupling. The advantage of hydrogen dominant hydrides for achieving HTS is in a chemical sense they have already undergone a sort of "precompression," and once impelled by external pressure enter into metallic phase, the electrons from both the hydrogen and the metal may participate in common overlapping bands. There is, however, another approach for achieving a compressed metal hydride 128
129
with a high-coupling constant, that may serve as a model alloy to search for HTS in hydrogen-dominant metallic systems. The deep dislocation core filled with hydrogen atoms could be considered as a sort of "nanotube" with an effective diameter of about two Pd Burgers vectors. Moreover, it is implied that within the deep dislocation core (R^ < b) the local hydrogen concentration might be large enough to provide the ability of overloading the Pd beyond the x = l. 2 Notice that the pressure inside such deep cores of the edge dislocation would be comparable to the local palladium bulk modulus, i.e., up to 100 GPa. Therefore, both conditions for hydrogen "precompression" and external pressure impelling would be satisfied. If hydrogen is trapped inside deep dislocation core sites it is anticipated that these sites could be characterized by - superstoichiometric hydrogen loading (loading ratio x = H/Pd > 1.0 or precipitation of condensed metallic hydrogen in the form of H„, (H2) n ; - high-local pressure/compression P ~ 120 GPa; - high-optic phonon frequency (hu> ~ 120 meV); - strong electron-phonon coupling (Ae-ph ~ 1.0); - strong Pd-H(D) band overlapping. In summary, such enhanced parameters of condensed hydrogen in Pd lattice suggest an excellent conditions to achieve both HTS and triggering LENR processes (to be active sites of cold fusion in Pd lattice). The observation of a diamagnetic/superconducting behavior from a hydrogen phase precipitated inside the dislocations confined to the Pd matrix could be feasible when two referenced conditions to dislocation network are satisfied:3 (1) there is a sufficiently large number of dislocations within the Pd crystal that contain tightly bound compressed hydrogen and (2) the network of dislocations is organized in the form of closed loops, which can carry a persistent current. In this work, we studied the structural and magnetic properties of PdHa, single crystal and Pd/PdO:!!^ heterostructure samples with a very low-average loading ratio of (x) ~ (4.5 - 6.0) x 10" 4 that were produced by cycling the pristine Pd single crystal or Pd/PdO in a H2 atmosphere or during electrolysis, respectively. Thermal desorption analysis (TDA) showed that the residual hydrogen, precipitates as a condensed phase within the deep dislocation cores. Magnetic measurements recorded the appearance of a strong diamagnetic contribution of the condensed hydrogen phase [PdH^-Pd] in the Pd matrix at T < 30 K (in a weak magnetic field, H < 5.0 Oe), and an antiferromagnetic behavior in the higher magnetic field.3'4 Transport and magnetic measurements performed with Pd/PdO:H x samples provide direct evidence of superconducting transition at T < 70 K. 2. E x p e r i m e n t a l To minimize the effect of impurities on the magnetic properties of the PdH^ system, a 99.999% pure Pd-single crystal produced by Metal Crystals and Oxides of
130
Cambridge, UK was employed in this work. The cylindrical ingot was grown using the Czochralski method with a [110] axis, a length of 10 cm, and a diameter of ~ 1.0 cm. The sample with dimensions of 2.7mm 3 x 2.7 mm 3 x 0.6 mm 3 and a weight of 52 mg. was cut from the as-grown ingot by using a low-speed diamond saw and mechanically polished to remove surface irregularities. Then, this single crystal was annealed in a high vacuum (p = 10" 8 Torr) at a temperature of 800°C for 5h. The annealed pristine single Pd crystal served as a reference and is labeled the "background" sample or (bgr), and the appropriate TDA and magnetic measurements were conducted on this sample prior to the hydrogen cycling. In order to create a condensed hydrogen phase in the Pd sample, a H2 gas cycling procedure was applied. The sample was loaded and degassed twice. The pristine Pd(bgr) sample (after TDA and magnetic measurements) was loaded at a pressure of 930 Torr at a temperature of 390 K and degassed in a vacuum of 1 0 - 6 Torr at a temperature of about 400-430 K. After the cycling, the PdH^ sample was subjected to a final annealing at a temperature of 570 K and a pressure of 10~ 8 Torr for 2h. This post-cycled PdH^ crystal is labeled "foreground" sample or (fg). The cold worked 12.5//m Pd foil (99.95%) of Nilaco, Japan has served as a basis for Pd/PdO heterostructure production. In accordance with ICP analysis performed by producer, the concentration of ferromagnetic impurities (mainly Fe) was found to be <10ppm. Other main impurities in the Pd foil included Pt (20ppm), Cu (20ppm), Ag (30ppm) and Na (lppm). Prior to oxidation the Pd substrate was annealed at t = 800° C in vacuum during 5h. Then it was treated in oxygen-butane torch at t =1000°C during 10s in order to produce a stable oxide layer about 40 nm thick. Accordingly to a SIMS study, P d O / P d / P d O heterostructure samples synthesized by this technique contain the PdO y (0.1 < y < 1.0) oxide, such that y value is exponentially decreased beneath the surface in the depth ranging from 0 < h < 35 nm. The small traces of carbon vanishing below 10 nm were also detected at the surface of the oxide. In order to create dislocation structure filled with hydrogen in Pd/PdO heterostructure, the samples with area S = 2.0-2.5cm 2 (m = 22-30mg), serving as a cathode were electrochemically cycled in the cell with Pt anode at j = 5.0 mA/cm 2 in high purity 1 M Li 2 S04/H 2 0 (99.99%) electrolyte. The procedure of electrochemical cycling included consequent cathode-anodic polarizations (loading-deloading) of the sample. After achieving the cathode loading up to x = H/Pd = 0.7 the current was switched to the anodic regime to extract hydrogen from PdHa, regular lattice. The cathode loading - anodic deloading cycles were repeated during 5-10 times. In order to remove all weakly bound residual hydrogen atoms from the Pd lattice, after electrochemical cycling the samples were additionally annealed in vacuum at t = 300°C during 2h. The resulting Pd/PdOiHa, samples obtained by electrochemical cycling with final annealing are called below as foreground (fg) samples. As the reference samples, (called background (bgr)) the pristine (uncycled) Pd/PdO heterostructure and Pd/PdOiHz (fg) foils annealed at high temperature {t = 600°C) in a high vacuum were served.
131
A high-vacuum thermal desorption technique was used to estimate the residual hydrogen concentration in the PdH^ and Pd/PdO:H x samples after hydrogen cycling and annealing. The samples were heated within the 20-900° C-temperature interval in the linear regime, at the rate of 9.0K/min in a high-vacuum (10~ 8 Torr) chamber that had a quadrupole mass-spectrometer. After analyzing the desorption species (Fig. 1) and comparing the yield with the data from the Pd(bgr) or Pd/PdO(bgr) (taking into account the residual hydrogen background in the vacuum chamber) we were able to calculate the real hydrogen desorption peak area and the temperature of its maximum. It was found that the background hydrogen desorption pressure (Pd(bgr) sample, plus the residual hydrogen in the chamber) was at least 5-10 times lower than the H2 pressure caused by the P d l ^ (fg) samples (Fig. la,b). For the quantitative estimation of the final average loading ratios x = H/Pd, we conducted a special calibration measurements with a known mass (0.3 mg) of T1H2 powder that has a decomposition temperature near 400° C. Comparing the hydrogen pressure in the chamber obtained from the TiH2 powder with the PdH^ we yielded an estimation of the residual hydrogen content in the H2 cycled Pd single crystal. Magnetic measurements were carried out with a IT-SQUID "Quantum Design MPMS-3" using DC-magnetization and AC-susceptibility modes. The Pd(bgr) and (fg) samples were placed in a gelatin aligned in the direction to the pick-up coil and covered with a small piece of cotton. The initial magnetic moment of the capsule with a piece of cotton, in a low-magnetic field H < 10.0 Oe was measured to be M < 10~ 8 emu well over the studied temperature interval (2.0-350K). Measurements with a calibration magnetic fluxgate, showed that without the application of the special ultra-low field condition, the SQUID has a residual magnetic field of AH ~ —0.2G. Ultra-low field installation with degaussing of the shielding produces an almost zero field (the remnant field is less than 1 mG). In the DC-magnetization mode, the SQUID was calibrated with a Pd standard. It was found that the sensitivity of the SQUID with capsule and sample is higher than 5 x 10~ 8 emu. To measure the magnetic moment, vs. T in the zero-field cooling (ZFC) regime, the samples were cooled down from T = 298-2.0 K at H = 0 after installation of zero field at room temperature. The measurements for the M(H) function at constant temperatures was carried out in the automatic regime. After the measurements of M(H) at the given temperatures were completed, the sample was heated at H = 0 to T = 350 K. The cooling of the Pd samples to the next temperature was conducted at the nominal H = 0 (without zero-field installation) after annealing the capsule at a temperature of 350 K for lOmin inside the SQUID. The AC measurement of the real and imaginary parts of the susceptibility for the Pd samples was carried out at H = 0 with driving amplitude h = 1.0 Oe, and the magnetic field frequency / = 20 Hz. During this measurement, the samples were cooled to 2.0 K at if = 0 without a special zero-field installation. Before AC measurement the setup was calibrated in the range of 2-10 K by using pieces of
132
high-purity Pb and Nb that were similarly shaped to the Pd samples. The R(T) and R(I) measurements with Pd/PdO and Pd/PdO:H x foils in the range of 4.2-294 K were performed with a standard four probe technique using high-quality pressed indium ohmic contacts to prevent damage of PdO coating and simultaneously to minimize current inhomogeneity. The voltage data were recorded with Keithely 182 digital voltmeter using current pulses of 1-10 s duration (/ = 0.001-10 mA) provided by Keithely 220 programmable source to exclude thermopower contribution. The mean sweep rate of the temperature between voltage measurements was in the range of 0.01-0.03 K/s. The sample was cut from the same Pd/PdO sheet used in the magnetic measurement and had dimensions 32 x 3.4 mm 2 . First series of R(T) and R(I) measurements was performed with the original annealed Pd/PdO(bgr) sample (with no hydrogen). After the first series of measurement, this Pd/PdO sample was electrochemically cycled with hydrogen (three times) and annealed at T = 300° C during 2h in vacuum to obtain Pd/PdOiH^fg) sample. In the second series the same measurements of R(T) and R(I) as in the first series were carried out with the Pd/PdChH^fg) sample. To keep possibility of direct comparison between Pd/PdO and Pd/PdO:H s resistance behavior, the distance between the potential contacts was fixed at 2.0 cm in both series of measurements. 3. Experimental Results 3.1. Thermal
Desorption
Analysis
Thermal desorption analysis performed with annealed Pd(bgr) samples in the temperature range of 20-900° C showed a total absence of any hydrogen desorption peaks. Hydrogen pressure in the vacuum chamber throughout the studied temperature intervals did not exceed 2 x 10~ 8 Torr (Fig. 1, curve a). This H2 pressure value equals the residual hydrogen background in the chamber. Therefore, the TDA with the annealed Pd single crystal indicates that there was no trapped hydrogen in the sample. Similar measurements performed for the PdH^fg) sample showed a H2 pressure behavior at T < 700°C that was similar to the Pd(bgr) sample (Fig. 1, curve b). This observation proofs that there is no hydrogen (in a or f3 phase) in the regular lattice of H-cycled PdrL^fg) sample. However, at T > 700°C, the hydrogen desorption (curve b) increased and the post-cycled (fg) sample produced a pronounced peak with maximum at a temperature of 870° C. (Notice that the TDA peak in this experiment was not completed because the heater in our apparatus could not heat the sample beyond 900°C.) The analysis showed that H 2 pressure at 870° C is about six times higher than that observed at the same temperature range in the background measurements. Integration of the PdH x (fg) H2 peak (with the background subtracting), and comparison of its area with calibration data obtained for TiH 2 powder allowed the estimation of the effective loading ratio x = H/Pd, averaged over the PdHa:(fg) sample volume as x — (4.5±0.5) x 10~ 4 . The averaged value of x is smaller than expected for any known stable phase of Pd hydride. Considering that after the H 2 cycling, the sample underwent additional annealing at a
133
temperature of 570 K, which caused the decomposition of the residual a-phase in the lattice, we assume that all remaining hydrogen detected in the cycled Pd single crystal is located in the dislocations, but not in the regular lattice. Extrapolating the results of SANS measurements performed in Ref. 2, for various residual hydrogen concentrations (x > 1.7 x 10~3) in Pd polycrystal it is possible to estimate a radius Ru of residual hydrogen distribution with respect to dislocation cores. At (x) = H/Pd = 4.5 x 10~ 4 in our sample, the P H ~ 2.75 A is close to the Burgers vector or minimal radius of H capture in Pd.
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In order to estimate the binding energy of hydrogen within the Pd, the hydrogen activation energy was calculated. The formal kinetics Garlick-Gibson model may be used to estimate the kinetic parameters of second-order thermal activation processes by accounting for the rising part of the hydrogen TDA peak: 2 ' 5 £R~ = ks^Ti/(T2 —Ty)} ln(P2/P\), where fee is the Boltzmann constant; Pi, P2 and T 1; T2 are the hydrogen pressures and temperatures, respectively, corresponding to those pressures, at the rising portion of the desorption curve (so that T2 > 7\ and Pi > Pi)- In accordance with the formula, the activation energy of the desorption which reflects the effective binding energy of hydrogen atoms in the Pd lattice was found to be e H = 1.6 ± 0.2 eV. The magnitude of activation energy of the hydrogen desorption that was found for the PdH x (fg) crystal is well above the H-trapping activation energy derived for H-cycled polycrystalline cold-worked Pd that has an extremely low-bulk hydrogen concentration captured inside the deep dislocation cores (en ~ 0.7eV). 2 ' 3 This provides us with a strong argument that the hydrogen is bound solely inside the deepest core sites. Thus, the TDA results show that the atoms of hydrogen are tightly bound inside the deep dislocation cores and can be fully removed only at
134
very high temperatures (T > 1000°C), which would suggest a full recrystallization of the Pd sample. The results of TDA allow us to conclude that PdHj; samples that are produced by H 2 gas cycling of the Pd single crystals followed by annealing at T = 570 K contain no hydrogen atoms in their crystalline lattice except those that are tightly bound inside the deepest dislocation cores (or "dislocation nanotubes") with a minimal radius RH = 2.75 A. Thermal desorption analysis performed with Pd/PdO(bgr) samples in the temperature range of 20-700° C showed an absence of any hydrogen desorption above the background level. The hydrogen pressure in a vacuum chamber in the whole studied temperature interval did not exceed 2 x 10~ 8 Torr (Fig. 2, curve a). This H2 pressure value is in good agreement with a residual hydrogen background in the chamber. In similar measurements performed with Pd/PdOirL^fg) sample, a broad H 2 thermal desorption peak with T m a x = 430° C is appeared and pressure still not returns to the background level up to T = 700° C (Fig. 2, curve b). Comparative TDA of a the Pd/PdO:H x (fg) main peak with T r a a x = 430° C (with subtraction of H2 background) and calibration peak obtained for TiH2 powder allowed to estimate an effective average loading ratio x = H/Pd in Pd/PdO:H :r (fg) sample, which was found to be (x) = (5.5 ± 0.5) x 10~ 4 . This effective value of x = H/Pd is rather smaller than that which could be expected for any known stable phase of Pd hydride. 2 Taking into account that after the H2 cycling the sample was underwent to additional annealing at T = 573 K caused a decomposition of remaining PdHj; aphase, it is reasonable to assume that all residual hydrogen remaining in the cycled sample is tightly bound with dislocations, but not in the regular lattice.
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Figure 2.
Thermal activation analysis of the rising part of the TDA curve with subtracting of a hydrogen background in the chamber gives an activation energy of the Hatom desorption e H = 0.63 ± 0.10 eV. The magnitude of this activation energy is well above the H-trapping activation energy in the H2-cycled single crystal Pd,
135
with residual a-phase and is in good agreement with the activation energy of Htrapping in polycrystalline Pd after electrochemical cycling. Notice that dislocations in Pd/PdOiHz are mainly stored at the interface between Pd and PdO because the maximum temperature of the hydrogen desorption peak (T m = 430° C) is still lower than that in a bulk Pd cycled with hydrogen (T ~ 800°C). 5 The traces of a bulk hydrogen presence in the Pd/PdOiHz sample could be seen as broad noncompletely resolved maxima in TDA spectrum (Fig. lb) at T = 540 and 640°C. Thus, we can conclude that H-atoms in Pd/PdOrH^ tend to trapping mainly inside deep dislocation cores at the boundary between Pd and PdO (where dislocation concentration must reach maximum value compared to Pd bulk). A large hydrogen binding energy £H = 0.63eV/atH is well above the H-binding energy or enthalpy of stoichiometric Pd hydride formation (| AH\ ~ 0.18 eV/at H), suggesting a significant Pd-H common band overlapping at the Pd-PdO boundary inside deep dislocation cores. TDA data allow to propose a simple model for the deep edge dislocation core filled with trapped hydrogen (Fig. 3). In accordance with Figs. 1 and 2 after the H-cycling, data the regular lattice of Pd contains no hydride and thus, all residual hydrogen is localized inside the deep core of the edge dislocation (in the direction of Pd [121]) determined by Burgers vector b[l 0 1 ] = 2.75 A. Depending on average residual concentration (x) and dislocation density Nd, the effective loading ratio inside the deep core in Pd f.c.c. lattice is determined by simple formula: xeS = \/2(x} /Ndxb2. Accordingly, to this formula at Nd ~ (1.0 2.0) x 10 11 cm~ 2 4 eS and (x) ~ (4 —6) x 10~ the x would be in the range of 1.0 < a;eff < 3.0, suggesting superstoichiometric hydride formation in the deep dislocation cores. 3.2. Magnetic
Measurement
Results for
PdHx
The ZFC experiment in the DC-mode showed that in a weak magnetic field (H = 0.5Oe), the magnetic moment of H2-cycled PdH^(fg) samples in the temperature range of 2 < T < 50 K is significantly lower than M(T) for the original Pd(bgr) single crystals (Fig. 4). The difference between the moments of the cycled sample and the original single crystal [PdH^-Pd] reflects the contribution of the condensed hydrogen phase inside the deep dislocation cores. This difference tends to increase at T < 30 K. There was no temperature dependence observed for the [PdH^-Pd] difference of moments in FC measurements at high-magnetic field (H = 1000 Oe) measurements. The moment of the PdH x is about 4-5% lower than that of the Pd(bgr). Thus, a nearly constant negative AM difference is detected within all temperature ranges 2-298 K. In order to ascertain the origins of the dramatic decrease in the paramagnetic properties of PdH^ compared to the Pd single crystal at T < 30 K, we studied the magnetization of the PdHa:(fg) and Pd(bg) samples as a function of the applied magnetic field. These measurements were performed at constant temperatures T = 2.0, 10.0, 50.0, 100.0 and 298K in magnetic fields ranging from 0 to ±200 Oe. The M(H) dependences at T = 2.0 K for the Pd(bgr) and PdH^fg) samples that
136
Pd (121) 1D(T01) = 2 . 7 5 A Figure 3.
are presented in (Fig. 6) have an essentially different character, especially below H ~ 10.0 Oe: (1) The total width of the hysteresis loop at M = 0 for the PdHE(fg) sample (AH = 7.45 Oe) is much higher than that of the Pd(bgr) single crystal {AH = 3.7 0e).
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(2) The slope of the magnetization (virgin) part of the hysteresis loop in the range of 0 < H < 200 Oe for the PdH x (fg) sample is lower than that for Pd(bgr). (3) Only the virgin part of M(H) in the PdH x (fg) sample has a point of inflection at H ~ 3.5 Oe, the presence of which cannot be discerned from the pristine Pd(bgr) crystal in the range of 0-10 Oe.
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The dramatic contrast between pristine Pd single crystal and hydrogen-cycled Pd magnetization behaviors is caused by the magnetization contribution of the [PdH^-Pd] phase. The resulting AM(H) function is obtained by subtracting the
138
M(H) Pd(bgr) data from the M(H) PdH^fg) (Fig. 5a) shows a minor hysteresis loop with a strong diamagnetic slope that is limited by the field values H = ±20.0 Oe. This "minor" loop with a high-negative slope is located on the major loop with a much lower slope that expands over the higher magnetic field (by ff = ±200Oe).
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Similar M{H) dependences are obtained for the Pd(bgr), the PdH x (fg) and the [PdH^-Pd] phases at T = 10 K. The changes of hystersis loop at T = 50 K are accompanied by a dramatic decrease in the diamagnetic slope for the [PdH^-Pd] AM{H). A minor diamagnetic loop at low H almost disappears, and the slopes at "low" (H < 5.0 Oe) and "high" magnetic fields (10 < H < 200 Oe) become the same. The results of the M(H) measurements allowed us to calculate the slopesusceptibilities X = AM/AH for the [PdH^-Pd] phase vs. the temperature in Fig. 6, for two different ranges of magnetic field strength (H): (a) 0 < H < 5.0 Oe ("low" magnetic field) and (b) 5.0 < H < 200Oe ("high" magnetic field). As seen from (Fig. 6) in a "low" magnetic field, the slope-susceptibility X of the condensed hydrogen phase inside the dislocation cores shows a strong diamagnetic transition at T < 50 K. In the "high" magnetic field, the clearly expressed dependence of X(T) is not observed within the temperature interval 2-298 K. Notice that the X(T) dependencies in the "low" and "high" magnetic fields are quite similar to each other above T = 50 K and demonstrate a significant divergence only at T < 50 K. For comparison (Fig. 6, curve 3) shows a difference between the DC susceptibilities of Pd colloid particles (15 nm in diameter) and bulk Pd single crystal, based on the X(T) measurement data obtained from Ref. 5. It was established that the Pd particle size reduction is caused by the decrease in the paramagnetism of the
139
Pd sample due to a Stoner-factor decrease caused by the distortion and partial disordering of the Pd lattice. As seen from (curve 3), the X(T) dependence for Pd nano-particles with a bulk Pd subtraction is very similar to that for the [PdH x -Pd] phase in a "high" magnetic field (Fig. 6, curve 2). These two curves are both almost temperature independent and show negative susceptibility behavior. The distinction between these curves is only in an absolute value of X that is caused by the different size of the Pd particles involved in the X(T) subtraction procedure (curves 2 and 3).
100 150 2 0 0 250 - TsttiperaTijre (K)
50
300
100 Temperature (K)
Figure 7.
The M(H) and M(T) experimental data presented for the Pd(bgr), the PdH x (fg), as well as the [PdH^-Pd] difference, allow us to suggest that the anomalous diamagnetic response at temperatures below 30 K in the low-magnetic field was induced by the appearance of superconductivity in Pd hydride phase inside the deep dislocation cores. This suggestion would satisfactorily explain the temperature and field dependencies of the [PdH x -Pd] phase magnetization curves. Both the shape and field behavior of the magnetization curves M(H) at T = 2.0 and 10 K for the [PdH x -Pd] phase are similar to the characteristics of a non-linear, irreversible magnetization function of a type II superconductor. 4. Transport and Magnetic Measurement in Pd/PdChHa, The R(T) data for the pristine/annealed Pd/PdO(bgr) and hydrogen cycled Pd/PdO:H a; (fg) series of measurements at J = 0.1mA are presented in Fig. 1 (curves 3 and 1, respectively). As seen, the resistance of the hydrogen cycled Pd/PdO:H a; (fg) sample is lifted significantly over all temperature range 4.2-294K compared to that for Pd/PdO(bgr), apparently due to massive structural defects (dislocations) generation in the hydrogen cycled Pd/PdO:H a: (fg). These defects are able to increase temperature independent residual resistivity that is achieved at T —> 0. Hence, in order to compare temperature-dependent parts of pristine
140
Pd/PdO and hydrogen cycled Pd/PdO:H x heterostructure's resistivity , the residual resistances of both samples could be subtracted from the full R(T) values according to Matthiessen's rule for metals. The residual resistance i?i(bgr) for Pd/PdO can be determined directly from the low-temperature tail of R(T) curve and found to bei?;(bgr) = 0.862 mfi. Note that taking into account geometry of sample, the i?;(bgr) value is found to be in good agreement with the specific resistivity of Pd, containing about 2000 ppm of impurities (including 500 ppm in Pd foil plus ~1500ppm of oxygen contained in PdO layers). However, direct estimate of the i?i(fg) for Pd/PdO:H x (fg) from the low-temperature tail of R(T) curve (at T < 10 K) may not be valid due to possible effect of hydrogen cycling on the resistivity of Pd/PdChH^fg) in the lowtemperature range, where residual resistance provides maximal contribution to the full one. In this connection, in order to compare temperature-dependant parts of Pd/PdO:H x (fg) and Pd/PdO(bgr) resistivities we normalized their resistances at higher temperature (T > 120 K) where the defect contribution to resistivity is assumed to be minimized. This normalization is suggested that Pd/PdO(bgr) and Pd/PdO:H^(fg) resistances would be the same after subtracting of the excessive defect contribution (Ai? ; ) into full resistivity introduced during the hydrogen cycling of the pristine Pd/PdO, i.e [^(Pd/PdOH^) - Ai?;(fg)]/[i?(Pd/PdO)] = 1. In fact, the contribution Ai?i is roughly represented a difference between residual resistances of Pd/PdO:H x (fg) and Pd/PdO(bgr) or contribution of dislocation with trapped hydrogen into a real resistivity of pristine Pd/PdO, because AR[ « i?i(fg)—i?i(bgr). The best high-temperature normalization fit was found to be achieved at Ai? ; = 12.50 ±0.10 mfi. The graphical result of the Ai? ; subtracting from the total i^Pd/PdOrH-j,) is shown in curve 2, Fig. 7. Comparison of this result with Pd/PdO(bgr) R(T) curve (curve 3, Fig. 7), indicates close coincidence between curves 2 and 3 above T = 120 K, followed by small divergence staring below 100 K, which becomes non-negligible at T < 75 K and tends to further increase with temperature decrease. The relative resistance Rn/Ro = [-R(Pd/PdO:Hx) - 12.5mfi]/[i?(Pd/PdO] at / = 0.1mA vs. temperature is presented in inset to Fig. 7. Above T > 120 K the Pd/PdOiHj; and Pd/PdO show exactly the same resistance (Rn/Ro = 1). In the range of 120-75 K the relative resistance is slightly decreased and than at T < 70 K it is demonstrated dramatic drop, rushing to zero value below 30 K. Notice that in absence of significant decrease in the temperature-dependant part of resistance or suggesting its increase due to enhancement of electron scattering by hydrogen induced phonons in Pd/PdOiH^, the relative resistance RH/RQ would remain >1. In contrast, Fig. 7 shows a resistive transition below 75 K referred to T-dependent resistivity part of R(T) that is occurred in the hydrogen cycled Pd/PdOtH^fg) sample. Thus, the deep dislocation cores with trapped hydrogen induce a "metallization" of the Pd/PdO heterostructure below Tc ~ 75 K in terms of dramatic reduction of resistivity fraction caused by thermal phonons. Metallization of PdO surface in Pd/PdOiH^fg) sample by H-cycling is con-
141 firmed by two-point (pseudo four probe) technique allowing direct measurement of resistance in the near surface layer of Pd-PdChELj; boundary. T h e result of this measurements depicted in Fig. 8 showed decrease in relative resistance of P d - P d O : ! ^ boundary [R(Pd/PdO:Ux)/R(Pd/PdO)} vs. T. T h e resistance of a hydrogen cycled sample drops below the resistance of the pristine sample {R(Pd/PdO:Rx) < i ? ( P d / P d O ) ) at T < 75 K.
R(H)/R(0) = (Pd/PdO:H x )/R(Pd/PdO)-2 Probe, / = 0.01 mA Jy,
J?
i J
DC 0.5
0
30
%l!jr l
60 90 120 150 T e m p e r a t u r e (K)
180
Figure 8.
T h e enhanced transport properties of P d / P d O H ^ sample compared to t h a t of the pristine P d / P d O heterostructure below 70 K are supported by the I-V characteristics of this sample and found to be not peculiar to normal metallic compounds. T h e I-V characteristics at different temperatures (4.2-203 K) referenced to the relative voltage V ( P d / P d O : H a ; ) / V ( P d / P d O ) vs. transport current ranging from 1 ^ A to 1 m A are presented in Fig. 9. As seen, relative I-V characteristics reflecting a contribution of hydrogen cycling (or condensed hydrogen in deep dislocation cores) to P d / P d O transport properties, measured at lower constant t e m p e r a t u r e (4.2-50 K) demonstrate constant voltage above / — 0.1mA following by its significant drop at lower current especially below 0.01mA (curves 1-7). At the same time, the relative I-V characteristics measured at T > 50 K (curves 8-11) showed almost constant voltage over whole current range 0.001 < I < 1.0 mA suggesting peculiarities of normal metals. T h e voltage or resistance drop at low current is not usually expected for the normal metals and could be referenced to emergence of a weak superconductivity in Pd/PdO:Ha; sample because such resistivity behavior at lower current may be a t t r i b u t e d to competition between a weak superconductivity and strong localization, observed, in particular, in superconducting composite materials containing small superconducting inclusions in the non-superconducting matrix.
142
Figure 9.
Results of magnetic measurements are complied with the anomalous electron transport behavior in a hydrogen cycled Pd/PdOH x heterostructure. This data presented in Fig. 10. ZFC and FC measurement of DC susceptibility X = M{T)/H for Pd/PdO:H x (fg) and ZFC for Pd/PdO(bgr) samples showed significant difference between their temperature dependences at H = 1.0 Oe. The X(T) curves for Pd/PdO:Ha;(fg) sample at H — 1.0-1.5 Oe demonstrate slight increase of X in the range 300-100 K and then significant decrease in magnitude in the range of 10010 K. At lower temperatures (2-5 K) the foreground sample showed sharp increase in X, referenced to ferromagnetic impurities (~10ppm). In contrast, at if" = 5.0 Oe the X(T) curve does not show any drop below 100 K demonstrating increase in X with temperature decrease, following by lower temperature tale similar to that at H = 1.0 and 1.5 Oe. The behavior of ZFC X(T) for Pd/PdO(bgr) sample at H = 1.0 Oe is very similar to that of Pd/PdOrfX^fg) sample but at H = 5.0 Oe, e.g. with no sign of reduction in susceptibility below 100 K. The FC result of X(T) measurements is similar to ZFC one, while in the high-temperature range of 300100 K. Below 100 K (T = 76 K) the FC curve shows some peculiarities and finally is diverged from ZFC curve demonstrating significant growth of X below T = 50 K. The data presented in Fig. 10 are suggested strong reduction of DC susceptibility in ZFC Pd/PdO:Ha; samples below 100 K at H < 1.5 K and absence of such reduction in both Pd/PdO:H x (fg) at H = 5.0 Oe and pristine Pd/PdO(bg) at H = 1.0 Oe. In order to confirm the presence of a low-field magnetic transition in the Pd/PdO:H a; (fg) sample at T < 100 K we measured low-field (H < 20 Oe) dependence of the magnetization for both pristine and Pd/PdOiH^fg) samples versus magnetic field. We found that Pd/PdO(bgr) sample showed anticipated paramagnetic behavior that could be described by Langevin function (at low field a smooth increase in moment M with increase in H). In contrast, the M(H) data obtained at various constant temperatures (T = 2-100 K) for Pd/PdOH^ (fg)
143
— . - Pd/PdO H x (fg) ZFC, H+1.0 Oe . - & - Pd/PdO H x (fg) ZFC, H+1.5 Oe . # • Pd/PdO Hx (fg) ZFC, H+5.0 Oe -•«-.pd/PdO(bgr)ZFC, H+1.0Oe
0
60
100
150
200
280
300
T e m p e r a t u r e (K)
Figure 10.
sample (inset to Fig. 10) demonstrates significant deviation from the paramagnetic behavior in the temperature range 5.0 < T < 100 K. As seen, the M(H) curves at T — 5, 10, and 50 K possess by clear displayed inflection points in the range of 5.0-7.5 Oe. At lower field the paramagnetic slope of M(H) curves at these temperatures (reflecting magnetic susceptibility) was found to be lower that that at H > 7.5 Oe. This finding is in agreement with X(T) ZFC data for Pd/PdO:H£C(fg) sample at H < 1.5 Oe and suggests some diamagnetic contribution in X(T) signal in the Pd/PdOrH^ sample existing at low applied magnetic field and disappearing at if > 7.5 Oe. At T = 2.0K the M{H) behavior of Pd/PdO:H E (fg) sample is similar to Pd/PdO(bgr) one and could be described by paramagnetic function. This results is corresponded to X{T) data showing a significant growth of X(T) in Pd/PdO:H x (fg) samples at T < 5.0 K for ZFC/FC measurements in the magnetic fields ranging from 1 to 5 Oe (resulting in magnetic impurities). In order to determine the origin of the transition belowlOOK in Pd/PdOiH^fg) sample the more sensitive AC magnetic-susceptibility measurement at / = 1.0 kHz was performed. The real and imaginary susceptibilities of Pd/PdO(bgr) and Pd/PdO:Ha;(fg) samples were measured at if = OOe and driving amplitude h = 1.0 Oe. In Fig. 11, the comparative AC measurement data for the other Pd/PdO:H x sample oriented in parallel (if||) and normal (ifj_) directions with respect to applied magnetic field are presented. The sample demonstrated almost temperature independent susceptibility X' in the range from 150 to 30 K, showed minimum with negative X' between 6 and 20 K and then paramagnetic susceptibility rose up below 6K (low-temperature tail). The Hj_X'(T) dependence for this sample in the range of 150-60K showed behavior similar to that for H\\ measurement, but demonstrate a strong diamagnetic transition below 60 K with minimum at T — 8K. The X't(T) peak dependence for ifj_ measurement with maximum at T = 6K is also similar to Xrr(T)H\\ run, but is 4.5 times higher. The results of AC
144
i?H and H± measurements showed an emergence of diamagnetic transition below 60 K in Pd/PdOiHa; and absence of this transition in Pd/PdO(bgr) sample. In general sense, the AC transition to negative susceptibility, especially at H± orientation of the sample could reflect diamagnetic screening whether due to direct superconducting Meissner effect or due to a sharp increase in the surface conductivity (below 60 K) at the interface between Pd and PdO in Pd/PdOiHz hydrogen cycled sample due to concentration of AC current near the surface (skin-effect).
0.000101
0.00005
° f W ^AXfoS&c
o.oooooE CD
-0.00005Q. CD O 3 CO
-0.00010
-•-Pd/PdO:H x (fg), AC H, ,=1.0 Oe -*-Pd/PdO:H x (fg), AC H =1.0 Oe -o-Pd/PdO (bgr), AC H, |=1.0 Oe
15 CD
-0.00015-f •;
-0.00020-
—I— 100
150
200
Temperature (K) Figure 11.
The H± diamagnetic signal at T < 60 K in Pd/PdO:H x sample is more than one order of magnitude stronger that that for H\\. Such a ratio between X' suceptibilities with respect to field orientation is expected if diamagnetic screening is occurred at the near - the surface two-dimensional layer of the sample. This screening cannot be attributed to the simple skin-effect because the magnitude of the diamagnetic signal at T = 10K (H±) in Pd/PdOrHa; suggests about four times the conductivity increase over the Pd-PdO top layer (h ~ 40 nm) compared with the conductivity of the high-purity bulk Pd. It is, however, known that PdO deposited on the metal substrate is a semiconductor with resistivity at least three orders of magnitude higher than that for pure Pd. Thus, the low-field proofs of diamagnetic behavior vs. T in DC-mode are found for [Pd/PdO:Ha;-Pd/PdO] contribution of hydrogen trapped inside dislocation cores at the temperature range 10-100 K. The resulting irreversible non-linear magnetization behavior of M(H) at low-field H obtained for Pd/PdO:H ;r (fg) sample are
145
very similar to that that characterizing type II superconductors. Simultaneously, the direct diamagnetic transition at T = 60 K is obtained during more sensitive AC measurements (/ = 1kHz) in Pd/PdO:H a: (fg) hydrogen cycled sample, that is not appeared in original Pd/PdO(bgr) sample. These findings regarding the DC and AC results for Pd/PdOiH^ sample indicate possible emergence of HTS attributed to the condensed hydrogen phase inside deep dislocation cores at the Pd-PdO boundary. 5. Conclusions and LENR Connections In summary, our Thermal Desorption, Magnetic and Transport measurements on PdiH^and Pd/PdO:!!^ samples showed that palladium H2-cycling and subsequent annealing at T = 573 is resulted in formation of the condensed hydrogen phase inside deep dislocation cores: {x} = H/Pd = (4.0-6.0) x 10~ 4 with respect to the bulk Pd concentration. We found that inside dislocation nanotubes (dislocation core, Fig. 3) the local hydrogen concentration would be well above x = H/Pd = 1. Accordingly to SQUID magnetic measurements the gas H2-cycled PdH x single crystal sample demonstrates signatures of a weak type II superconductivity, involving the condensed hydrogen phase in deep dislocation cores (or [PdH^-Pd] phase) below 30 K. Results of both magnetic and transport measurements in electrochemically cycled Pd/PdOifLr thin foils present evidence for the direct superconducting transition below 70 K. Reproducible Meissner-effect was obtained in the low-magnetic field H = 1.0 Oe in AC field (/ = 1 kHz). That is why, the deep dislocation cores in Pd compounds must be considered as a H-dominant Pd hydride (x = H/Pd > 1.0) sites suggesting high-temperature superconducting HTS properties. In view of our findings, the deep dislocation core sites produced during deuterium loading in Pd could be referenced to the active centers of LENR triggering, which assume significant enhancement of DD-fusion probability in Pd compared to the regular lattice sites. Triggering of LENR at dislocation core sites would be strongly appreciated due to: - shortest DD-distance (close to Bohr radius as it predicted for metallic deuterium) ; - highest D-loading accompanied by a lattice compression comparable with Pd share modulus; - high-electron concentration resulting in a most effective electron screening of deuterons in Pd; - large optic phonon energy (huiv ~ 120 meV) resulting in a most effective lattice-nuclei energy transfer. Acknowledgements This work was partially supported by the NSF under Grant No. DMR-9982520. The magnetic measurements were performed at the Center for Microanalysis of
146
Materials at t h e Frederick Seitz Material Research Laboratory at UIUC. This facility is supported by the U.S. Department of Energy under Grant No. DEFG02-91ER45439.
References 1. N. W. Ashcroft, Phys. Rev. Lett. 92, 187002 (2004). 2. B. J. Heuser and J. S. King, Metal. Mat. Trans. A29, 1594-1598 (1998). 3. G. Lipson, A. Bezryadin, C. H. Castano and G. H. Miley, Bullet. APS 48 (1), 983 (2003). 4. G. Lipson, B. J. Heuser, C. H. Castano, A. Celic and G. H. Miley, J. Phys.: Cond. Matt, (submitted) 5. D. A. Van Leeuwen, J. M. Van Reitebeek, G. Schmidt, and L. J. De Jongh, Phys. Lett. A170, 325 (1992).
CALORIMETRY OF E N E R G Y - E F F I C I E N T GLOW D I S C H A R G E A P P A R A T U S D E S I G N A N D CALIBRATION
THOMAS B. BENSON The Greenview Group, Pleasanton, CA, USA E-mail:
[email protected] THOMAS O. PASSELL TOP Consulting, Palo Alto, CA, USA E-mail:
[email protected]
1. Introduction This work aims to develop a "family" of low-powered calorimetrically accurate glow discharge units, similar to that reported by Dardik et al. at ICCF-10, and to use these to test a wide range of cathode materials, electrode coatings, gas types, gas pressures, and power input levels. We will describe the design and calibration of these units. The strategy is to use a large number of very similar units so that the calorimetric response does not vary significantly for a given power level. The design is metal or sealed glass cylindrical tubes, charged with 0.4-50 Torr mixtures of deuterium, hydrogen, argon, or helium gases. Units operate from 0.2 to > 2 W power input. The units have low mass (<400g) to enhance their sensitivity to excess heat, and they are designed to allow visual observation of the discharge, on-line spectroscopic analysis of the gas to follow any changes in composition, and replication of the geometry and thermal mass during numerous changes in electrode composition. The discharges are presently powered by several power supplies, including 1000 V DC, 40 kHz, 1200 V AC, and multiple-frequency/variable-waveform modulated DC. To allow accurate measurement of "true" power, all high-voltage power supplies are driven from 6 to 12 V DC input and are enclosed in separate and redundant calorimeters. Calibration is by heat from resistors with known power input from regulated power supplies. Potential electrodes would incorporate nickel, copper, and palladium in thin film or nanoscopic form, although only a small number have been tested initially. The glow discharge has distinct advantages over the electrochemical approach. It can be operated over a much wider range of temperature; hence, if excess heat is produced, the heat will be more widely useful. A wide range of elements can be applied at either of the two electrodes without regard to their compatibility with a water-based electrolyte. The energy input can be reduced so that excess energy 147
148
signal will be more distinct, and the system can be scaled to essentially any desired size without deviating from the core design. Finally, the glow discharge area is a novel and potentially valuable area of study. Preliminary data using these two approaches show their basic feasibility in that they can be reliably calibrated. Thus far excess heat levels have been less than the known uncertainties in energy balances, which range from 5 to 30% depending on configuration. 2. Design of Apparatus 2.1. General
Layout
(1) Glow discharge tube, gas pressurized with electrodes, encased in calorimeter sleeve, and insulation (optional). Temperature measured and compared against ambient at equilibrium. (2) Driving power supply, high-voltage, miniaturized, and encased in calorimeter sleeve, with temperature measurement. (3) Temperature-controlled air-flow enclosure (optional). (4) Data capture system, logging temperature of ambient, and active elements of calorimeter, and DC power input. (5) Precision DC power supply, providing known voltage.
Figure 1.
2.2. Design
of Glow Discharge
Layout of apparatus.
Tube
Devices have been built in three different configurations, with input powers ranging from 0.2 to >2W. Configuration 1. Brass or other metal pipe approximately 40 mm in length and 30 mm in diameter serves as a cylindrical outer cathode, with an axial inner rod of
149
1-2-mm diameter, running the length of the cylinder, as the anode. The device is made vacuum-tight and includes a viewing window to monitor the progress of the glow. The anode and cathode are composed of a variety of materials. Configuration 2. Similar to configuration 1, except the entire system is enclosed in a sealed glass tube enclosure. Rolled metal foil or metal mesh is inserted into the glass sleeve, forming a cylindrical outer cathode of approximately 12-mm diameter and 100-mm length. The anode is an axial inner rod of 1-2-mm diameter, running the length of the cylinder. The anode and cathode are composed of a variety of materials. Configuration 3. A glass tube enclosure is built, encasing two opposing "hollow cup" electrodes of approximately 30-mm length and 10-mm inner diameter. Electrodes are made from tungsten with a variety of coatings. The opposing electrodes are linked by a glass tube surrounded by a wire coil; this coil is energized with RF high-frequency signal which ionizes the gas in a highly efficient manner. Highvoltage current of various types (DC, AC, and Modulated DC) is applied between the electrodes to further ionize the gas.
- RF ionizing coil
til)
Electrode connecting wire
Left fi'j.ti'.-J.in glass sleeve
Figure 2.
2.3. Gas
Opposing "cup" electrodes in sealed glass.
Handling
In configuration 1 (brass tube), standard commercial parts are assembled and made sufficiently vacuum leak tight to allow a bleed-through system to maintain 1-50 Toripressures of chosen gases or gas mixtures in a number of tubes simultaneously from a single manifold without significant levels of atmospheric or internal off-gas impurities to interfere. Configurations 2 and 3 use an initial fixed gas pressure in a sealed glass envelope which is then independent of a vacuum system or a gas
150
0 Figure 3.
Cutaway drawing of cup electrode in glass.
source and thus can be more fully enclosed for more accurate calorimetry than is practicable in the first method. 2.4. Driver
Power
Supply
The driving power for the glow discharge comes from DC high voltage (700-1200 V) or variable waveform, multi-frequency modulated DC (700-1200 V, with modulation of ±300 V in frequencies from 5 to 5000 Hz). Also an AC high-voltage unit (40 kHz, 1000 V) is used to help ionize the gas with RF energy. In all cases these driver power supplies are miniaturized and encapsulated in a small metal enclosure (on the order of a 10-cm long, 5-cm wide) which is used in online, continuous calorimetry in order to measure the true power delivered into the tube. Input power to these driver power supplied comes from regulated DC power supplies with voltage and current measured to 3-figure accuracy. The total system is capable of 3 W output but can be run stably down to less than 0.2 W by reducing the input DC. 2.5. Accurate
Measurement
of Input
Power
The calorimetry of the a low-power glow discharge system can be done with acceptable accuracy, as long as we understand some key issues related to input power. • Issue 1. In order to do calorimetry on a glow discharge system, some method of measuring input electrical power must be employed. • Issue 2. Direct measurement of "driving" power is extremely difficult, given the complex unpredictable waveforms of a glow discharge system. Dardik et al.1 has reported using a 50kHz-l MHz sampling data collection system to measure the current and voltage of a complex high-voltage AC (or modulated DC) circuit. This approach is quite expensive and requires an unusual degree
151
of effort, which many researchers may not be able to afford. Therefore, direct measurement of the AC/modulated DC power may be impractical. • Issue 3. Measure simple DC power into the power supply. The solution therefore is to measure the DC power flowing into the driver power supply that creates the high-voltage AC (or modulated DC) power. For example, in our system, we might input approximately 6 V DC, 150 mA (about 0.9 W) of steady electric current into our oscillator/amplifier circuit, which converts this DC input into high-voltage modulated DC or AC. This approach, however, requires that we understand how much of that input power is being delivered to the glow tube, and how much is lost as waste heat in the electronic circuit. • Issue 4- Conversion efficiency of the power supply varies constantly. For any given glow discharge, the amount of power lost as waste heat in the driver power supply can fluctuate from 30 to 90%. This conversion efficiency is based on gas pressure, temperature, power level, gas composition (D2, H2, or Argon), surface conditions of the electrodes (metals in glow discharge will sputter, dynamically creating and destroying nanopores in the electrode surface and changing the ionization potential of the system) and many other factors. Essentially there is no way to predict or rely on any predicable power supply conversion factor. • Solution. Real-time calorimetry of power supplies. In our system, we miniaturize all power supplies and perform calorimetry on them in parallel (usually with the same apparatus) as the glow tube itself. Therefore, we can very easily measure the low-voltage DC power and current into the system, giving us an unambiguous energy input {Qi), then measure the proportion of this DC input power that is lost as waste heat in the power supply (Q p ). The total energy into the glow tube (Q a ) can easily be seen as Q\ — Q p . In Fig. 4, we see data from our "zero" control tubes; input power Qi can be compared to the sum of the two calorimetrically measured powers Q a and Q p , demonstrating an accuracy of better than 5% accuracy. If there were excess heat being produced in the tube, we would see it easily as excess in Q a .
Power in
Power out (calculated from calorimeter)
Qi DC (W)
Q p (power supply loss) Q a (tube)
Total DC power (%)
0.1378 0.988
0.1246 90.39% 0.5854 59.25%
0.138 1.00
Figure 4.
0.0138 10.00% 0.4142 41.92%
100.39 101.17
Typical breakdown of power to supply or glow tube (control tube).
152
2.6. Calorimetry
of Tube
Calorimetry is based on measurement of equilibrium temperature of the device in air. We use two methods, based on screening speed vs. accuracy of measurement. Calorimetry Method 1. Both glow tube and power supply are enclosed in separate copper or aluminum enclosures, with the only connection being wires to conduct the low- or high-voltage currents. Thermocouples and/or thermistors (5kfi, 2% precision) are attached to the outside of the metal enclosures, which measure the equilibrium temperature reached in the ambient air environment. Calibrating heaters are installed inside the metal enclosure (adjacent to the glow tube and/or power supply) and the system is calibrated for several given levels of power. In some cases a thermal fluid is poured into the enclosure to ensure even distribution of heat inside the unit. This method is very fast, for large-scale screening of systems, but provides at best 10% uncertainty (and at worst 30%) because of low-temperature differences between the tube and ambient, variable air currents. Calorimetry Method 2. The above metal enclosures are inserted into a thick insulating body (either Dewar or Styrofoam) with only a small portion of the metal exposed to the air. This insulated body is placed in a controlled laminar airflow box with temperature-controlled ±0.1°C. The temperature of the exposed metal surface is measured by thermocouple or thermistor at equilibrium, compared to ambient. System is again calibrated for a number of input powers to an internal heater. This is similar in principle to the "double wall isoperibolic calorimetry" as described by Storms. 2 Because the heat flux is concentrated into a smaller, more controllable point of exposed metal, and the airflow and temperature are more precisely controlled, this method provides much better accuracy, with uncertainty less than 5%. Note that any number of other calorimetric approaches such as liquid isoperibolic, flow, or Seebeck, could be used with equal or better success to the above. Refer again to Storms 2 for discussion of relative merits. Data are collected using a Keithley 2700 40-channel data collection device, which feeds data into MS Excel spreadsheet on any PC. This system is simple to use and robust.
2.7. RF
Noise
Another common problem of the glow-discharge system is RF noise from the highvoltage signal or RF ionization signal. In our system this problem is avoided by enclosing both glow tube and power supply in copper or aluminum enclosures. These shield the external thermocouples or thermistors from RF noise, and also, as described above, serve as integral parts of the calorimeter. Finally, the Keithley data collection system are quite effective at filtering stray RF noise.
153
2.8. Time
Constants
Time constants vary from 30 to 45 min when exposed with no insulation to ambient air to 3h, encased in insulation, in thermally controlled enclosure. Time constants are defined as the time to reach thermal equilibrium for steady input power. Our approach assumes the excess heat, when and if detected, will be of sufficiently long and steady nature to be observable with systems with relatively long time constants. Highly fluctuating excess power would be detectable but not easily quantified by these methods. 3. Results Figures 5 and 6 give the time history of temperature of the calorimeters surrounding the power supplies feeding 40 khz AC to two "Configuration 1" tubes. These temperature differences, while generally precise to ~ 0.2°C are accurate to ~ 0.5°C. The differences in the various thermistors are not significant when looking for > 50% values of excess heat and are the primary cause of the uncertainty of up to 30% in these measurements. Of the four tubes operated simultaneously, thermal balances varied from 87 to 111% where these percentages are the observed energies in the discharges divided by the power delivered to the tubes. Similar runs were performed with Configurations 2 and 3 tubes, with similar results. No heat was seen in excess of known uncertainties. Figures 7-10 are photos of a selected set of power supplies and tubes used or developed in this research effort. 4. Discussion The above results are the first set of measurements attempted by this approach and the absence of excess heat is not unexpected. We purposely tried a much simplified experiment from that described by Dardik et al.,1 but with a great number of changes to process variables to allow us to see a wide range of behaviors in the apparatus. In the first place, we tried placing the active metals (Pd) leaf wrapped around the center electrode, with none on the cylindrical electrode surface. Then we tested palladium powders and wire. Furthermore, we used AC power, DC power, and 3-frequency modulated DC power to drive the glow. Finally, we used mixtures of argon and deuterium, in addition to pure deuterium, to test a variety of discharge modes. Different configurations were shown to have different advantages: (1) Configuration 1 (gas bleed through system) allows the measurement of any product gases generated within the discharges to be captured and subjected to various measurements of composition on the fly. It comes to equilibrium quickly and is quicker to build, so that very large numbers of materials to be screened very quickly, although it is less accurate. (2) Configurations 2 and 3 (sealed glass tubes) have important advantages. They do not need a continuously operating vacuum system or gas supply.
154
They can employ much cleaner electrodes, more free of surface contamination. Their calorimetry is slightly more complex with a longer time to reach thermal equilibrium, but they are small enough to fit inside a small temperature-controlled chamber, which gives them greater accuracy. Additionally the sealed glass tube can be run for extended periods of time, allowing product gases to accumulate to higher concentrations. 5. Conclusions Methods have been developed for efficient screening of candidate materials on electrode surfaces of glow discharge tubes that will provide an environment conducive to nuclear reactions between deuterium and itself or other light elements. This method can detect excess heats ratios >1.2 with more than 95% certainty. It provides a valuable new platform for large-scale exploration of excess heat effects in the gas phase, using low-power inputs in the 0-3 W range. This method proves to be inexpensive, quick, accurate, and easy to perform once the basics are mastered. Note: The authors are interested in testing electrode materials from other sources, especially those that have already been successful in a liquid (electrolytic) environment. Also we would be pleased to provide advice or equipment to other researchers. Interested parties please contact the authors. Acknowledgments We are indebted to many of our colleagues in the research community for helpful discussions. In particular Arik El-Boher, Mike McKubre, and Russell George were generous in answering our questions. Bill McCarthy with whom we share laboratory space and Ed Wills have been helpful in building our apparatus. The skills of persons employed by Microscientific Glass Blowing Co. of Milpitas, CA have contributed to apparatus design. References 1. I. Dardik, H. Branover, A. El-Boher, D. Gazit, E. Golbreich, E. Greenspan, A. Kapusta, B. Khachatorov, V. Krakov, S. Lesin, B. Michailovich, G. Shani, and T. Zilov, Intensification of low energy nuclear reactions using superwave excitation, in Proceedings of the Tenth International Conference on Cold Fusion (Camridge, MA, USA, August, 2003); Text available at LENR-CANR.org. 2. E. Storms, Calorimetry 101 for Cold Fusion; Methods, Problems and Errors, 2004; LENR-CANR.org.
155
Additional Lists of Figures
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Photo of sealed-glass type glow tube (mounted on vacuum station).
G E N E R A T I O N OF HEAT A N D P R O D U C T S D U R I N G P L A S M A ELECTROLYSIS
TADAHIKO MIZUNO AND YOSHIAKI AOKI Hokkaido
University,
Kita-ku
Kita-13
Nishi-8,
Sapporo
060-8628,
Japan
DAVID Y. C H U N G A N D F . S E S F T E L Department
of Physics,
Howard
University,
Washington
DC 20059,
USA
Direct decomposition of water is very difficult in normal conditions. Hydrogen gas can be usually obtained by electrolysis or by a pyrolysis reaction at high temperatures, starting at approximately 3700°C. However, as we have already reported, anomalous heat generation can occur during plasma electrolysis, and this process makes it rather easy to achieve both electrolysis and pyrolysis simultaneously. In this paper we describe anomalous amounts of hydrogen and oxygen gas generated during plasma electrolysis. The generation of hydrogen far in excess of amounts predicted by Faraday's law is continuously observed when conditions such as temperature, current density, input voltage, and electrode surface are suitable. NonFaraday generation of hydrogen gas sometimes produces more than 80 times as much hydrogen as normal electrolysis does. Unfortunately there have been few claimed replications of excess hydrogen, even in rare cases in which excess heat is claimed. In most cases, no excess heat or hydrogen is observed. The reaction products found after electrolysis were different after excess heat generation.
Keywords: plasma electrolysis, pyrolysis, hydrogen generation, transmutation 1. Introduction Hydrogen gas can be easily obtained by electrolysis. However, direct decomposition of water is very difficult in normal conditions. The pyrolysis reaction occurs at high temperatures, starting at approximately 3700°C. 1,2 We have already reported anomalous heat generation during plasma electrolysis.3'4 Some researchers have attempted to replicate the phenomenon, however, they report difficulty generating a high level of excess heat. They tend to increase input voltage to a very high value, hundreds of volts, a technique we do not recommend. It is very important to replicate the excess heat and other products during plasma electrolysis. The generation of hydrogen in excess of Faraday's law is continuously observed then conditions such as temperature, current density, input voltage and electrode surface are suitable. Non-Faraday generation of hydrogen gas sometimes produces more than 80 times as much hydrogen as normal electrolysis does. Usually, the plasma state can be easily started if input voltage is increased up to 140 V at a rather high temperature. 5 ~ 7 when the plasma forms, a great deal of vapor and 161
162
hydrogen gas are released from the cell. At the same time, this effluent gas removes heat (enthalpy), which then cannot be detected with calorimetry based only on temperature. It is difficult to calibrate the exact enthalpy balance. A mixture of gas and heat is especially complicated and difficult to measure. In this paper we describe a heat measurement system used to during plasma electrolysis that accounts for all enthalpy. 2. Experiment 2.1. Electrolysis
Cell
Figure 1 shows the experimental set up. We measure many parameters including sample surface temperature, neutron and X-ray emission, mass spectrum of gas, input and output power, and so on. Figure 2 shows the schematic sketch of the cell and measurement system. 1 ' 2 The cell is made of the Pyrex glass 10 cm diameter and 17 cm in height and 1000 cm 3 in solution capacity. It is closed with a Teflon rubber cap, 7cm in diameter. The cap has several holes in it, three for platinum resistance temperature detectors (RTD) (Netsushin Co., Plamic Pt-lOOfi), two for the inlet and outlet of the flowing coolant water, and one to hold a funnel that captures the effluent gas from the cathode. The funnel is made of quartz glass, and is 5 cm in the diameter at the top of the cell, and 12 cm in length. Gas leaving the top of the funnel flows into a water-cooled condenser, which is connected to the funnel with another Teflon rubber cap. This is shown in Figs. 3 and 4. 3. Measurement of Hydrogen Gas A mixture of steam, hydrogen and oxygen (from pyrolysis) passes from the cell to the condenser. The steam condenses and falls back into the cell. An 8-mm diameter Tigon tube is coupled with the gas exit of the condenser, connecting it to a gas flow meter (Kofloc Co., Model 3100, controller: Kofloc Co., Model CR-700). The flow to voltage transformer element is a heated tube of thermal flow meter system, the minimum detection rate of hydrogen gas flow is 0.001 cm 3 /s, and the resolution is within 1%. The power output from the measurement system was led to the computer through a logger. After path through the flow meter, the gas goes to a mass spectra analysis system. A small amount of constant volume of the gas such as 0.001 cm 3 /s paths continuously through a needle valve and was analyzed by a quadruple mass analysis method. The main composition of gas released from the cathode was then continuously analyzed by above-mentioned method. 3.1.
Calorimetry
Temperature measurements were made with 1.5-mm diameter RTDs. Calorimetry was performed by combining the flow and isoperibolic method.
163
Figure 1.
Photo of the experimental setup.
Flow calorimetry is based on the temperature change of the cooling water. The cooling water is tap water flowing through Tigon tubing. It passes first through a constant temperature bath to keep the temperature constant. From there, it flows through the outer jacket of the condenser, and then through the coil of tubing wrapped around the funnel. (The outside of this cooling water coil is covered with the anode and a platinum mesh.) The flow rate is measured with a turbine meter (Japan Flow Control Ltd., Model T-1965B). The inlet temperature is measured before the cooling water enters the condenser, and outlet temperature is measured where it exits the cell. Heat from both condensation and glow discharge electrolysis are combined together. Isoperibolic calorimetry is performed by placing three other RTDs were in the cell electrolyte at different depths in the solution to measure the temperature. The solution is mixed with a magnetic stirrer. Figure 5 shows the notional sketch for heat measurement. Heat out can be divided into several factors. These are energy for water decomposition, heat of
Figure 2.
Sketch of experimental setup.
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Detail of the gas measurement.
electrolyte, heat bring by the coolant, heat releasing from the call wall, and heat releasing with the vapor through the cell plug. The heat balance is estimated by input and output formulas, input and output power is given in the following equations: Input (J) = / (current) x V (Volt) x t,
Out =
Hg+Hw+HC+Hr+Hy,
here, Hg = Heat of decomposition — / 1.48 x dl x di,
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-/-
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Glass dome Coolant coil Pt anode Rectangular Pt had an integral lattice constructed using a 15 cm length of 0,1 cm in diameter. 15 cm in height
Figure 4.
Photo of cell.
165
where Ww is the electrolyte weight, C w heat capacity, and ST is the temperature difference. Hc = Heat of coolant =
Wc x Cc x ST,
where Wc is the coolant weight, C c heat capacity, and ST is the temperature difference. HT = Heat release = / (Ww xCw + Wcx
CC)T,
where Tr is the temperature change. Hv = vapor = Wv x Cc.
Fxcess gas Hc: Heat of coolant Hg: Heat of decomposition
Figure 5.
Schematic representation of heat balance.
The heat balance calculation is straightforward. Input power is only from the electric power source. Output is divided into several parts. The first factor is heat of water decomposition (designated Hg). It is easily calculated from the total electric current. The second factor is electrolyte enthalpy (Hw). It is easily derived from the solution temperature difference. The third factor is heat removed by the coolant (Hc). This is measured from the temperature difference between the coolant inlet and outlet, and the coolant flow rate. The fourth factor is heat release from the cell (-ffr)- This is rather complicated and can be estimated with a semi-empirical equation. The fifth factor is heat release by vapor (Hv). This is difficult to measure precisely. However, I have measured most of the heat in the condenser directly by monitoring the inlet and outlet temperature of the cooling water that passes through the condenser outer jacket.
166
I Figure 6.
W sample. Left, before; Right, after glow discharge electrolysis.
If there is excess hydrogen and oxygen gas, we have to measure the gas volume precisely, because even a small volume of gas removes a large amount of enthalpy. This is done with the precision gas flow meter. The first factor, water decomposition (jffg) has a large effect on the rest of the equation. 3.2. Electrode
and
Solution
The electrode is tungsten wire, 1.5 mm in diameter and 15 cm in length. The upper 13 cm of the wire is covered with shrink-wrap Teflon and the bottom 2 cm is exposed to the electrolyte and acts as an electrode. The light water solution was made from high purity K 2 C 0 3 reagent at 0.2 M concentration. 3.3. Power
Supply
Data from the electric power supply (Takasago, Model EH1500H) were collected with a power meter (Yokogawa Co., Model PZ4000) and averaged every 5s. The sampling time was 40 us and the data length were 100 k.
Figure 7.
Photo of power supply.
167
Figure 8.
3.4. Data
Photo of EDX.
Collection
All data, including the mass of cooling water flow from the flow calorie measurement, the temperature of coolant entrance and exit, electrolyte temperature measured by three RTDs, input voltage, current, electric power and the amount of the hydrogen gas generated were collected by a data logger (Agilent Co., Model 34970A), and stored in a personal computer.
3.5. Element
Analysis
The sample electrodes and the electrolyte were subjected to element detection by means of energy dispersive X-ray spectroscopy (EDX), Auger electron spectroscopy (AES), secondary ion mass spectroscopy (SIMS) and electron probe microanalyzer (EPMA).
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4. Results We changed the input voltage stepwise as shown in Fig. 10. In this example, plasma formed at 120 V. Once plasma formed, input current suddenly dropped. Meanwhile, the solution temperature reached roughly 80° C. We increased voltage in stages to 350 V and then decreased it to 100 V. Plasma continued at 100 V and ceased at 80 V.
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Change for input voltage, current and Temperature.
The gas collected by the funnel over the cathode is collected by the Q-massspectrometer continuously as shown in Fig. 11. It is mainly composed of three gasses: hydrogen, oxygen, and nitrogen were always detected. Other gases were under the background levels and were not detected after electrolysis started. Oxygen gas increased after plasma electrolysis occurred. Hydrogen gas appeared when electrolysis started. When plasma electrolysis began, hydrogen production decreased while at the same time oxygen increased. The increased oxygen gas means that
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H2 and O2 ion current and the ratio over time in 1000 s.
direct water decomposition by pyrolysis had begun. (Although total hydrogen production decreases when glow discharge begins, "excess hydrogen" increases. In other words, the ratio of hydrogen to input power sharply increases, glow discharge consumes much less power than ordinary electrolysis, and power falls even more than hydrogen production does.) The behavior of the hydrogen isotope molecules is the same as hydrogen molecular ion. Figure 12 shows changes over time for hydrogen and oxygen molecules and their ratio. The ratio increases as input voltage increases, reaching 0.45 at 2500 s and 350 V. This means the gas from the cathode had begun direct decomposition by pyrolysis. The ratio of the hydrogen in gases released from the cathode is exactly same as the Faradaic value from the current. The equation is (i7!—0.1161) x 0.667 + 0.1161. Here, F\ is the rate of hydrogen gas estimated from the flow meter and, I is current. The factor of 0.116 is the rate of ordinal hydrogen generation, i.e., 0.5 x 22 414/F (F, Faraday constant of 96 500C/mol). The factor of 0.667 is atomic ratio of hydrogen for water.
Figure 13.
Hydrogen generation over time.
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Figure 13 shows the changes of hydrogen generation estimated from current, and measured with the gas flow meter. These rates were same with ordinary electrolysis. However, the value measured by the flow meter shows an upward deviation compared the value estimated from the current. The change of the ratio between these two values, i.e., current efficiency (e) and the ratio of the oxygen gas to the total generation with hydrogen from the cathode are shown in Fig. 4c. Here, e exceeds unity when the plasma electrolysis started, gas generation increased with the input voltage. It reached as 8000% at 350 V input voltage. The ratio of oxygen reached 30%. This means that almost all of the hydrogen came from water decomposition (pyrolysis) during high voltage plasma electrolysis. Figure 14 shows the change of the ratio between these two values, i.e., current efficiency (e) and the ratio of the oxygen gas to the total generation with hydrogen from the cathode. Here, the e exceeded unity when the plasma electrolysis started; gas generation increased a great deal with the input voltage. It reached as much as 8000% at 350 V. For the entire run, the theoretical value of hydrogen generation calculated from the input current was 1144 cm 3 , and the value measured during plasma electrolysis was 2190 cm 3 . That is, the generation of excess hydrogen during a whole electrolysis reached 1046 cm 3 . For measurements made only during times when the plasma was present, the measured value was 1470 cm 3 compared to the theoretical value were 460cm 3 , so the excess was 1010cm 3 . Figure 15 shows the e and V relationship. Here, it can be seen that e has a tendency of increase with input voltage. Some points of e value under 100 V in the figure show up to twice the theoretical value of unity; these points were obtained during plasma electrolysis. On the other hand, e remains at unity during normal electrolysis. It can be expected that if the input voltage is increased up to several hundred volts, then e would far exceed unity. Figure 16 also shows the ratio of excess hydrogen to input power. These values were subtracted from the faradic hydrogen from the previous graph and converted into units of energy. It shows steep increase with the input voltage. It exceeds 10% and sometimes reaches 30%.
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Figure 17 shows the heat balance for the run shown in Fig. 16. This indicates no excess heat. However, during this run, enthalpy release from excess hydrogen and oxygen evolution was not measured. So, there may be excess enthalpy, but in this case it can only be said that the heat balance was almost 100%. Figure 18 apparently indicates a tendency of the excess hydrogen generation with the negative excess heat. The total endothermic heat was calculated as 6540 J during plasma electrolysis. Figure 18 shows an example in which no excess heat was generated. We changed the input voltage stepwise as shown in Fig. 19. We used 0.1 M of K2CO3 electrolyte. Plasma formed at 120 V. Once plasma formed, input current dropped. The solution temperature reached 70°C. We increased voltage in stages to 320 V and then decreased it to 100 V. Plasma continued at 140 V and ceased at 100 V. Figure 20 shows the changes of hydrogen generation estimated from current and flow meter. The value estimated by flow meter exceeded the value of the current estimation.
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If there were no excess heat, apparently the points for the excess hydrogen distribute around the no excess heat region like Fig. 21, that means the difference between heat out and electric power is zero. Figure 22 shows the e and V relationship for plasma electrolysis in 0.1 M of K2CO3 electrolyte. Figure 23 shows an example of excess heat. We changed the input voltage stepwise as shown in the figure. In this case, we used 0.05 M concentrate K2CO3 electrolyte. The plasma electrolysis started at 120 V. Once the plasma formed, input current dropped. The solution temperature was 80°C. We increased the voltage stepwise to 320 V and then decreased it to 100 V. Plasma continued at 160 V and ceased at 120 V. Figure 24 shows the changes of hydrogen generation estimated from current and flow meter. The value estimated by flow meter exceeded the value of the current estimation.
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Figure 25 shows another relationship, between excess hydrogen and excess heat. In this case, the exothermic heat was estimated as 1100 J during plasma electrolysis.
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In all three cases, I have considered the contribution of excess hydrogen formation. However, apparently, the heat balance was not unity, it was changed by other parameters. Figure 26 shows the e and V relationship for the plasma electrolysis in 0.05 M of K2CO3 electrolyte. We have analyzed the elements in the electrode and electrolyte by EDX and XPS, to estimate all of the elements in the electrolysis system. After electrolysis the element deposition for these three cases changed, as shown in Fig. 27. These depositions were also observed in various cases with electrolysis systems. 8 - 1 2 There were several major elements observed in the system after excess energy was released. These were Ca, Fe, and Zn. On the other hand, In and Ge were detected after systems were endothermic (absorbing heat). However, no major changes in
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It is still difficult to determine the conditions needed for excess energy generation. However, our results strongly suggest that we have to consider the contribution of the excess hydrogen. Sometimes the occupation percentage of excess hydrogen to the input energy reached to 30%. After that, we obtained excess energy during the plasma electrolysis. However, excess energy generation only continued for several hundred seconds. One of the key factors that produce the excess energy seems the input voltage. Hydrogen general ion and heat generation seems to correlate with the input voltage. Energy output can go over unity during plasma electrolysis if the input voltage is kept very high. Apparently, we have sometimes replicated excess heat generation at high input voltage region, even though the duration of the reaction is brief. One point of e value in the figure shows up to 80 times of the theoretical value of unity; the point was obtained during plasma electrolysis at 350 V. On the other hand. e remains at unity for all other normal electrolysis. Our equipment is only capable of producing 350 V. Il can he expected that if the inpul voltage were increased to several hundred volts, the excess heat would greatly exceed unity. 5. Conclusions We have reached several conclusions: (1) current efficiency for the plasma electrolysis reaches 8000% to the input current. (2) power efficiency for the plasma electrolysis reaches 30% to the input voltage, (3) in some cases, excess heat was observed, (4) in other cases, no and endothermic heat were confirmed, (5) the reaction products after electrolysis were changed with the excess heat generation.
177 Acknowledgment We wish to express our thanks t o the T h e r m a l and Electric Technology Foundation for funding this research.
References 1. H. Arakawa, Creation of new energy by photocatalyst: technology of clean hydrogen fuel production from solar light and water, Reza Kenkyu 25(6), 425-430 (1997). 2. R. Rocheleau, A. Misra, and E. Miller, Photo electrochemical hydrogen production, P r o a , 1998 US-DOE, Hydrogen Program Review, NREL/CP-570-25315. 3. T. Mizuno, T. Ohmori, T. Akimoto, and A. Takahashi, Production of heat during plasma electrolysis in liquid, Jpn. J. Appl. Phys. 39(10), 6055-6061 (2000). 4. T. Mizuno, T. Akimoto, and T. Ohmori, Confirmation of anomalous hydrogen generation by plasma electrolysis" H. Yamada (Ed.), in Proceedings of the 4th meeting JCF Research Society, October 17-18 (2002); Iwate University, Japan 27-31 (2002). 5. A. Hickling and M.D. Ingram, Trans. Faraday Soc. 60, 783 (1964). 6. A. Hickling, Electrochemical Processes in Glow Discharge at the Gas-Solution Interface, J.O'M. Bockris and B.E. Conway (Eds.) Modern Aspects of Electrochemistry (Plenum Press, New York, No. 6, 329-373, 1971) 7. S.K. Sengupta, O.P. Singh, and A.K. Srivastava, J. Electrochem. Soc. 145, 2209 (1998). 8. T. Mizuno, T. Akimoto, T. Ohmori, A. Takahashi, H. Yamada, and H. Numata, Neutron evolution from a palladium electrode by alternate absorption treatment of deuterium and hydrogen, Jpn. J. Appl. Phys. Part 2, No.9A/B, Vol. 40, L989-L991 (2001). 9. T. Mizuno, T. Ohmori, and M. Enyo, anomalous isotopic distribution in palladium cathode after electrolysis, J. New Energy 1(2), 37 (1996). 10. T. Mizuno, T. Ohmori, K. Kurokawa, T. Akimoto, M. Kitaichi, K. Inoda, K. Azumi, S. Shimokawa, and M. Enyo, Anomalous isotopic distribution of elements deposited on palladium induced by cathodic electrolysis, Denki Kagaku oyobi Kogyo Butsuri Kagaku 64, 1160 (1996) in Japanese. 11. T. Mizuno, T. Ohmori, and M. Enyo, Isotopic changes of the reaction products induced by cathodic electrolysis in Pd, J. New Energy 1(3), 31 (1996). 12. T. Mizuno, T. Ohmori, and M. Enyo, Confirmation of the changes of isotopic distribution for the elements on palladium cathode after strong electrolysis in D2O solutions, Int. J. Soc. Mat. Eng. Resources 6(1), 45 (1998).
EXCESS HEAT P R O D U C T I O N I N P d / D D U R I N G P E R I O D I C P U L S E D I S C H A R G E C U R R E N T IN VARIOUS C O N D I T I O N S
A. B. KARABUT FSUE "LUCH", 24 Zheleznodorozhnaya St, Podolsk Moscow Region 14S100, Russia Experimental data from low-energy nuclear reactions (LERN) in condensed media are presented. The nuclear reactions products were found in solid cathode media used in glow discharge. Apparently, the nuclear reactions were initiated when bombarding the cathode surface by plasma ions with the energy of 1.0—2.0keV. Excess heat from a high current glow discharge reaction in D2, Xe, and Kr using cathodes already charged with preliminary deuterium-charged Pd and Ti cathode samples are given. Excess heat up to 10-15 W and efficiency up to 130% was recorded under the experiments for Pd cathode samples in D2 discharge. Excess heat up to 5 W and efficiency up to 150% was recorded for Pd cathodes that were charged with deuterium before the run, in Xe and Kr discharges. At the same time excess heat was not observed for pure Pd cathode samples in Xe and Kr discharges. The formation of impurity nuclides ( 7 Li, 1 3 C , 1 5 N, 2 0 Ne, 2 9 Si, 4 4 Ca, 48 Ca, 5 6 Fe, 5 7 Fe, 5 9 C o , 6 4 Zn, 6 6 Zn, 7 5 As, 1 0 7 Ag, 1 0 9 Ag, 1 1 0 Cg, l n C g , 1 1 2 Cg, 114 Cg, and 1 1 B In) with the efficiency up to 1 0 1 3 a t . / s was recorded. The isotopic ratios of these new nuclides ware quite different from the natural ratios. Soft Xray radiation from the solid-state cathode with the intensity up to 0.01 Gy/s was recorded in experiments with discharges in H2, D2, Ar, Xe, and Kr. The X-ray radiation was observed in bursts of up to 10 6 photons, with up to 10 s bursts per second while the discharge was formed and within 100 ms after turning off the discharge current. The results of the X-ray radiation registration showed that the exited energy levels have a lifetime up to 100 ms or more, and the energy of 1.22.5 keV. A possible mechanism for producing excess heat and nuclear transmutation reactions in the solid medium with the exited energy levels is considered.
1. Introduction We have conducted experimental research on low-energy nuclear reactions (LENR). By LENR we mean nuclear reactions initiated by a low-energy action (from units up to a thousand of eV) in condensed media. Under such a low-energy action the non-equilibrium energy states with a temperature up to 3keV and lifetimes up to tens of milliseconds can be formed in the condensed medium. Occurrence of such states was found during the experiments when registering X-rays with energy up to 3 keV. Hypothetically, X-ray emission and other accompanying effects indicate a fundamentally new physical phenomenon unknown before: metastable long-living (up to tens of milliseconds) states with the excitation energy of 1-2 keV and more are formed in the crystal solid lattice within the solid when bombarding its surface by plasma ions of an electrical discharge. Therefore, L, M excited energy states with 178
179
the occupation density n v _ d (cm - 3 ) and characteristic temperature TL,M ~ 1-2 keV and more (20,000,000°K) are formed in the solid after each pass of the current glow discharge pulse. These power conditions exist for the characteristic time TL,M (up to 100ms and more). Realization of nuclear reactions of transmutation with evolving heat power and accumulation of impurity elements within the cathode material is possible in such medium. The probability of such reactions proceeding is defined by the characteristic temperature, excitation energy level density, and lifetime of excited levels. These nuclear reactions (LENR) can be called non-equilibrium nuclear reactions. The experimental measurements of the excess heat yield, anomalous isotopes in the cathode material, heavy particle emission and soft X-rays at large densities of the discharge current were carried out with a device that underwent high-current glow discharge for a long time. As applied to developing a long operating reactor for the heat power production, the research was carried out on the modes with small density of discharge current, to finding a possible mechanism of initiating nonequilibrium nuclear transmutation reactions in the solid medium of the cathode sample. 2. Measurement of Excess Heat by a flow Calorimeter The measurements were carried out using the glow discharge device consisting of a water-cooled vacuum chamber, cathode and anode assemblies. The cathode design allowed placing the cathode samples made of various materials on the cooled surface. The device consisted of three units: the cathode, anode and chamber had independent channels of water-cooling. Each cooling channel included two thermocouples at the inlet and outlet, and a flow meter. The device was placed into a thermal insulating package (Fig. 1) and was a flow calorimeter. Non-deuterium-charged Pd cathode samples in Xe and Kr discharges were used in the tests. In contrast to the experiments carried out before, the mode of "plasma anode" was used. The anode was set out at the chamber wall (Fig. 1) and was put into the plasma area being above the cathode. The pulse-periodic electrical power supply was used. The electrical parameters: discharge current and voltage were recorded using a two-channel computer digital oscillograph. The electrical power was determined according to the expression
Pel = ^Ju(t)I(t)dt. When excess heat was released inside the chamber P E H , its value could be determined by ^EH = (PHC + PliA + P HC h) " -Pel ± AP e r r o r ,
(1)
where Pei is the input electrical power of the glow discharge, PHC, PHA, and Pnch are the output heat power by the cooling water of the cathode, anode, and chamber, respectively, AP e r r o r is the complete absolute error of the power measurement for
180
Figure 1. Experimental glow discharge device (flow continuous calorimeter). 1, vacuum discharge chamber; 2, cathode unit; 3, anode unit; 4, thermal insulation cover; 5, insulation of the anode cooling system; 6, the chamber cooling system; 7, the discharge chamber tube; 8, the chamber cooling jacket tube; 9, windows in thermal insulation cover; 10, the vacuum hose; 11, insulation of the cathode cooling system; 12, Be window; 13, X-ray detector.
given measuring system, T is the period of following the pulses of the glow discharge current. The measurements system allowed to record the electrical power input into the discharge and heat capacity output by the cooling water with accuracy of 0.6 W at the absolute value of the electrical power up to 120 W. (Relative error ±0.5%.) Two typical operating modes of the device were used in the experiments. Highdensity discharge current (more than 20mA/cm 2 ) was used in the first set of experiments. Under these modes deuterium loading into Pd cathode samples did not take place. The absolute excess power had a large value (up to 20 W) but total efficiency coefficient was less than 130% (Fig. 2). In the other set of experiments the current density did not exceed 100mA/cm 2 . Under such values of the discharge current in D2, continuous loading of D2 into Pd ran up to saturation. The experiments were carried out with Pd cathode samples in D2 discharge, with the preliminary deuterium-charged Pd cathode samples in Xe and Kr discharges. The amount of D2 loaded into the cathode was determined by reducing the pressure in the chamber. The D2 was periodically supplied into the chamber for maintaining the required pressure. Deuterium loading was determined by the volume of the gas absorbed from the discharge chamber. When high loading was achieved, the D/Pd ratio was close to 1.
181
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Figure 2. Excess heat (a) and efficiency (b) in relation to input electric power. Cathode sample - Pd, d = 9 mm, gas-D 2 ; 1 - j = 1 2 m A / c m 2 , 2 - 2 2 m A / c m 2 , and 3 - 7 0 m A / c m 2 .
T h e heat measurements were carried out for P d cathode samples in glow discharge when changing the following parameters: discharge current density, voltage, duration of current pulses and time period between the current pulses of the power supply. T h e absolute value of the excess heat power and thermal efficiency grew with increasing power input into the discharge (Fig. 3). T h e maximum excess heat power and thermal efficiency were recorded under the following conditions: while loading D into P d took place, or when D left Pd; and when the time period between the current pulses was much greater t h a n the duration of the discharge current pulses. This result showed t h a t the excess heat continued in the cathode sample after the current was t u r n e d off (during the time period between the current pulses). T h e maximum value of the excess heat was recorded at the discharge burning voltage of 1000-1400V. Large values for excess heat power and thermal efficiency were recorded for previously deuterium-charged cathode samples in Xe and Kr discharges (Fig. 4). Two typical groups of the results can be noted: relatively large values of the excess
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Figure 3. Excess heat (a) and efficiency (b) in relation to input electric power. Cathode sample - Pd, d = 9 mm, gas-D2; 1, D2-charged Pd with D2 loading and unloading; 2, D2-charged Pd without D2 loading or unloading.
heat power and efficiency coefficient (curve 1) and the group of results with lower values for excess heat power efficiency coefficient (curve 2). The large values of the excess heat power and efficiency coefficient were observed when partial loading of deuterium into Pd cathode samples took place, or when deuterium left Pd cathode samples. Excess heat was not produced using cathodes made of pure Pd (not deuterium charged) in Xe and Kr discharges (Fig. 5). Thus, it was experimentally shown that excess heat production was defined by two processes: (1) deuterium should be loaded into the medium of the crystal solid lattice. (2) The crystal lattice should obtain initial excitation; high-energy long-living exited levels should be created in the solid. These exited conditions could be created by an additional source (e.g., by a flow of inert gas ions).
183
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The three-channel system of separate recording of the output heat power (anode, cathode, and chamber) allowed us to define the structure of the excess heat during glow discharge. As Figs. 6 and 7 show the high-efficiency values were recorded in the experiments with the large relative heat release on the cathode. These results show that the excess heat was released mainly on the cathode.
184
Efficiency (%)
Pd-Kr
105
100 95 J
0
i
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3. Registration of Anomalous Nuclides The analysis of impurities and or possible anomalous nuclides in the cathode sample material before and after the experiments when using the device of the high-current glow discharge1 was made, assuming that the recorded excess heat 1 was caused by nuclear reactions. 2 The following methods were used: spark mass spectrometry, secondary ionic mass spectrometry, and secondary neutral mass spectrometry. Difference in the content of the anomalous elements before and after the experiment was defined as storage of the elements during the experiment. The secondary ion mass spectrometry (SIMS) analysis included the following operations: removal the upper 1.5 nm layer of the cathode surface by plasma etching;
185 Efficiency (%)
160
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Figure 7. Dependence of excess heat and efficiency on parameters: relation of heat power released on cathode to electrical power input into discharge. 1, D2-charged Pd with D2 loading and unloading; 2, D2-charged Pd without D2 loading or unloading.
scanning the first and second layers down 5nm to determine the content of any anomalous nuclides that might be present, removal another layer 700-nm thick and repeating the scan of the third and fourth layers to a 5-nm depth (Fig. 8).
800 nm
5 nm
1.5 nm
Figure 8. Registration procedure for the impurity contents in the cathode samples (methods SIMS and SNMS). 1, dirty superficial layer; 2 and 3, analyzed layers; 4, surface of the cathode samples; 5, removal of a metal layer; 6 and 7, analyzed layers.
186
Anomalous or impurity elements with the mass approximately half as large as Pd and with mass close to Pd mass were recorded in the near-surface layer having the thickness of 100 nm in amounts up to several dozen percent. The main elements (those with more than 1% of the content) were 7 Li, 1 2 C, 15 N, 20 Ne, 29 Si, 44 Ca, 48 Ca, 56 Fe, 57 Fe, 59 Co, 64 Zn, 66 Zn, 75 As, 107 Ag, 109 Ag, 110 Cg, m C g , 112 Cg, 114 Cg, and 115 In (Table 1). The impurity content in the cathode bulk sample at different depths was defined. The content at the depth of 800 nm decreased by 1.5-2 times in comparison with the near-surface layers (Fig. 9, Table 1).
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The results of these measurements show that production of the anomalous nuclides occurred in the sample material at depths of up to 1000 nm (up to 4000 at. layers) from the cathode surface.
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4. X-Ray Registration Intensive X-ray emission from the solid medium of the cathode samples was recorded in the experiments. The recording of the X-rays was carried out using thermoluminiscent detectors (TLD), X-ray film, and scintillator detectors with photomultipliers. 1 The TLD on the base of AI2O3 crystal recorded the values of penetrating radiation, starting from the background values of the environment radiation. These were used to measure the intensity and evaluating the average energy of the soft X-ray emission from the cathode. The detectors are in the form of disks with a diameter of 5 mm and thickness of 1 mm, enclosed by beryllium foil of various thickness (15, 30, 60, 105, 165, 225, and 300 /jm) were arranged above the cathode in the special cassette (seven-channel spectrometer). The evaluation of the X-ray energy was made according to changing the radiation dose adsorbed by the TLD detectors provided with Be shields of various thickness. The radiation intensity (dose power) was defined as the radiation dose absorbed by the detector divided by the experiment time. This expression, and a dependence chart of lg thickness of the half absorption on lg energy of X-rays for beryllium, were used to evaluate the X-ray energy. The values of lg thickness of the half absorption from lg energy of X-rays for beryllium were taken from Ref. 2, Appendix G. The radiation dose absorbed by the TLD detectors was reduced by an order of magnitude in the 300/xm Be foil compared to the 15 /im foil (Fig. 10). The main component of X-ray energy was in the range of 1.0-1.5 keV. The value of the X-ray energy determined experimentally increased from 1.2 to 1.5 keV when increasing the thickness of the Be shield from 15 to 300/im (Fig. 11). It could be assumed that X-rays was emitted from the bulk of the solid-state cathode medium. The part of the radiation from the deeper layers lost initial energy when passing the cathode material. In this case, the energy radiation spectrum was displaced to the side of reduced energy. The initial X-rays energy was evaluated as 1.5-2.5 keV. The time X-rays characteristics were studied using the scintillator detectors with the photomultipliers. 1 These measurements showed that X-rays emission was observed as a lot of bursts up to 109 photons in a burst. The single bursts were recorded after turning off the discharge current within 85 ms (Fig. 12).
5. Discussion The experiments results with the high-current glow discharge carried out for several years to allow allocating the basic processes and conditions of their running. (1) Production of the excess heat. Excess heat was produced in the bulk of the solid-state medium of the cathode sample under the following conditions: • Deuterium should be loaded into the solid-state cathode medium. • Initiating excitation of the energy levels of the crystal lattice of the cathode material was necessary.
189
Background dose
100
300
200
Figure 10. The X-ray dose absorbed by TLD detectors covered with Be foil with the different thickness. Pd—D system; current, 200 mA; the exposure time, 6000 s. 1, discharge voltage is 1750 V; 2, 1770 V; 3, 1650 V; 4, 1530 V; 5, 1400 V; 6, 1250 V; 7, 800 V.
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Figure 11. The X-ray emission energy dependence upon the discharge voltage (TLD detectors with Be foil shields measurement). 1, discharge voltage is 1750 V; 2,1770 V; 3, 1650 V; 4, 1530 V; 5, 1400 V; 6, 1250 V; 7, 800 V.
• This initiation could be carried out from by a foreign source (e.g., by a flow of inert gas ions).
190 'x-ray photons/beam
J_ « L 0
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f(ms) Figure 12. Typical oscillogram of X-ray bursts within long time interval after turning off the discharge current.
• The production of the excess heat occurred mainly in the near-surface layer of the cathode sample with the thickness up to 1/im (by the results of recording the impurity nuclides). The volume density of the excess heat had a value up to 105 W/cm 3 . (2) Production of the elements isotopes as an impurity to the basic cathode material. • The production of the impurity nuclides occurred in the bulk of the solid-state cathode medium presumably as a result of the nuclear transmutation reactions. • The emission of high-energy heavy ions was not recorded under the experiment. From this fact it was possible to assume, that the nuclear reactions energy was released not as a kinetic energy of the formed impurity nuclides. The impurity nuclides were presumably formed as nuclear isomers (nucleus being in the excited state). From the results of the experiment it followed, that the relaxation of these excited nuclear levels through the gamma-radiation channel was strongly suppressed. (3) Excitation of the energy levels of the solid-state cathode medium. • Formation of the excited energy levels of the crystal lattice was determined by recording the X-rays from solid-state cathode. • The X-rays was observed as the bursts of small time duration (presumably up to 10~ 13 s). Each burst contained up to 109 X-ray quanta with the energy of 1.5-1.8 keV. The bursts were recorded in amounts up to 105 bursts in a second during the discharge and within 100 ms after turning off the current.
191
• Hypothetically, the mechanism of forming this radiation was as follows. When bombarding the cathode surface by the discharge plasma ions in the solid medium, the excited energy levels with the energy of 1.5-2.5 keV and lifetime up to 100 ms were formed. Looking into the concrete physical mechanism of forming these levels calls for additional research. It is possible to assume one of the two possible physical phenomena. (1) Excitation internal L, M electronic shells without ionizing the external electrons. (2) Oscillatory deformation of the electronnuclear system of the solid ions. The core of electronic shells was displaced from a nucleus with forming a dipole (optical polar phonon). • The relaxation of the excited energy levels of the solid medium occurred by emitting the X-rays and, perhaps, fast electrons. • Hypothetically, the relaxation of the excited levels occurred simultaneously from the micro monocrystals making the solid medium. In other words, the totality of the excited ions of the micro monocrystal relaxed simultaneously and gave the X-rays burst. (4) Nuclear transmutation reactions. The excited energy states with the population density of n ex ; t (cm - 3 ) and characteristic temperature of T ex ; t PS 1.5-1.8 keV and more (up to 20,000,000°K and more) were formed in the solid after every passing the pulse of the glow discharge current. These energy states existed for the characteristic time rexjt (up to 100 ms and more). Such medium in which the temperature of the crystalline lattice did not exceed some hundreds °K we call a non-equilibrium medium. • Non-equilibrium nuclear transmutation reactions are possible in such medium. The probability of running these reactions (and accordingly the value of the excess heat) was determined by criterion: nexit x Texit > V^exit X T e x i t J m ; n .
• This is a modified Lawson's criterion used to estimate the positive heat output at inertial thermonuclear synthesis. • The population density was defined by the parameters of the discharge burning and the cathode sample geometry. The characteristic duration of the existence of excited states was defined by the balance between the processes of the energy levels excitation when passing a pulse of the pumping discharge current and processes of these levels relaxation by emitting the X-rays. Thus, to obtain large quantities of excess heat is necessary to create the high population density of vibration-dipole energy states n e x i t and to suppress the X-rays emission (to increase the lifetime of the excited states r e x i t ). (5) The following types of the nuclear transmutation reactions resulting in the formation of the stable nuclides are possible: A+mB^[AB]*,
(2)
[AB]* ^ F * - ^ F + Heat,
(3)
192
[AB]*
C* + D* - • C + D + Heat,
(4)
where A is the Pd or other element nucleus; B is the deuterium or hydrogen; [AB]* is the short-lived intermediate compound nucleus; m = 1, 2 , 3 , . . . , C* and D* are the nuclear isomers of nuclides with masses less than Pd one; C and D are the stable nuclides, F is a nuclide with mass more than Pd. First, a composite compound-nucleus in the excited state was formed. Then one of the two possible modes was realized: • The compound-nucleus could lose its excitation and formed a stable nucleus being heavier than Pd one. • The compound nucleus could be fissionable into two nuclei-fragments with masses less than Pd. In so doing the two nuclei should be in the excited isomer state. (Experiments showed that the nuclear reaction energy was not produced as kinetic energy.) (6) Determining the specific physical mechanism of these reactions will require additional research. One of the possible types of these reactions that form anomalous nuclides may be a long-range (resonant) nuclear reaction. The mechanism of such long-range reactions can be considered by the example of the specific transmutation reaction (Fig. 13). The formation of many 13 C nuclides was recorded in these experiments. A possible reaction can be the following.
E nr = 7820keV . £ 1 3 C = 6860.9 keV 5/2 + £ 1 3 C . = 6864.0 keV
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Nb stable
C stable
Figure 13. Assumed pathways for long-range (resonant) nuclear reactions.
104
Pd
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106
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13
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93
Nb + 7.820MeV.
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193 of 6.864 MeV and excited level width of 6 k e V existed for 1 3 C . T h e excited level with the energy of 0.9498 MeV existed for 9 3 N b . T h e difference between the energy received by nuclide 1 3 C and the energy of one of the excited nucleus state was equal 3.2 keV. At the excitation energy of the crystalline lattice of 1.5 and the width of the excited energy level of 6.0, these conditions gave a high probability of carrying out the long-range (resonant) nuclear reaction (Fig. 13). T h e totality of the experimental results supports the assumption t h a t the energy of excited nuclear levels of the formed nuclides converts into heat. T h e specific physical mechanism of such conversion requires additional research.
6.
Conclusions
T h e obtained results - excess heat u p to 5 W / c m 2 at the efficiency u p to 150% should allow t h e development of a demonstration heater. T h e technology of multielement cathode fuel elements with plasma anodes has been developed. New nuclear engineering is possible, based on non-equilibrium nuclear t r a n s m u t a t i o n reactions in solid-state medium. This type of engineering can be called the "Third way" in nuclear engineering, in comparison with the nuclear engineering on the basis of uranium fission and thermonuclear fusion.
References 1. A.B. Karabut, Excess heat power, nuclear products and X-ray emission in relation to the high current glow discharge experimental parameters, in Proceedings of the ^International Conference on Cold Fusion (China, 19-24 May 2002), p. 151. 2. A.B. Karabut, Patent No. 2240612 RU, Method of heat energy production, Russia.
ACCELERATOR E X P E R I M E N T S A N D THEORETICAL MODELS FOR T H E ELECTRON S C R E E N I N G EFFECT IN METALLIC ENVIRONMENTS
A. H U K E , K. C Z E R S K I , A N D P. H E I D E Institiit
fur Atomare Physik und Fachdidaktik, Technische Universitat Hardenbergstr. 36, 10623 Berlin, Germany
Berlin,
An overview of our experiments and their results concerning the electron screening effects in metallic environments are presented. The measurements of the reactions 2 H(d,p) 3 H and 2 H(d,n) 3 He were performed with an electrostatic accelerator at incident deuteron energies between 5 and 60 keV at different serf-implanted target materials. The resulting screening energy values are about one order of magnitude larger compared to gas target experiments and exceed significantly the theoretical predictions. A thorough investigation of the processes in the targets under ion irradiation shows that there are multiparameter collateral effects, which are crucial for the correct interpretation of the observed enhancements. They mainly originate from target surface contaminations due to residual gases in the vacuum as well as from inhomogeneities in the deuteron density distribution in heterogeneous targets. For the special situation of deuterium in the metallic environment an improved analysis method has been developed beyond the standard procedures. Experimental evidence for the influence of such effects and a mathematical model for their assessment are given and compared with the results of other groups. We also present a numerical model of the electron screening effect in metallic lattices based on an ab initio Hartree—Fock simulation.
1. Introduction A way for the in depth exploration of the cold fusion phenomena is the reduction of the unknown number of free parameters determining the standard electrolysis and gas cell experiments by the ascription to known and more controlled conditions. Such is done here with accelerator experiments at known energies in a better controllable environment. Therewith, we were first able to demonstrate that the screening energies in deuterated metal targets are one order of magnitude larger than in gaseous targets and hence to provide an initial explanation for the adopted nuclear reaction rate enhancement in cold fusion cells by the screening effect. 1-3 Meanwhile our results received confirmation from other groups.4™9 However, there are particularities and pitfalls in this kind of experiments making them special compared to usual nuclear physics procedures. Taking this not into account results in fatal misinterpretations of the obtained raw data. This is discussed in comparison with results from other groups. The accelerator experiments can furthermore provide access to the branching ratio of the channels of the fusion reactions whose alteration could be observed, too. 10 Additionally, to analytic models in 11 a 194
195
numerical simulation is presented for the prereaction impact of the deuterons in the crystal lattice. 2. Accelerator Experiments 2.1. Set up and Data Acquisition
and
Analysis
The experiments have been carried out at an accelerator optimized for low-energy beams. Figure 1 illustrates the principal set up and the data acquisition system. The accelerator consists of a radio frequency ion source, an acceleration line powered by a highly stabilized 60 kV supply and subsequent electric quadrupoles for focusing and a magnetic dipole for beam analyzation. The beam impinges onto a Faraday cup just inside the target chamber where beam adjustment can be done without disturbing the deuteron density in the targets. A horizontal magnetic steerer is then used to deflect the beam onto the target and removes neutral particles and contaminations carried along by the beam. A cylinder box set to a negative potential surrounds the target in order to suppress secondary electrons. The isolated target holder is connected to a current integrator. The targets were disks made from different pure metals becoming self-implanted deuterium targets under the beam irradiation. Four Si-detectors at the laboratory angles of 90°, 110°, 130°, and 150° were used for the detection of all charged particles, p, t, 3 He, of the reactions 2 H(d,p)t and 2 H(d,n) 3 He. The detectors needed to be shielded from the backscattered deuterons in order to prevent a congestion of them and the data acquisition system. Therefore grounded Al-foils of thicknesses from 120 to 150/xg/cm2 were placed in front of the detectors. The thickness is sufficient in order to block deuterons up to 60 keV and let pass all other ejectiles. The detector voltage pulses travel through pre-amplifiers and spectroscopic amplifiers. The signals are digitized by four ADCs in an embedded VME system connected to a computer which automatically integrates the proton lines of the spectra in fixed time intervals8, and records the four differential counting numbers N(8) and the charge q of the integrated beam current at the target in a file which then can be further processed. An example spectrum is shown in Fig. 1; all ejectile lines are clearly identifiable. Due to the anisotropic angular distribution of the ejectiles of the d + d fusion reactions even at the lowest energies, a total counting number N is calculated*3 providing the tabulated function N(q), which is the basic quantity for the further data analysis. Correspondingly, the yield from the experiment is given by
where the number of impacting projectiles is already substituted by their charge, e is the detector efficiency and z the charge state of the projectile. On the other hand the yield is calculated for an infinitely thick target (regarding the projectile a b
Down to 10 s limited by the serial line. See also Ref. 10.
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Figure 1. Experimental set-up.
197
range R) from scattering theory by R
Ytheo(E)=
fna(E(x))dx
(2)
o with the number density of the target nuclei n and the cross-section a. Unlike other chemical compounds the small hydrogen atoms are not trapped in firm chemical bonds with metals. The hydrogen density is not bound to a fixed stoichiometric ratio and can and indeed does change under ion irradiation. Changes in the yield may now originate from both the density and the cross-section and need to be discriminated. The density is here a function of the depth, the projectile energy, the implanted charge, the beam flux and other material dependent and environmental conditions. The tabulated function N(q) provided by our data acquisition system makes it possible to retain the differentiation in (1) and thereby gain information on the charge development of a depth averaged density n(q). So assuming depth homogeneity of the deuteron density in (2) the depth x can be substituted by the projectile energy E with the stopping power differential equation 12 d£ / n(q) - 7 - = - CM + - ^ c dx \ nB
D
\ ry/E, J
(3)
where CM and CD are the stopping power coefficients in the metal and in hydrogen, no the appendant hydrogen density. One arrives with this substitution at a motivation and an interpretative expression for the here defined reduced yield n(q) y ( E ;
q
)
x F{E)
: = ^
f°WdE o y/E
(4)
I'D
< M I
«D
Since both the cross-sections in the metallic environment and the deuteron density are unknown the yield need to be set in relation to a known gas target cross section. We therefore chose the parameterization from Ref. 13 because they have the highest precision. It forms together with the low-energy function (VE) of the stopping power (3) the integral in the denominator on the right-hand side. The gray printed expression is per se a constant. So if the reduced yield is not constant it is based on deviations of the prescribed progression in the cross-section or the functional dependency of the stopping powers or changes in the density. It is a sensitive measure for such deviations but the distinction of the possible reasons is a matter of reasonable interpretation. Figure 2 shows plots of the reduced yield at two different energies. One can see long-term changes in the individual measurements indicated by the straight lines. These are attributed to changes in the density profiles scattered by the counting statistics, of course. In contrast, the large discontinuities of the reduced yield at the switching of the beam energy result from a modification of the cross section. This is taken into account by the enhancement
198
3.0x10'
2.5x10
-Monitor measurement— E, = 25 keV 2.0x10
<\+ N <7(MC)
Figure 2.
Analysis procedure at the example of Zirconium at lOkeV.
factor F(E) in (4). Since the absolute quantity of the deuteron density is unknown for the practical analysis a normalized enhancement factor is defined ,(E) :-
y(E) y(Eo)
F(E) F(E0)
(5)
with the normalization energy EQ which is chosen to be 25keV for the monitor measurements. The gray rectangles indicate the points from which the error for •Fnorm is inferred. Thus, not only errors from the counting statistics but also from long-term changes of the density are included. Results are displayed in Fig. 3. Assuming electron screening as the reason for the enhancement and adopting Ue as a kinetic energy shift parameter in the cross-section14 of the yield one receives
F(E)
VE
o o
(6)
v^
for the screening enhancement factor of thick target yields.0 The corresponding curve in Fig. 3 fits well to the data supporting the screening hypothesis. Our data analysis procedure is thus independent of the absolute value of the deuteron densities inside the targets and the stopping power coefficients with errors from 10 to 20%. The functional dependency of the stopping powers on the energy \[E has been repeatedly confirmed (see Ref. 16 and references therein). The reduced yield can be used to calculate a deuteron density estimate by solving (4) toward n(q) and c
T h e screening energy Ue should only be applied to the Coulomb barrier penetration in a, see Refs. 11 and 15. The correction becomes only important for far lower beam energies.
199
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-
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Figure 3. Exemplary results for the enhancement factor .Fnorm. Screening enhancement for Zr theoretically described by the curve with the single parameter Ue. No enhancement for carbon.
supposing F = 1. Only for this purpose the stopping power coefficients are explicitly required. A corresponding density plot for an initial implantation in Al is shown in Fig. 1. T h e numbers above the gray boxes in Fig. 2 are density estimates for those areas. 2 . 2 . Experimental
Specialties
and
Pitfalls
T h e investigation of nuclear reaction cross-sections on deuterium in metals should be performed at the lowest possible energies. This means t h a t the composition of the topmost atomic layers of the metallic target is of crucial importance because of the quickly decreasing range of the b e a m ions, considerably below 1 /jm. This is exactly unusual for experimental nuclear physics. T h e usual set ups in experimental nuclear physics are constructed in high-vacuum technology. B u t here the contained water vapor from the surfaces of all materials leads under ion impact to a progressing oxidation of the metal because of the stronger electron negativity of oxygen in comparison to hydrogen. Hence hydrogen is contained in metal oxides only in segregation at low and unstable densities. Consequently, the oxidation diminishes and eventually destroys the screening effect with the growth of the metal oxide layer. Carbon hydrides contained in HV systems pose another problem leading to carbon layers on the target as will be discussed below. In such a way generated alterations in the depth profile of the deuteron density distribution in the target is the singular dominating error source for the observed enhancement and the inferred screening energies. Our vacuum system is made of aluminum with elastomer gaskets p u m p e d by t u r b o molecular pumps with auxiliary oil lubricated two stage rotary vane pumps and LN 2 cooled cryogenic t r a p s . A residual gas analyzer (RGA) was used in order to monitor the composition of the residual gas in the vacuum. In accordance to the literature about H V systems the main constituent of the residual gas is water. Water vapor is due to its extraordinarily high-dipole moment very adhesive to solids and
200
is hence chemisorbed to surfaces. Now under the ion irradiation several processes are enabled. Via heating and phonon excitation at the surface the beam provides the activation energy for dissociative chemisorption of the water molecule, i.e., the protons are splitted-off and the remaining oxygen radical forms a chemical bond to the metal atoms. Essentially, the same happens by direct impact excitation of the water molecule by the ions. The hydrogen implantation into the metal causes aside from the usual surface deterioration a in depth destruction of the crystal integrity of the material known as embrittlement which always occurs if the hydrogen loading rate is too high and not proceeding in thermal equilibrium. 10 ' 17 Thus, the surface is fractalized and the oxidation can progress into the bulk of the metal quickly creating a thick metal oxide layer. Figure 4 contains as an example for it a picture of the surface of an Al target, which turned into a sponge like structure. The rate of the oxidation process depends on the concrete form of the mutual interaction potential between the water molecule and the surface atoms, establishing a material dependency. The energy supply of the beam enables these processes even for the noble metals. Albeit generally spoken, more reactive metals apt more to oxidation and embrittlement while for the latter the structural difference between the metal and the metal hydride is more important. Aside from the overall beam heating the energy of the projectiles is also important because lower energy projectiles are more effective at the surface.18 The partial pressure of water in HV is so high that there are ample supplies for the surface reactions. The hit rate of water molecules with a sticking coefficient of almost one is in comparable orders of magnitude as usual beam currents of 10-100/LtA. This implies a dependency on the ion flux, too. There are two counteracting processes: Sputtering and thermal or ion stimulated desorption. The sputtering yield of the lightweight deuterons is far too low in order to keep the surface clean with the resulting sputtering rate. One would expect that an increased temperature of the surface would increase the desorption rate of the water molecules. If the activation energy barrier for dissociative chemisorption of water is positive an increased temperature yet proliferates the oxidation. d Similar is valid for ion stimulated desorption/chemisorption. Such again depends on the interaction potential but usually oxidation prevails. Unless UHV systems equipped for entire baking are used the oxidation cannot be avoided. A deuteron irradiation of only 1 C is enough to produce a considerable metal oxide layer (Fig. 1 in Ref. 20). There is, however, a process that is nonetheless able to prevent oxidation: large carbon hydride molecules, e.g., back streaming from the forepumps, can be physisorbed at the surface, cracked up and the carbon atoms can react with the oxygen radicals to carbon monoxide keeping in that way"the surface clean. Differently from water, carbon hydrides are physisorbed to surfaces. The strength of this weaker bond increases with growing molecular mass. The ratio of absorption and desorption under the ion irradiation has similar dependencies. An evidence for this chemical
d
See, e.g., Ref. 19 or any surface physics textbook.
201
surface reaction is the detection of a considerable CO fraction by the RGA, which was below the detection threshold without beam irradiation. These processes were thoroughly explored by the regulated infusion of decane with monitoring feedback. The surface can only be kept clean if the fraction of water and carbon hydrides in the residual gas is in an equilibrium, which is of course also dependent on pre-mentioned parameters. If the fraction of carbon hydrides is too low the surface will oxidize. If it is too high a carbon layer will build up. Both are essentially irreversible. Figure 5 shows some of the results of these experiments for Ta demonstrating the high spread in the inferred screening energies depending on the surface composition, which were verified by EDX. e In order to limit the layer formation the totally implanted charge was reduced. For the analysis a more sophisticated expression for the yield in (4) and (5) was used based on a model of the target with three stacked layers. 20 The top layer consisting of either metal oxide or carbon, a deuterized zone of the metal and the bulk of the metal containing essentially no hydrogen. Each can have different thicknesses and relative deuterium contents. The results for Ue in Fig. 5 were obtained with only the additional parameter £M for the thickness of the deuterated zone in the metal in energy equivalent units of the stopping. The differences for Ta-A and Ta-E are already considerable though the thicknesses of the surface layers were small and just started forming. Figure 4 shows the beginning of the formation of a carbon layer starting from islands, which will eventually cover the whole surface in concordance with experiences from thin film technology.18 Ta-C has already a relatively thick carbon layer, which strongly reduced the screening energy. Just as the metal oxide layer does in Ta-D. Those layers were just thick enough in order to be included in the model and infer their thickness. The thickness of the metal oxide layer is 0.09 VkeV, which conforms to about 7nm. The corresponding screening energy would be 433 eV. Fifteen nanometers are enough to let the screening enhancement completely vanish. Much thinner surface layers already reduce the inferred screening energy considerably. So the real value for the screening energy of Ta is possibly around 400 eV. Carbon can achieve high densities but it does not show the electron screening effect as Fig. 3 proves. Thin deuterated carbon layers can, however, simulate a screening enhancement as inhomogeneous density profiles can do. 20 As already said, the metal oxide contains only few deuteriums in segregation. Those low densities are unstable and change under different conditions. At the example of a Na target with a very thick metal oxide layer the development of the density is illustrated in Fig. 6. The density estimates are calculated from the reduced yield as previously described. Before the monitor measurement at 25 keV a measurement at a low energy had been taken. The density quickly decreased then at 25keV. Thereafter, a measurement at 12keV were started. The density very quickly increased reaching a higher level than at 25keV. But the discontinuity at the beginning was in the wrong direction. The density for the sequencing monitor measurement started once again at a high density, which quickly decreased. The
e
Electron dispersive X-ray microanalysis.
202
discontinuity at the beginning was once again in the wrong direction. So there is definitely no screening. The quick shifts in the densities after the change of the implantation energy going to a "saturation" level originate from a shift of the deuteron distribution depth profile in the metal oxide linked to the different ranges of the ions. With our method of recording a yield function Y(q) over the implanted charge we can recognize those shifts and reject them. If, however, only the total yields of the long-time measurements were regarded as in the standard method their comparison would erroneously lead to a screening interpretation. The same problem arises when working with low-implantation densities below the stoichiometric ratio even when the metal oxide layer is negligible. Except for insufficient implantation the density remains low if the thermal energy of the deuterons is higher than their chemical binding energy to the metal so that they can float. This applies mainly to transition metals with low ability to bind hydrogen (groups 6A-8A and IB) or if the metals are heated. An example for the consequences of heating is shown in Fig. 6 for a Ta-foil of 7/xm, which was heated by the beam power. One observes the same behavior and no real screening enhancement. The density returns to an equal saturation level if the surrounding conditions are the same, i.e., same beam energy, current, target heat flow, etc. The most effective heat transportation mechanism in solids is the free electron gas. Cooling the target holder has little effect since the thermal resistance at the connection is very high. Besides from heating the density profile of the deuterons in target materials with low-binding ability for deuterons (metal oxides, metals with low affinity to hydrogen, and metals at high temperatures) is also changed by direct projectile hits and close phonon generation at the target deuterons depending on the beam energy. Furthermore, the metal oxide as a thermal insulator will be considerably heated by the beam power. It is therefore preferable to use thick target disks at moderate temperatures with high densities. On the other side, cooling a target to very deep temperatures would transform it into a cryogenic trap accumulating water in thick layers on its surface prior to irradiation promoting the oxidation. The detailed investigation is covered in Ref. 3.
Figure 4. Scanning electron microscopic pictures of target surfaces. Left: Symptoms of embrittlement for Al. Right: Beginning layer formation for Ta in island growth mode.
203
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Fi gure 5. Effects of different surface compositions on the inferred screening energy for Ta. Ta-A has a small C-excess, Ta-E has slight C-traces, Ta-C a thick C-layer, Ta-D a thick MO^-layer.
2.3.
Comparison
Paying attention to all the above discussed experimental problems we can state that our results represent lower limits to the real screening energy values: 190 ± 15 eV for Al, 297 ± 8eV for Zr, 313 ± 2eV for Pd, and 322 ± 15 eV for Ta. Due to our monitoring method, we estimate the upper limit of Ue to be probably not larger than additional 100 eV. The value for Sr ranges between 350 and 800 eV since the measurement was impaired by layer formation, even more for Li where only an upper bound of 150 eV could be determined and no screening for Na (Fig. 6). Two tests with Y and Er led to thick metal oxide layers, too. In Fig. 7, an overview of screening results from other experiments is plotted. Historically the two elements Pd and Ti were of special interest. So one of the first accelerator experiments was done on Ti. 2 1 The authors made no effort to determine the deuteron density but used a literature value and obtained no enhancement. All further measurements on Ti resulted in very low-screening values. The higher the deuteron density, the lower the screening value. Ti is chemically very similar to Zr, both belong to the group 4A. From our experience Zr oxidizes readily. So a relatively thick metal oxide layer explains the results and the discrepancy to the value in Ref. 22. It was obtained with a glow discharge of ~0.5A deuteron current. Despite of the low-sputtering yield of the deuterons the high current permits a sputtering rate, which is so high that it can impair the oxidation enough. A deliberately produced 30 nm thick PdO layer on a Pd target in Ref. 5 yielded an especially high-screening energy with a low-density obtained from the total yield only. Such a thick PdO layer would show quick shifts in the density profiles with higher averaged densities at lower projectile energies like in the Na example in Fig. 6 when changing the projectile energy and
204 1.8x10 21 1.6x10 21 jl
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Figure 6. Development of low-deuteron densities. Left: Na target with a thick metal oxide layer. Right: A beam heated thin Ta foil.
using the differential analysis method. So this screening is simulated by the density alteration in the total yield. The same applies to the extraordinary high-screening value for Pd of Ref. 9 at a low density. The screening energies for Pd of Refs. 4 and 5 agree within their errors though obtained at very different densities and both at deep temperatures. The value in Ref. 5 is in concordance with our result. For Au there is a discrepancy between Refs. 4 and 5 in the densities at low-screening energy values and deep temperatures. We made a test with a thin Au foil and observed behaviour like for the Ta foil in Fig. 6 without the screening enhancement discontinuities. While the targets SrZr
Pd
e e m A
[91 [8] [7] [22] Ti [21] Ti [5] [5] 30 nm PdO [4] This work
Figure 7. Overview of screening experiment results. Bottom: Screening energies Ue. Top: Deuterium to metal ratio x. The values for x of Ref. 5 were estimated from Fig. 2 therein. The values of Ref. 9 are the database; data points from Refs. 8 and 7 are included if they differ, only.
205
as described in Ref. 5 are thick enough ~ l m m to guarantee an effective heat transport in the bulk of the material by the electron gas, the heterogeneous target Au/Pd/PdO with a total thickness of only 60 /im (thereof 0.1 /jm Au) is too thin therefore leading to a considerable temperature increase in the beam stopping volume which is to this extend not detectable by an outside mounted thermocouple. So the observed high-screening energy of 602 ± 23 eV can be explained by the shifts in the density profile due to elevated temperatures and the heterogeneity of the target and accordingly the density. In order to explain the relation between the screening energy and the density the concept of deuteron "fluidity" was introduced in Ref. 5 where fluid deuterons and conduction electrons are to behave like hot plasma. But in palladium oxide there are no conduction electrons. In view of the stated density dynamics this explanation is decrepit. The explanation by density dynamics is also sustained by the significantly larger standard deviations of the repeated density measurements at lOkeV for targets with low densities in Fig. 2 in Ref. 5. Indeed the saturation density in our experiments returns to the same level for the same conditions but with higher deviations. The largest data set of screening energies is provided by Refs. 7-9. They only observed the total yield of the measurement, too. The density is determined by a global fit to the previously extracted relative cross-sections by using the imprecise stopping power coefficients to a known cross-section at 30keV and consequently obtains a density estimate, which is valid at 30keV only.6 The intention is to find a connection between the observed screening energy and some electronic properties of the elements. The authors propose the Hall coefficient to be this quantity stating that the free charge carriers, i.e., electrons and holes likewise, form a Debye sphere around the deuterons and thus generate the screening potential. The classical Debye screening is, however, not applicable for low temperatures (electron energies below the Fermi energy) and dense plasmas (solid states) where the quantum mechanical effects dominate and the screening effect depends only on the charged particle density and not on the temperature. 23 Additionally the motion of the bound electrons simulating the hole is not free but governed by quantummechanical tunneling between neighbor atoms. The fact that the screening energy is vanishing for high-deuteron densities is explained by the assertion that these metal hydrides are insulators. This is not right for the majority of the metal hydrides, which are metallically or covalently bound and retain their metallic properties. The Baranowsky-curve of the electric resistance of metal hydrides shows that the resistance at the chemical stoichiometric ratio is even lower than for somewhat lower densities and comparable to the metal. Using a 3 He beam on a deuterated 3 4 7 8 Pt target via the reaction d( He,p) He a screening energy was inferred about twice as high as for the d beam which was regarded as a confirmation of the Z dependency of the Debye hypothesis. 8 In Ref. 9, however, the screening energies for 3 He and d beams at Pt became equal. The homogeneity of the depth distribution of the deuterons in the targets was reconfirmed by a subsequent off-line
206
ERDA f with a 4MV tandem accelerator. 7 Pointed to the problem of oxidation RBS g analysis was performed on the targets with the result that there were "no detectable surface contaminations" with the exception of Al where there was an AI2O3 layer with a thickness of about 150 monolayers. Then a Kr ion sputtering treatment at 15 or 35keV was applied prior to the implantation measurements in order to remove natural metal oxide layers which is the main difference from Refs. 7 to 9. This procedure does not take into account that the major cause of the oxidation is contributed by the water in HV systems under deuteron irradiation. For both ERDA and RBS it is valid that light projectile ions with a kinetic energy of some MeV cannot provide a wide energy spectrum of the ejectiles, which would be necessary in order to resolve single atomic layers. Therefore, a HIERDA h with incident energies of the heavy ions in the 0.1 GeV order of magnitude would be required with sophisticated magnetic analyzing systems. This is additionally complicated by the circumstance that these methods deliver expressive results only if heterogeneous samples are made up of well-defined layers. This is not fulfilled for the implantation targets with indistinct chemical composition and surfaces fractalized by embrittlement and beam deterioration. So the applied methods are not able to detect metal oxides with a thickness of a few 10 s monolayers (some nanometers) which is already sufficient to obliterate the screening enhancement while they are not thick enough to affect the density determination at 30 keV significantly. While the high-sputter yield of the Kr ions may allow for a surface cleaning the large Kr atoms thoroughly destroy the crystal structure of the target and get trapped in the material fractalizing the surface and thus possibly even promoting the oxidation process under subsequent deuteron irradiation since the necessary annealing is omitted. The deviations in the screening energies between Refs. 7 and 9 are in both directions, anyhow giving an indication for the magnitude of the true error in the determination of the screening energies in this way similar to our dedicated experiments on Ta (Fig. 5). Like in the data of Refs. 4 and 5 there is a clear connection between the density and the screening energy. High densities are linked to lowscreening energies because of moderately thick metal oxide layers. Examples are the elements of the groups 3A (21SC, 39Y, and the lanthanoides Z = 57-71) and 4A (Ti, Zr, and 72IK) emphasizing the chemical kinship with regard to the described surface reactions. Low densities generate high-screening energy findings due to shifts in the density profile either in thick metal oxide layers or materials with low-hydrogen binding ability. Such can be recognized at the transition metals (groups 6A-8A: Z ~ 24-28, 42-46, and 74-78) for example. In contradistinction thereto our high-screening energy results were f
Elastic recoil detection analysis. Rutherford back scattering. h Heavy ion elastic recoil detection analysis.
g
207
obtained at high densities close to the chemical stoichiometric ratios. Using the data of Ref. 9 (Table 1) a Spearman rank correlation calculation can be done. For the test of a correlation between Ue and the deuterium ratio \ one obtains rs = —0.800 and P — 5.1 x l O - 1 4 , which means a rather high correlation with a very high significance. On the other side, the result for a correlation test between Ue and the effective charge carrier concentration neg calculated from the Hall coefficient is r s = 0.489 and P = 0.013, which is a medial correlation with a weak significance. This is not enough in order to rule out the testing null hypothesis of no correlation thus deprecating the Debye hypothesis, too.
< > ? -30
Li: -0.0523
H: 0.0345
r(A) Figure 8. Left: Screening force and cumulatively integrated potential during the prereaction impact. Right: Electron probability density on a plane with 4 Li atoms at the sites and the target deuteron at the center.
3. Numerical Simulation In Refs. 11 and 15, we presented an analytical model based on the dielectric function theory for the description of the screening effect and extrapolation to room temperatures. It remains, however, below the measured screening energies by a factor of 2 though better than other approaches cited therein. Therefore, a first effort was undertaken to simulate the prereaction impact with an ab initio quantum mechanical Hartree-Fock calculation which is able to consider the actual crystal structure while the analytical model only operates on averaged material properties. The concrete form of the electron density distribution around the nucleus indeed influences the screening energy to a great extend as was shown in Ref. 24 on a D2 molecule with a time dependent Hartree-Fock calculation. Since only workstation class computational power was available several too far-reaching simplifications needed to be implemented. The motion of the projectile needed to be abandoned for an adiabatic limit. Only a very small LiD crystal consisting of six Li atoms on a limited set of basis functions were feasible for the calculation, which lasted
208
1.6 years netto. The calculations were done with the quantum chemical program GAUSSIAN. 2 5 An intersection of the electron probability densities is plotted in Fig. 8. It is actually the difference between the molecular density and that of the single atoms thus exposing electron transfers at the chemical bond. One can clearly see an increase of the electron density at the deuterium on the expense of the Li atoms in concordance with the ionic nature of this bond. This is even enlarged during the approach of the colliding deuterons. The electronic force between the two deuterons is plotted in Fig. 8. Its integration yields the screening energy, which is with 43.4 eV twice as high as from the simple model 14 but still far below the measured values. Using enhanced basis sets leads to an increase of the calculated screening energy. A complete treatise can be found in Ref. 3.
4. Conclusion We developed a differential data analysis method, which gains the maximum information from the raw data. The method is independent of the imprecise stopping power coefficients and the actual absolute value of the deuteron number density in the targets. It allows for the recognition and rejection of measurements with unwanted shifts in the density depth distribution profile thus preventing the erroneous extraction of an artificial screening enhancement in contrast to the standard analysis based on the total yield measurement used by Refs. 4, 5, 7-9. Those undesirable density profile changes occur in targets with low-hydrogen binding ability, like many of the transition metals, at elevated temperatures and heterogeneous targets with metal oxide or carbon layers or different (relatively) thin metal layers. The fatal alteration of the inferred screening energies due to layer formation under beam irradiation depends on many parameters and is inevitable in high-vacuum systems that are used by all groups. The deviation from the "real" value of the screening energy is probably around 100 eV. So any conclusion based on the observed material dependence of the screening energies is pre-mature. On the other hand, the theoretical calculations performed within an improved dielectric function theory 11 ' 15 predict only a weak material dependence of Ue in contradiction to the experimental results of Refs. 7-9. Furthermore, an error of 100 eV implies an error in the reaction rate of many orders of magnitude when extrapolating to room temperature, i.e., the cold fusion condition. 11 ' 15 Consequently, aside from the sustained fact that there is a great screening enhancement at this time no further assertion can be made. For a precise determination of the screening energies ultra high-vacuum systems with pressures well below 1 0 _ 1 0 h P a , where only hydrogen and noble gases are in the residual gas, and equipped with in situ target diagnosis techniques are mandatory. The presented numerical simulation bases on a too simplified model due to limited computational power hence failing to reproduce the observed screening energies, while already exposing shifts in the electron distribution. An extended model capable of describing the situation realistically would require massive parallel
209
supercomputers though very instructive insights into the electron dynamics for the understanding of the mechanism can be expected.
References 1. K. Czerski, A. Huke, P. Heide, M. Hoeft, and G. Ruprecht, Nuclei in the Cosmos V, in N. Prantzos and S. Harissopulos (Eds.), Proceedings of the International Symposium on Nuclear Astrophysics, Volos, Greece, July 6-11, 1998, p. 152 (Editions Frontieres). 2. K. Czerski, A. Huke, A. Biller, P. Heide, M. Hoeft, and G. Ruprecht, Europhys. Lett. 54 (4), 449-455 (2001). 3. A. Huke, Die Deuteronen-Fusionsreaktionen in Metallen, PhD Thesis, Technische Universitat Berlin, 2002. http://edocs.tu-berlin.de/diss/2002/huke_armin.htm. 4. H. Yuki, J. Kasagi, A. G. Lipson, T. Ohtsuki, T. Baba, T. Noda, B. F. Lyakhov, and N. Asami, JETP 68 (11), 823 (1998). 5. J. Kasagi, H. Yuki, T. Baba, T. Noda, T. Ohtsuki, and A. G. Lipson, J. Phys. Soc. Jpn. 71, 2281 (2002). 6. F. Raiola, et al, Eur. Phys. J. A 13, 377 (2002). 7. F. Raiola, et al, Phys. Lett. B 547, 193 (2002). 8. C. Bonomo, et al, Nucl. Phys. A 719, 37c (2003). 9. F. Raiola, et al, Eur. Phys. J. A 19, 283 (2004). 10. A. Huke, K. Czerski, T. Dorsch, and P. Heide, Evidence for a target-material dependence of the neutron-proton branching ratio in d + d reactions for deuteron energies below 20keV, in Proceedings of the International Conference on Condensed Matter Nuclear Science, ICCF-11, Marseille, France, November 2004. 11. K. Czerski, A. Huke, and P. Heide, Electron screening constraints for the cold fusion, in Proceedings of the International Conference on Condensed Matter Nuclear Science, ICCF-11, Marseille, France, November 2004. 12. H. Anderson and J. F. Ziegler, The Stopping and Ranges of Ions in Matter, Vol. 3 (Pergamon Press, New York, 1977). 13. R. E. Brown and N. Jarmie, Phys. Rev. C41 (4), 1391 (1990). 14. H. J. Assenbaum, K. Langanke, and C. Rolfs, Z. Phys.A (327), 461-468 (1987). 15. K. Czerski, A. Huke, P. Heide, and G. Ruprecht, Europhys. Lett 68 (3), 363-369 (2004). 16. S. P. M0ller, A. Csete, T. Ichioka, H. Knudsen, U. I. Uggerhoj, and H. H. Andersen, Phys. Rev. Lett. 93, 042502 (2004). 17. W. M. Mueller, J. P. Blackledge, and G. G. Libowitz (Eds.), Metal Hydrides (Academic Press, New York, London, 1968). 18. W. Ensinger, Nucl. Instrum. Methods B (127/128), 796 (1997). 19. A. Zangwill, Physics at surfaces (Cambridge University Press, Cambridge, 1988). 20. A. Huke, K. Czerski, and P. Heide, Nucl. Phys. A 719, 279c (2003). 21. J. Roth, R. Behrisch, W. M0ller, and W. Ottenberger, Nuclear Fusion 30 (3), 441 (1990). 22. A. G. Lipson, A. S. Roussetski, A. B. Karabut, and G. H. Miley, Proceedings of the International Conference on Cold Fusion, Cambridge, MA, USA, 2003, ICCF-10. 23. E. E. Salpeter, Aust. J. Phys. 1 (2), 12 (1954). 24. T. D. Shoppa, M. Jeng, S. E. Koonin, K. Langanke, and R. Seki, Nucl. Phys.A (605), 387 (1996). 25. M. J. Frisch, G. W. Trucks, et al, Gaussian 94, revision e.l. Technical Report (Gaussian Inc., Pittsburgh, 1995).
E V I D E N C E FOR A TARGET-MATERIAL D E P E N D E N C E OF T H E N E U T R O N - P R O T O N B R A N C H I N G RATIO IN d + d R E A C T I O N S FOR D E U T E R O N ENERGIES BELOW 20 keV
A. H U K E , K. C Z E R S K I , T . D O R S C H , A N D P. H E I D E Institut
fur Atomare Physik und Fachdidaktik, Technische Universitdt Hardenbergstr. 36, D-10623 Berlin, Germany
Berlin,
Angular distributions and the neutron—proton branching ratio of the mirror reactions 2 H(d,p) 3 H and 2 H(d,n) 3 He have been investigated using different deuterized metallic targets at projectile energies ranging from 5 to 60keV. Whereas the experimental results obtained for Al, Zr, Pd, and Ta targets do not differ from those known from gas-target experiments, an enhancement of the angular anisotropy in the neutron channel and a quenching of the neutron—proton branching ratio have been observed for Li and Sr targets at deuteron energies below 20keV. Both effects can be explained assuming an induced adiabatic polarization of the reacting deuterons in the crystal lattice.
1. Introduction As known for a long time from accelerator experiments the d + d fusion reactions have three possible outgoing channels, 2 H(d,p) 3 H, 2 H(d,n) 3 He, and 2 H(d,7) 4 He. Two of them mediated by the strong interaction generate high-energetic particles with a branching ratio of about 1 below 50keV while the third one is an electromagnetic transition suppressed by >10 7 . Close to the reaction threshold there are two 1~ resonances in the compound nucleus 4 He. They can be excited by deuterons with an orbital angular momentum of 1. This is the reason for the unusually strong anisotropy of the angular distribution of the ejectiles even at the lowest energies. In our previous works 1 ' 2 we have found a strongly enhanced electron screening effect for the d + d reactions in metallic environments. Angular distributions and relative intensities of the proton and neutron channels investigated for d + d reactions taking place in Al, Zr, Pd, and Ta targets were, however, in agreement with the results of gas-target experiments. Here, we present new results obtained for Sr, Li, and Na targets giving a first evidence for an alteration of the neutronproton branching ratio and the angular distributions. Initial results were presented in Ref. 3 and hitherto completely published in Ref. 4 but now a first theoretical explanation for this surprising observation can be presented. 5 210
211
2. Experimental Results The experiment has been carried out at a cascade accelerator optimized for low-energy beams. The targets were pure metal disks becoming self-implanted deuterium targets under the deuteron irradiation. Four Si-detectors at the laboratory angles of 90°, 110°, 130°, and 150° were used for the detection of all charged particles, p, t, 3 He, of the reactions 2 H(d,p)t and 2 H(d,n) 3 He. 6 ' 2 The detectors needed to be shielded from the backscattered deuterons in order to prevent a congestion of them and the data acquisition system. Therefore, grounded Al-foils of thicknesses from 120 to 150 /xg/cm2 were placed in front of the detectors insulated from them. The thickness is sufficient in order to stop backscattered deuterons up to 60 keV. The low-energy part of some representative spectra from the 90°-detector is depicted in Fig. 1 magnifying the two lines of the recoil nuclei 3 He and t. The spectra are normalized to an integral value of one in order to make them commensurable. The energies above the peaks are the kinetic energies of the ejectiles in the laboratory system. They drop for increasing projectile energies, which is especially significant for the back angle positions. The gray filled spectra are from Ta targets while the black and gray step lines are for Sr and Li and Na, respectively. The two plots compare the form of the spectral lines at a low-projectile energy of 8 keV to a high energy of 30 keV. At 8 keV, the t-line of Ta is well separated while the 3He-line sits on an exponential background. The background is subtracted by fitting an exponential function to the lowest energy part and then by extrapolating it to the high energies. The spectral lines for Sr are already broader with an enhanced lowenergy tail leading to an overlap of both lines. This effect becomes even stronger for Li and Na. At 30 keV the Ta lines are broader but the tails of the Sr, Li, and Na lines are much more distinctive. The overlap of the two lines is even higher. For Li and Na the 3He-line is hardly more than an edge. The p-line at 3 MeV has also a long low-energy tail but it vanishes before the t-line. The appearance and the properties of these tails can be explained by a phenomenon known from the physical chemistry of the metal hydrides, called embrittlement7 which means that the crystal structure of the metal is bursted by the recrystallization process that accompanies the formation of the metal hydride crystal. Reactive metals change their crystal structure while forming the metal hydride. If the hydration proceeds not in a thermal equilibrium and relatively slow, the material cannot compensate the tension of the recrystallization process and bursts. Since deuteron implantation is far off the thermal equilibrium, embrittlement is a hardly avoidable concomitant phenomenon for reactive metals. How embrittlement effectuates the tails is elucidated with the sketch in Fig. 1. Assuming, the projectile travels through the target along a path covering many empty regions, the energy loss becomes smaller and consequently the nuclear reactions occur deeper below the target surface than in the case of compact materials. Therefore, the ejectiles that in turn can travel through more compact target regions loose more energy additionally contributing to the low-energy tail of the particle spectrum. The increase of the tail with the projectile energy arises from the simultaneous increase in the overall range of the projectiles. The material
212
dependence can be explained, too. Ta is almost a noble metal with low reactivity but nonetheless able to chemically bind hydrogen to high amounts. It just stretches its lattice dimensions but does not recrystallize like the highly reactive metals of the groups I and II of the periodic system. So there is no embrittlement and hardly a tail visible. On the other hand the effects of embrittlement and the tail increase from Sr over Li to Na with decreasing electron negativity. The symptoms were even visible, e.g., dust particles crumbled from a strontium target, the thickness of a natrium target grew considerably. The low-energy tail formation complicates the integration of the spectral lines till unfeasibility in the case of Na. The 3He-line sits on the tail of the t-line. All efforts to describe and extrapolate the tail of the t-line to the lower energies analytically failed, since the form of the lines is dependent on the nucleus species, ejectile and projectile energy. Uncertainties and imponderabilities in the integral of the spectral lines are taken into account in the errors additionally to the counting statistic. Consequently they are the dominating error source. If in doubt, events were attributed to the 3He-line only, gaining a conservative estimate at least. Fortunately, the tails are small at the low-projectile energies were the asymmetry in the branching ratios becomes observable. Neglecting I > 2 contributions the angular distribution can be described as follows: ^($)
= A0 + A2cos2$.
(1)
U.LU
Because of the identical bosons in the entrance channel the angular distribution is symmetric around 90°. $ and u> are the polar angle and the solid angle in the CM system, respectively. Since the experimentally determined thick target yield is dominated by the high-energy contributions below the Coulomb barrier a similar expression is valid for the differential counting number: — (tf) =a0 + a2 cos2 •&. (2) dw The expansion coefficients a$ and a2 now include a constant factor containing a product of detector and target properties and the number of incident projectiles. A measurement at 20 keV for Sr exemplary shows the results for the differential counting number and the corresponding fitting function in Fig. 2. The fit is computed with a non-iterative generalized linear fitting algorithm employing singular value decomposition thus allowing for more accurate values and better error handling. The data points obtained for the protons are included. As can be seen protons and tritons follow the same angular distribution. One observes a significantly stronger angular anisotropy for the neutron channel. The angular anisotropy is quantitatively given by the ratio (a2/ao = A2/AQ). Again with the previous argumentation the two fitting coefficients can be used to calculate the branching ratio of the two mirror reactions with ^d(d,n)3He = y( 3 He) = JV(3He) = a 0 ( 3 He) + |a 2 ( 3 He) crd(d,p)t Y(p) N(p) a 0 (p) + |a2(p) where in the last step N is simply the integral over the unit sphere of the differential counting number (2). When calculating with the fitting coefficients one
213
must consider that they are not independent variables. Then the Gaussian error propagation formula needs to be completed by a term containing the off-diagonal element of the covariance matrix from the fit. The results are plotted in Fig. 3. The branching ratios and angular distributions determined for Ta, Al, Zr, and Pd agree with the results of the gas target experiment. 8 Not so for Sr and Li. While for p there are no pecularities, for 3 He the anisotropy raises at lower energies (see also Fig. 4). Simultaneously, the n branch is suppressed. The results for protons and tritons are concordant. The low quality of the Li points results from the ambiguity of the integration of the spectral lines with large low-energy tails. For the same reason, the spectra obtained for Na could not be analyzed quantitatively, though the spectra indicate a strong suppression of the neutron-proton ratio at low energies, too. For details refer to Ref. 4.
!
0
I 1
L,,
,,l
50
S
1
I
I
1
>
.<,, J A,„.,J..,,
100
150
.
•
L
!
200
Channel (a. U.) Figure 1. Normalized spectra from the 90°-detector. The low-energy tail complicates the discrimination and is caused by embrittlement, which becomes stronger for more reactive metals. The sketch shows how different paths through the target explain the tails.
214 T
i
|
i i
j
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i
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1 J
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|
r—i
i
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i
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i
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R
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6
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•o 2.0x106 1.9x106 1.8x106 1.7x106 0
30
60
90
L A
120
I
150
180
•&
Figure 2. Angular distribution of the 2 H(d,p) 3 H and deuteron energy E& = 20 keV for Sr.
2
H(d,n) 3 He reactions obtained at the
3. Theoretical Considerations and Discussion The problems of integrating the overlapping spectral lines cannot be circumvented by the use of detector telescopes for particle identification. The A£?-detector of the usual semiconductor detector telescopes would already absorb the recoil nuclei. The embrittlement cannot be responsible for the observed anomalous asymmetry in the branching ratios because the effects of embrittlement like tail formation rise with the projectile energy in contradiction to the deviations in the branching ratio. This is also valid for conceivable weird surface textures. Multiple scattering of the ejectiles in the thick target could possibly redirect leaving particles depending on the nucleus species and thereby change the detection rate. Such has been tested with a Monte Carlo simulation having given a negative result. 9 Furthermore, anisotropic symmetries in crystal structures cause effects like optical activity and piezo and pyro
215 2.0
rjTjTTT i p i l i j ( r r r y r i i > [ i i I i J i i H j i i n j i n
1.8
o(r.t) = a 0 + a.j cos 2 *
a Ta - P A Ta -6He • Sr - P J A Sr - H e • Li- P J * Li- He
1.6 1.4 1.2 CO
q-rrrrj
1.0 0.8
*
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:
*
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.-H+UH11 n n |ni ill i ill int 1 mi hi i ih m l i n i l n '
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"§& O Ta • Sr • Li
0.7
t. !.'...!. i . i l J
0.6
10
15
20
25
30
LLUDJ.I
JJJJJXI
35
45
40
50
55
lab (keV) a
E
Figure 3. The upper part displays the anisotropy from the detection of the p and 3 He ejectiles. The lower part shows the branching ratio for the two mirror reactions.
electricity. So this could be a conceivable reason for the experimental observations. Enantiomorphy is a necessary condition for such effects. However, the point groups belonging to LiD, SrD 2 , and NaD do not allow for this. From the theoretical point of view the cross section for the mirror reactions 2 H(d,p) 3 H and 2 H(d,n) 3 He at deuteron energies below 100 keV can be described with 16 collision matrix elements, corresponding to S-, P-, and D-waves in the entrance channel. The matrix elements for incoming D-waves cannot be omitted as frequently asserted since they are mandatory to describe the angular anisotropy down to the lowest energies. The values of the matrix elements are relatively well known and were obtained by fitting experimental cross sections, vector and tensor analyzing powers measured in gas target experiments. 10 ' 11 The differential cross section for both reactions can be presented by a coherent superposition of all 16 matrix elements 5 (dashed line in Fig. 4) and agrees with our results obtained for Al, Zr, Pd, and Ta. In the case of Sr (also for Li) a polarization of the deuterons
216 0.8 0.7 0.6 0.5 0.4 0.3 0.2
A Neutrons: filled Sr, open Ta • Protons: filled Sr, open Ta , . , Normal curve: a(S=0,1,2)=1 •»™ Polarization
0.1 0
LiLi
Lib_A±i_h
1.05 1.00 1.95 0.90
• Li • Filled Sr, open Ta . . . Normal curve: o(S=0,1,2)=1 • Polarization
0.85 0.80
i-4~tl~U~UU l I E U , . l ~ t i i . i I, S }
0.75 5
10
15
20
25
30
35
40
45
50
ix.Li^Ij^~i~
55
60
EfVv) d Figure 4. The dashed line represent the normal curve. The solid lines result from a deuteron polarization corresponding to a suppression of the S = 0 channel at lower energies.
in the crystal lattice had to be assumed. A suppression of the channel spin 5 = 0 (spins of the deuterons are anti-parallel) and allowing the other channels with spins S = 1,2 to be undisturbed permits to describe simultaneously the enhancement of the angular anisotropie of the 2 H(d,n) 3 He reaction and the decrease of the n/p branching ratio at very low energies down to 0.83. The results of corresponding calculations are presented in Fig. 4 as full lines. Here we have assumed that the deuteron polarization takes place gradually below the Fermi energy (for Sr about 25keV), reaching its maximum value already below lOkeV. A strong quenching of the neutron channel might also be explained by different screening energies for relative angular momentum L = 0,1. Supposing that the screening energy for the L = 1 contribution is much smaller than for L = 0 one gets a decreasing n/p branching ratio at low energies reaching a minimum of only 0.93. In this case, however, the anisotropy of the angular distribution for both channels will be reduced till isotropy, in contradiction to the experimental results. For details refer to Ref. 5.
217 4.
Conclusion
We presented a first experimental evidence for a alteration of the branching ratios in the d + d fusion reactions obtained in an accelerator experiment which can be theoretically explained by polarization of the reacting deuterons in the crystal lattice while other rather trivial causes could be excluded. T h e reason for the deuteron polarization is, however, still unknown. A distinctiveness of the (earth) alkaline metals is the formation of an ionic bond to hydrogen, which might be a starting point for a possible explanation based on the spin-spin interaction. In view of the experimental indications for a strong n e u t r o n - p r o t o n asymmetrie in the d + d reactions at room temperature, our experiment supports an understanding of the cold fusion phenomena although further efforts are necessary. An experiment with more sophisticated particle detection techniques is in progress in order to refine the data.
References 1. K. Czerski, A. Huke, P. Heide, M. Hoeft, and G. Ruprecht, Nuclei in the Cosmos V, in N. Prantzos and S. Harissopulos (eds.), Proceedings of the International Symposium on Nuclear Astrophysics, Volos, Greece, July 6-11, 1998, p. 152 (Editions Frontieres). 2. K. Czerski, A. Huke, A. Biller, P. Heide, M. Hoeft, and G. Ruprecht, Europhys. Lett. 54 (4), 449-455 (2001). 3. A. Biller, K. Czerski, P. Heide, M. Hoeft, A. Huke, and G. Ruprecht, in Verhandlungen der DPG, Vol. 1, Gottingen, DPG-Fruhjahrstagung, 1997, p. 28. 4. A. Huke, Die Deuteronen-Fusionsreaktionen in Metallen, PhD Thesis, Technische Universitat Berlin, 2002. 5. Tatiana Dorsch, Theoretische Untersuchung der anomalen Asymmetrie im Verzweigungsverhaltnis der Reaktionen d(d,p) H und d(d,n) He im Verbund der Hydride der (Erd)Alkalimetalle. Diplomarbeit, Institut fur Atomare Physik und Fachdidaktik der Tech-nischen Universitat Berlin, 2004. 6. A. Huke, K. Czerski, and P. Heide, Accelerator experiments and theoretical models for the electron screening effect in metallic environments, in Proceedings of the International Conference on Condensed Matter Nuclear Science, ICCF-11, Marseille, France, November 2004. 7. W. M. Mueller, J. P. Blackledge, and G. G. Libowitz (Eds.), Metal Hydrides (Academic Press, New York, London, 1968). 8. R. E. Brown and N. Jarmie, Phys. Rev. C41 (4), 1391 (1990). 9. A. Biller, Einflufi der Vielfachstreuung auf Dicktarget-Yields in niederenergetischen Kernreaktionen. Diplomarbeit, Institut fur Atomare und Analytische Physik der Technischen Universitat Berlin, 1998. 10. H. Paetz gen. Schieck, and S. Lemaitre, Ann. Phys. 2, 503 (1993). 11. O. Geiger, S. Lemaitre, and H. Paetz gen. Schick, Nucl. Phys. A (586), 140-150 (1995).
E X P E R I M E N T S ON C O N D E N S E D M A T T E R N U C L E A R E V E N T S IN KOBE U N I V E R S I T Y
T . M I N A R I , R. N I S H I O , A. T A N I I K E , Y. F U R U Y A M A , A N D A. K I T A M U R A Division of Environmental Energy Science, Graduate School of Science and Technology, Kobe University, 5-1-1 Fukaeminami-machi, Higashinada-ku, Kobe 658-0022, Japan E-mail:
[email protected]
We review three kinds of experimental works underway in our laboratory to investigate nuclear events in solid or liquid materials. The largest effort has been given to experiments to confirm the 7 Li(d, n2a) reaction rate enhancement reaching 10 1 5 in liquid lithium which was reported by H. Ikegami and R. Pettersson, Evidence of Enhanced Nonthermal Nuclear Fusion (Bulletin of Institute of Chemistry, BENF No. 3, Uppsala University, Sweden, September 2002). Li liquid droplets are formed as targets, and to keep them as pure as possible, we built a liquid Li loop. Thus far, in all cases of irradiation at the temperature from 520 to 570 K with 1024keV deuterons, we have not been able to reproduce the Ikegami enhancement for the 7 Li(d, n2a) reaction.
1. Introduction Experimental studies on condensed matter nuclear reaction using ion beams at Kobe University are reviewed. First, we are continuing experiments on keV-deuterium ion irradiation of deuterated Au/Pd samples, searching for possible anomalous nuclear reactions in solids. 1 ' 2 The Au-coated surface of the Pd sample is irradiated with the keV-deuterium ions and with MeV ion beams for simultaneous characterization of the surface, while the rear surface is exposed to D2 gas at atmospheric pressure to load the sample. In addition, a modified version of the sample system without the implanter has been installed at another beam line of the accelerator exclusively in order to reproduce the so-called Iwamura effect.3 Iwamura et al. observed transformation of 133 Cs into 1 4 1 Pr during forced permeation of deuterium through a multi-layered film of Pd and CaO. In the present system of ours the nuclear transformation is monitored by in situ PIXE analysis during forced permeation of deuterium. The third system has been installed to reproduce the experiments made by Ikegami and Pettersson, 4 in which they observed an enormous enhancement of 7 Li(d, n2a) reaction rate in liquid lithium. To maintain high purity, we have set up a keV-deuteron irradiation system with a liquid Li loop, which enables us to continuously bombard pure Li in a closed container. 218
219
2. D(d, p)t Reaction Rate Enhancement The D(d,p)t reaction rate under irradiation of deuterium ion beam has been measured in the keV energy range in various samples to determine whether the nuclear reaction rate can be enhanced in a condensed matter. Kasagi et al. reported that in PdO the enhancement factor relative to the reaction rate for the deuteron pair in vacuum increases up to 50 at E<± = 2.5 keV, and that the screening energy deduced from the excitation function amounts to 600 eV.5 We are continuing the experimental study on the D(d, p)t reaction rate enhancement under deuterium ion irradiation of Au-deposited Pd (Au/Pd) with in situ and simultaneous measurement of deuterium density by accelerator analyses. In this section, we report recent results. The details of the experimental procedure are described in previous papers. 1,2 In the latest experiments, the time of exposure of the 1-mm-thick Au/Pd to deuterium gas was extended to 60 h to make the deuterium density as high as possible. The results are summarized in Fig. 1 as a function of the center-of-mass energy Ec of the reacting pair. In this figure, the theoretical curves calculated with screening energy Us6 taken into account are also shown for comparison.
103F
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i
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ioiev
\
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0.5
1
5
10
50
E c (keV) Figure 1.
Enhancement factor for D(d, p)t reaction rate.
In the experiments by Kasagi et al.,7 the value of Us was found to be 250 eV for the Pd bulk. With our Au/Pd sample, we have Us of the order of keV in some cases, but with rather poor reproducibility. It seems that the enhancement factor depends on an unknown parameter which we have not controlled yet. Further experiments with purified conditions are needed to clarify the enhancement mechanism.
220
3. P I X E Analysis of Palladium Complex under D 2 Gas Permeation In Ref. 3, it is claimed that deuterium permeation through a Cs-doped Pd/(CaO + Pd)/Pd sample induced a transmutation from 133 Cs to 141 Pr. In the present work, the experimental apparatus for PIXE analysis made in situ and simultaneously with gas permeation through samples has been built up. Fi gure 2 shows a schematic of the experimental system. A sample with a Pd(Cs)/CaO/Pd multilayer on the surface is placed in a vacuum chamber, and its rear surface is exposed to D 2 gas at a pressure of 0.1 MPa typically. The multilayer surface is irradiated with probe beam ions to emit characteristic X-rays, which are analyzed with a lithium-drifted silicon (Si(Li)) detector positioned at 135° relative to the probe beam direction. Another solid-state detector (SSD) is provided at —135° for RBS characterization of the sample. , Probe beam SSD for RBS
Si(Li)-detector for PIXE analysis
Figure 2.
Experimental system of PIXE analysis of metallic samples under gas permeation.
The density N of any target element can be evaluated from the X-ray yield AF X during irradiation with Q projectiles: AYX = QN At^-^-coKka 47T
Afi exp
-jit
cos 9
Te,
(1)
where Ci(E), WK, ka and Af2 denote the ionization cross section at a colliding energy of E, fluorescence yield for the K-shell, fractional transition probability of the KQ-line to all K-lines and the solid angle of the detector, respectively. Then, fj,, 9, T and s are the X-ray absorption coefficients of the target itself, the detection angle, X-ray transmittance of the absorbers in front of the detector and the detection efficiency of the detector, respectively. Here, homogeneous distribution of the element throughout the thickness At is assumed. A rough estimate shows that the minimum detectable areal densities of Pr and Cs a r e 4 . 3 x l 0 1 4 a n d l . 6 x l 0 1 4 cm 2 for 100-p//C/5-MeV a analysis. These limiting values of the areal densities have been confirmed by preliminary analyses of the Au/Pd sample and a CaO/Pd sample. Experiments using multilayered Pd(Cs)/CaO/Pd samples are in progress.
221
4.
7
Li(d, n 2 a ) Reaction Rate Enhancement in Liquid Lithium
An enormous enhancement of r Li(d, n2a) reaction rate in liquid Li was reported by Ikegami.8 They bombarded metallic Li targets in both liquid and solid phase with deuterium ion beams at the energy range of some tens of keV. In solid phase, no event was observed with the a-particle and neutron detectors, which was consistent with the reaction rate estimation based on the published nuclear cross-section data. On the other hand, in the liquid phase, a large number of a-particles were observed on the SSD. Consequently, the rate enhancement of 7 Li(d,n2a) reaction was estimated to be a factor of 10 10 -10 15 . They explain the phenomenon as follows. Deuterons with keV energy ("buffer energy"), where the nuclear collision dominates over the electronic one in the stopping process, penetrate deep into the s-electron cloud of Li atoms to form "united atoms" (LiD) at the classical turning point. This means formation of the atomic fusion state which makes adiabatic transition to the nuclear fusion reaction with some probabilities determined by the well-known Gamow factor. Regarding the energetic deuterons as solutes, this process can be treated within the framework of thermodynamics of chemical reactions in dilute solutions. As a consequence the Arrhenius equation for spontaneous chemical reactions is applied. The Gibbs free energy change AG in the exponent of the enhancement factor is negative in the present case of endothermic reaction d + 7 Li —> (LiD). Thus an enhancement exp(—AG/kT) by many orders of magnitude of nuclear fusion reactions in the metallic Li liquids could be realized. In the present work, we investigate the reproducibility of the 7 Li(d, n2a) reaction rate enhancement. The details of experimental procedure and experimental results are described below.
4.1. Experimental
Procedure
A schematic of the experimental system is shown in Figs. 3 and 4. Beams of 20keV deuterons are extracted from a duoplasmatron ion source and mass-analyzed with a 60° sector magnet. Deuterons are injected into the liquid Li target through an aperture of 10 mm in diameter. In the experiments made by Ikegami, the detection of the a-particles was frequently disturbed by hydroxide/nitride formation on the Li surface. To supply pure surface of liquid Li to the beam target, we have built a liquid Li loop in the present work. A total of 400 g of Li is prepared in the upper reservoir. Liquid Li heated in the reservoir is dripped into a manifold through a 0.25-in. pipe to form spherical liquid droplets which are bombarded with deuterons at the center of the target chamber. The end of the pipe, from which the droplets fall into the beam, was located close to the beam to make the irradiation time as long as possible. The temperature of Li is controllable to 570 K at the maximum so that the pipe does not get clogged. It takes about 10 h to finish dropping the total mass of Li, which is divided into several thousand droplets. The irradiation time for one
222
/CR-39 Figure 3.
View port /4 msr SSBD
Plane view of the experimental system.
droplet is controlled by adjusting the conductance of the valve, and ranges from a few tens ms up to several minutes when a drop hangs on the outlet of the nozzle. For the total mass of Li, the maximum irradiation time is several hours per a run, giving the total dose of 1016 protons. After one run Li is pumped from the bottom reservoir up to the upper reservoir by pressurizing the former with Ar gas. During the run the beam current measured with a Faraday cup placed at the downstream end of the manifold is monitored with an oscilloscope. A current dip due to a droplet crossing the beam is a measure of the current flowing into the droplet. a-particles are observed as the products of the 7 Li(d, n2a) reaction using an SSD and some sheets of solid-state track detectors (CR-39). Neutrons are observed with a rem-counter. The solid angles are defined to (1.1-5.0) x 10~ 3 sr by the active area of the detector with a 5.6 mm diameter. During the first run, a 12.5-/xm-thick Al film was mounted on each detector to shield it from the Li vapor. But some dots introduced by scattered Li droplets were found in the film. To prevent melting, we changed the filter from Al to 10.0-/im-thick Ti. An 241 Am alpha source was located in the target chamber to allow calibration of the SSD simultaneously with the ion beam irradiation of the Li droplets.
223
Figure 4.
4.2. Data
Vertical view of the target chamber and the liquid Li loop.
Analysis
The enhancement of the 7 Li(d, n2a) reaction rate could be confirmed by observation of enormous yields of a-particles. Ikegami observed the cc-particles forming a single peak on the MCA with an energy shifting around 7.5 MeV, which is a half of the Qvalue (15.1 MeV) of the 7 Li(d, n2a) reaction. All the counts in the range of interest (ROI), Ya, is regarded here as caused by the reaction a-particles. The 7 Li(d,n2a) reaction rate i? m per incident deuteron is calculated from the measured a-particle yield Ya as Ya/2
_
4TT
(2)
where Ad is t h e number of deuterons incident on a droplet, Nu is t h e number of Li droplets in a run, a n d AQ is t h e solid angle of t h e detector. Although a pair of a-particles is produced in every reaction, one of t h e m is observed on t h e detector, while t h e other is stopped in t h e Li bulk. Therefore, t h e number of t h e nuclear reaction is half t h e number of t h e detected a-particles multiplied by 4ir/AQ. T h e Rm is compared with t h e reaction rate Rc calculated under a n assumption
224
of continuous slowing down of the incident ions: -Eir
a(E) (-dE/dx) / " "
&E,
(3)
o
where nu is the Li density, — dE/dx the stopping power of the target, E{n the incident energy of deuterons, and a(E) is the reaction cross section for solid Li 9 with S = 2100 keV-b:10 al2{E)
EG E + Es
Si
E^iE
- exp + Es)1/2
1/21
(4)
The hypothetical reaction rate with a thermodynamic enhancement, Re, is expressed in the form of Arrhenius equation as follows: Re = Rc x exp
(5)
kBT]
where fee is the Boltzmann constant, T the temperature of the metallic Li, and AG is the change in Gibbs free energy during transition from the "dilute solution of deuterium in the Li" to the intermediate complex (LiD) which is transformed adiabatically to the [8Be + n] state through a transient 9Be* state. The exponential term in Eq. (5) is the enhancement factor defined in Refs. 8 and 11. 1000
a-Particles from 241 Am
1000
=100
Li(d,n2<x) reaction a-partic as 100
10
10
1 2 3 4 5 6 7 8 9 10 11 12 Energy (MeV) 24.0 keV-D+ 0.1 jUA/cm2 570 K 1.1 msr 10-/imTi Figure 5.
a-Particles from 241 Am Li(d,n2a) reaction q-particl
0 1
Incident particle Current density Temperature of Li Solid angle of SSBD Filter
2 3 4 5 6 7 8 9 Energy (MeV) 10.0keV-D+ 0.3 /Wcm 2 570 K 1.1 msr 10-jimTi
10 11 12
Two examples of energy spectra.
5. Results and Discussion 7
Li(d, n2a) a-particles having an energy of 5.7 MeV after passing through the Ti filter foil would be detected in the range from 5 to 6 MeV. Here the assumed broadening of the spectral peak may possibly be due to inhomogeneous deposition of
225
(6a) 520 K 1E-05
(6b) 570 K
1E-10
1E-15
1E-20 O
10.0keV, 570 K
•
13.3 keV, 520 K
A
20.0 keV, 570 K
O
24.0 keV, 570 K
1E-30 0.0
10.0
20.0
30.0
Deuteron energy £ d (keV)
Figure 6.
Energy dependence of the 7 Li(d, n2a) reaction rate.
Li on the Ti foil and FWHM degradation of the SSD in the environment with an elevated temperature. Two examples of the energy spectra recorded on the MCA are shown in Fig. 5. The spectra are dominated by 241 Am a-particles and electronic noise produced mainly in the ion source. We observe few counts, which could be electronic noise, in the energy ROI where the 7 Li(d, n2a) reaction products would appear. Figure 6 shows energy dependence of the 7 Li(d, n2a) reaction rate. Since there (a) 1E-04 %\ olO.OkeV 1E-05 • 13.3keV 1E-06 £20.0 keV • V a 24.0 keV 1E-07 \ \ X \ xX 1E-08 x 1E-09 \ x, 1E-10 \ | v N v , N 10.0 keV I k „ ^.'"x. 1E-11 i 13.3 keV v 1E-12 t \ X 1E-13 LU 1 x •"•"•"•'. 1E-14 I % 20.0.keV • -^ -s. 1E-15 ""*24.0keV 1E-16 400 500 600 700 800 900 1000
\ \
v .
Temperature of liquid Li (K) Figure 7.
1E+16 1E+15 1E+14 1E+13 1E+12 1E+11 1E+10 1E+09 1E+08 1E+07 1E+06 1E+05 1E+04 400
M.
X
£ 500
600
700
olO.OkeV • 13.3 keV A.20.0 keV O24.0 keV
800
900 1000
Temperature of liquid Li (K)
Temperature dependence of the reaction rate (a) and the enhancement factor (b).
226
are few observed counts in the ROI, as seen in Fig. 5, it is rather difficult to distinguish the reaction a-particles from the electronic noise. Assuming that only one count in the spectrum is ascribed to the 7 Li(d, n2a) reaction product, the maximum value of Rm corresponding to the one count is expressed as the data point with a vertical line extending to null in Fig. 6. The data points are shown in the figure as an open circle (lOkeV, 570K), a closed circle (13keV, 520K), an open triangle (20keV, 570 K), and an open square (24keV, 570 K). The solid curve shows the theoretical reaction rate Rc. The broken curves (Fig. 6a and b) show the thermodynamically enhanced reaction rate Re evaluated at the two different temperatures by using Eq. (5), where the value of the Gibbs energy change was assumed to be —1.35eV.xl Figure 7 shows the same data expressed as temperature dependence of the 7 Li(d,n2a) reaction rate and the enhancement factor, Rm/Rc. The symbols are the same as those used in Fig. 6. In Fig. 7b, the experimentally observed enhancement factor Rm/Rc is compared with the enhancement factor, Eq. (5). It is found that in all cases examined the enhancement factors are nearly equal to or much smaller than the thermodynamic enhancement factor. For example, the reaction rate Rm observed in the latest experiment for 20 keV deuteron irradiation is less than 2.3 x 10~ 13 . On the other hand, the reaction rate Rc calculated using Eq. (4) is 4.8 x 10~ 21 . The reaction rate enhancement Rm/Rc is therefore 4.8 x 107 at the maximum, while according to Eq. (5), the enhancement factor at a Li temperature of 570 K is expected to reach 8.6 x 10 11 . In summary the enhancement observed in the present work is much smaller than that claimed by Ikegami. At least it could be said that the Ikegami enhancement, if any, is realized under rather specialized condition, and therefore difficult to reproduce. 6. Summary We have described three kinds of experimental works at Kobe University: D(d, p)t reaction rate enhancement in deuterated Au/Pd samples, PIXE analysis of Pd complex under D2 gas permeation, and 7 Li(d, n2a) reaction rate enhancement in liquid lithium. The largest effort has been given to the last item, where we established the new experimental system capable of bombarding slag-free liquid Li droplets with mass-analyzed deuterium ion beams. Thus far, in all cases of irradiation at the temperature of 520-570 K with 10-24 keV deuterons, we have not been able to reproduce the Ikegami enhancement for the 7 Li(d, n2a) reaction. References 1. A. Kitamura, Y. Awa, T. Minari, N. Kubota, A. Taniike, and Y. Furuyama, in Proceedings of the 10th International Conference on Cold Fusion (LENR-CANR.org, Cambridge, MA, USA). 2. Y. Awa, et at, in Proceedings of the. JCF5, 15-16 December 2003 (Kobe University, Japan), pp. 6-10.
227
3. Y. Iwamura, M. Sakano, and T. Itoh, Jpn. J. Appl. Phys. 4 1 , 4642-4650 (2002). 4. H. Ikegami and R. Pettersson, Evidence of Enhanced Nonthermal Nuclear Fusion (Bulletin of Institute of Chemistry, BENF No. 3, Uppsala University, Sweden, September 2002). 5. J. Kasagi, H. Yuki, T. Baba, T. Noda, T. Ohtsuki, and A.G. Lipson, J. Phys. Soc. Jpn. 71, 2881-2885 (2002). 6. H.J. Assenbaum, K. Langanke, and C. Rolfs, Effects of electron screening on lowenergy fusion cross sections, Z. Phys. A - Atomic Nuclei 327, 461-468 (1987). 7. J. Kasagi, H. Yuki, T. Itoh, N. Kasajima, T. Ohtsuki, and A.G. Lipson, in Proceedings of the ICCF7, 1998. 8. H. Ikegami, Buffer Energy Nuclear Fusion (Bulletin of Institute of Chemistry, BENF No.l, Uppsala University, Sweden, September 2002); H. Ikegami, Jpn. J. Appl. Phys. 40, 6092 (2001). 9. S. Ichimaru and H. Kitamura, Phys. Plasma 6, 2649 (1999); also Refs. 15 and 16. 10. C.H. Johnson and C.C. Trail, Estimated from the data, Phys. Rev. 133, B1183 (1964). 11. H. Ikegami, et al, Enormous entropy enhancement revealed in linked nuclear and atomic Li + D fusion in metallic Li liquid, in Proceeding of the Fusion 03 Conference (Matsushima, 12-15 November 2003).
ELECTRON S C R E E N I N G C O N S T R A I N T S FOR T H E COLD FUSION
K. C Z E R S K I , P. H E I D E , A N D A. H U K E Institut
fur Atomare Physik und Fachdidaktik, Technische Universitdt Hardenbergstreet 36, D-10623 Berlin, Germany E-mail: czerskiQkalium.physik.tu-berlin.de
Berlin,
The observation of an enhanced electron screening effect in the 2 H(d,p) 3 H and H(d,n) He reaction taking place in deuterized metallic targets may be a breakthrough for explaining the phenomenon of cold fusion. Based on our experimental results, theoretical calculations of screening energies for five different target materials (C, Al, Zr, Pd, and Ta) have been performed within an improved dielectric function theory. The theory, including polarization of both quasi-free and bound electrons, describes the observed target material dependence of the screening energies qualitatively correctly, underestimates, however, the absolute values by about a factor of two. Applying an effective screening energy approach and realistic stopping power values, the theoretical cross sections, thick target yields as well as nuclear reaction rates have been calculated down to the energies corresponding to the conditions of cold fusion experiments. This allows for a comparison of the experimental results at higher energies with those achieved in the heavy-water electrolysis experiments. Constraints for the cold fusion reaction rates and the energy production arising from the experimental screening energies are discussed.
1. Introduction Apart from a poor reproducibility, there were two additional reasons for which the first cold fusion experiments (1) observation of a heat excess1 and (2) neutron emission2 during the heavy water electrolysis were faced with a large skepticism in the scientific community. First, a simple calculation of the penetration factor through the Coulomb barrier at room temperature 3 gave reaction rates for the d + d fusion reactions being a factor of 1050 smaller than the rates needed for explanation the experimental results. Second, since the neutron emission should be about a factor of 107 weaker than a reaction channel responsible for the heat production and clearly correlated to the fusion of the 4 He nucleus,4 the reaction branching ratios at room temperature completely contradict the experimental results obtained by means of the accelerator technique at deuteron energies of a few keV. Here, the mirror stripping reactions 2 H(d,p) 3 H and 2 H(d,n) 3 He, being equally probable, dominate by a factor >10 6 the electromagnetic transition 2 H(d,7) 4 He. Whereas the reproducibility of the cold fusion experiments has highly increased in the last decade 5 ' 6 and some important experimental relations have been found to achieve a larger energy production rate (e.g., a high deuteron density in a cathode 228
229
material 7 ), there are still only little efforts to compare the room temperature results obtained in metallic environments with those investigated at higher energy. The fairly developed experimental technique as well as higher counting statistics makes the accelerator experiments especially suitable to bridge the classical nuclear physics and the cold fusion research. Our last experiments, 8 ' 9 showing an enhanced electron screening effect in metallic targets for the d + d stripping reactions, and similar observations of other groups 1 0 - 1 3 can be the best example for such a development. Due to screening of the charges of reacting nuclei by surrounding electrons, the Coulomb barrier penetrability increases leading to an exponential-like enhancement of the cross sections compared to those measured for a gas target. Thus, an increase of nuclear reaction rates at room temperature due to the screening effect should amount to many orders of magnitude and contribute to an explanation of the cold fusion puzzle. For an overview of the experimental results (see Ref. 14). The purpose of the present work is to determine the d + d reaction rates at room temperature applying our experimental results with regard to the strength of the electron screening effect in metallic targets at higher energies. The approach presented here is based on an improved dielectric function theory 9 ' 15 ' 16 that enables to derive a reliable deuteron-deuteron potential in the host metal and calculate the reaction cross section, the thick-target yield and the reaction rate down to room temperature. The theoretical results will be compared with the data obtained in cold fusion experiments. 2. Electron Screening Effect In the case of Bohr screening, the screened Coulomb potential energy between two reacting deuterons can be presented as follows: 9
9
V(r = - e x p ( — ) « r \ a) r
9
a
,
1
where a is the screening length being of order of the Bohr radius. For projectile energies used in accelerator experiments where r
^'•7TOS(SJ,'(-^)-
(2)
Here Ecm denotes the energy in the center of mass system and EQ is the Gamow energy. The screening energy Ue takes into account a drop of the Coulomb barrier in the expression for the penetration factor. In comparison to the bare nuclei, the cross section for reactions in metallic environments increases exponentially, whereby Ue can be taken from fits to the experimental data. The Ue values determined in our experiments for C, Al, Zr, Pd, and Ta targets are depicted in Fig. 1. For
230
heavier metals the screening energy amounts to about 300 eV, which is one order of magnitude larger than the value 25 ± 5eV obtained in the gas target experiment. 17 From the theoretical point of view, the screening effect in metals can be described within the dielectric function theory. It enables to treat the electron screening as a static polarization of the metallic medium induced by the positively charged deuterons. The screened Coulomb potential V(r) is a solution of the Poisson equation and can be expressed as a Fourier transform:
where ev(q) and ec(q) are the static wave-number-dependent dielectric functions resulting from quasi-free valence electrons and from bound metallic core electrons, respectively. The elementary charge e is multiplied by a self-consistent charge formfactor ip(q) for deuterons with the screening electrons in the Thomas-Fermi approximation: p(q) = l - z + zq2/(q2 + k^F).
(4)
Here, the Thomas-Fermi wave number fc|F — Q/Ke2n/E-p has been used; n and Ep are the electron number density and the Fermi energy, respectively. The number z corresponds to the fraction of electrons bound to deuterons and can vary between 0 and 1. Since we are interested in the evaluation of the strongest possible screening effect, we set z = 1. In the absence of screening sv = ec = 1 and z = 0, V{r) reduces to the bare Coulomb potential ($(r) = 1). The response of the valence electron gas to an external field is given by the dielectric function: £v{q)
= 1
-l+v(q)G(q)P(qy
(5)
where v(q) — Aire2/q2 and P(q) is the static Lindhard RPA polarizability.18 G(q) is the static local field correction that takes into account the short range electron correlation and the exchange interaction. 19 In the case of core electron polarization we applied the dielectric function proposed in Ref. 20. Different from the valence electron polarization, ec takes a finite value at the limit q = 0. In the case of Ta the core-dielectric constant £c(0) = 3.21. The screening function 3>(r) calculated by a numeric integration of Eq. (3) differs from the simple Bohr screening exp(—r/a) particularly for larger distances, where the numeric potential becomes negative and shows characteristic Friedel oscillations. For the smaller distances the potential becomes attractive reducing appropriately the screening length (see Fig. 2). In the metallic lattice, besides electrons also positive ions can contribute to the screening of the Coulomb barrier between reacting nuclei. This effect, called cohesion screening, can be calculated in analogy to the dense astrophysical plasmas within the ion-sphere model of Salpeter 21 providing in the case of the TaD target a screening energy of 18 eV. In our calculations we used a more realistic model based on the universal ion-ion potential introduced by Biersack.22 This potential describes
231
the interaction between light as well as heavy ions at low energies with very good accuracy. Since the potential energy of two deuterons in the field of a host metal atom is larger than that of the helium atom produced in the fusion reaction, one obtains a gain in potential energy. For a rough estimation of the cohesion screening energy Ucoh, we calculated the potential energy gain resulting from the surrounding 12 host atoms assuming the same fee crystal structure for all target materials investigated. The theoretical value for the total electron screening energy Ue is a sum of the polarization and cohesion screening energies Upoi + Ucoh- The theoretical and experimental Ue values determined for all target materials investigated are presented in Fig. 1. -i
r
300
•
-•
•
Exp
250-
(!) 200 > > ra 0) 150
- • Theo
c
0 U)
c c
ffi (D 0
CO
100 50
0
Polarization
V
Cohesion
o-50 20
40
60
80
100
Atomic number Figure 1. Experimental and theoretical electron screening energies obtained for C, Al, Zr, Pd, and Ta targets.
The theoretical calculations describe the observed material dependence of the screening energy qualitatively correctly. The main contribution to the theoretical values is provided by polarization of the free valence electrons, although the contribution of bound electrons (core polarization) cannot be neglected. In the case of TaD, the resulting core polarization energy amounts to about 1/3 of the valence electron screening energy. An increase of Ue with the atomic number arises mainly from the cohesion contribution. However, the absolute values of the theoretically calculated Ue fail by a factor of about two. Including the self-consistent correction and the full wave number dependence of the dielectric function leads to lower
232
screening energies than those determined within the simplified theory. 15 No reason for such a large discrepancy between theoretical and experimental values has been found so far. Even if a possible contribution of the channeling effect to the experimentally determined Ue values would be taken into account - in the case of Ta much smaller than 100 eV (Ref. 23) - the difference between experiment and theory remains large. The biggest advantage of the theory presented is its ability to evaluate the screening energy for different target materials, not only metals but also semiconductors and insulators. A comparison with ongoing experimental studies performed with many target materials 13 ' 14 may allow in future to determine the strength of the various screening contributions and to find out which component should be enhanced to describe the experimental data completely. 3. Deuteron Stripping Reactions at Room Temperature Because of non-linearity of the screening potential, the screening energy, as defined in Eq. (1), loses its physical sense for the closest approach distances comparable with the screening length a. That corresponds to projectile energies comparable or smaller than the value e2/a. Thus, in order to apply Eq. (2) for calculation of the reaction cross section at projectile energies down to room temperature, we have to replace Ue by an energy-dependent effective screening energy /7eff • Similar to Ue, the effective screening energy can be still interpreted as an appropriate reduction of the bare Coulomb barrier, which should match to the penetration through the screened Coulomb potential. Therefore, Ueg has to be calculated from a condition setting equal the penetration factors as applied in Eq. (1) and that obtained within the WKB approximation with the screened potential V(r):
/ S - (-ffi) = - (-^fvwrw^ . (.) Here Ri and i?2 are the classical turning points in the WKB expression, and M is the deuteron mass. The results of calculations for Pd are presented in Fig. 2. There are two well-defined limits: at the high energy (Ecm > 1 keV) and at the low energy {Ecm < 10eV). The ratio between the low-energy and the high-energy C/eff value amounts to about 0.58, being nearly independent of the actual deuteron-deuteron potential. The total screening energy is the sum Ueg + Ucoh the value of which taken at the zero projectile energy UQ corresponds to 0.78 of the high-energy limit Ue. At deuteron energies below 10 eV, the effective screening energy remains almost constant, hence the expression for the cross section takes a very simple form. Starting from Eq. (1) we obtain <7scr(£cm) =
^ = 5 ° V^O^cm
e X
P I " V 7 T J y V VO J
K
~i= V-C'cm
^
^
c m
~*
0
'
^
where UQ and S 0 &re the screening energy and the S-factor taken at the projectile energy zero, respectively. Surprisingly, the cross section increases at low energies
233
as the barrier-penetration factor stays constant and the wave-length dependence dominates. 9 The cross section at room temperature strongly depends on the screening energy UQ and takes on the values for the 2 H(d,p) 3 H reaction: erscr = 4 x 10~ 24 b for UQ = 234 eV (corresponding to Ue = 300 eV for Pd at the high energy limit) and 0"scr = 1 0 - 3 5 b for UQ = 117eV (Ue = 150eV). In the accelerator experiments one deals with a flow of projectiles impinging on resting target nuclei, thus the total number of reactions per projectile stopping in the target, which is thicker than the projectile range can be expressed by the so-called thick-target yield: Bern
Yscr(Ecm) = [ ^§ddEcmocln^p
forfU^O.
(8)
E0
The denominator of the integral function represents the stopping power being proportional to the square root of the projectile energy. At very low energies, this is valid for both the nuclear and the electronic contributions to the stopping power. E$ is the minimum energy of the deuterons in the target before they will be captured in the crystal lattice, corresponding to the activation energy for deuteron diffusion in the target material (for Pd EQ = 150eV). Assuming the projectile energy equal to 1 eV and the realistic stopping power values for Pd, 24 one obtains F scr = 10~ 32 (Ue = 300eV). Even if we take into account that the slow projectile deuterons win kinetic energy due to adsorption at the palladium surface (ca. 4 eV, Ref. 25) and due to the electron capture in the bulk (13.6 eV) leading to the initial deuteron energy of about 18 eV, the resulting yield is still very small y scr = 2 x 10 - 3 1 . Multiplying this last value with a typical deuteron current used in the heavy water electrolysis experiments of about 1020 deuterons, one obtains a total neutron production rate in the 2 H(d,n) 3 He reaction smaller by 10 orders of magnitude than that of Jones et al.2'26 (about 1 0 - 3 to 10 _ 1 neutrons/s). The estimation for the neutron production at room temperature changes, however, completely if we assume that the target deuterons are not trapped in the crystal lattice but can move. This assumption seems to be reasonable for the electrolysis experiments where intensive irradiation of the palladium target (having very small deuteron binding energy) can lead to strong lattice oscillations in the surface region of the target, causing, in turn, a quasi-free movement of target deuterons. In the case of a thermal equilibrium, a useful quantity for a comparison with experimental data is the nuclear reaction rate:
RSCr(Ecm) = NaSCT(Ecm)vrel
= Nascr(Ecm)\j~p-
^ — = 2 = exp (9)
Here wrei is the relative velocity between the reacting deuterons, M is the deuteron mass, and N denotes the deuteron density of the target. Because of the energy dependence of the cross section at very low energies (see Eq. (7)), the reaction rate depends only on UQ and not on Ecm. Therefore, no assumption about the distribution of the deuteron velocity at room temperature is necessary.
234
1,2 • 0.8-
|PdD|
\ \
. V
0.4-
\%_ "
00 -
0.0
0.4
. Screening function with LFC Exponential screening function
- Screening function with LFC • Exponential screening function
-~ 0.8
20 12
1.6
2.0
0.1
10
100
1000 10000 100000
10
Deuteron-deuteron distance (10~ m)
Figure 2. Screening function calculated with the local field correction (LFC) (left) and the corresponding effective screening energies (right) obtained for PdD. For comparison results for the Bohr screening are also presented as dotted lines.
1
600 U0(eV)
800
'
r
1000
Figure 3. The nuclear reaction rate in dependence of the electron screening energy UQ. The calculations are performed for Pd.
In Fig. 3 the 2 H(d,n) 3 He reaction rate according to Eq. (9) in dependence of the screening energy UQ is presented and compared with the experimental reaction rates determined in the heavy-water electrolysis experiments. Additionally, a theoretical
235
estimation made by Koonin and Nauenberg 3 who applied the deuterium molecule potential for the deuteron-deuteron interaction, is also depicted. The range of the electron screening values Uo determined in our experiments is marked by vertical lines. The neutron production rates measured by Jones et al.2 are by about a factor 107 smaller than the nuclear fusion rates determined by Fleischmann et al.1 from the heat excess release and require UQ = 220 eV which corresponds to the screening energy Ue of about 280 eV at the high-energy limit in agreement with our experiment. Contrary, the energy production rate 1 demands Uo = 620 eV (790 eV at high energies) being clearly outside our experimental constraints. 4. Discussion and Conclusions Applying the improved dielectric function theory we could qualitatively describe the observed target material dependence of the screening energy. The theory provides, however, absolute values being by a factor of two smaller than the experimental ones. Additionally, based on the derived deuteron-deuteron potential in metallic environments, we were able to determine the energy dependence of the screening energy and consequently to calculate the cross section, the thick-target yield and the reaction rate down to room temperature. An agreement with the neutron production rates at room temperature reported by Jones et al.2 could be obtained under the assumption of quasi-free moving deuterons in the target lattice during the heavy-water electrolysis. The 2 H(d,n) 3 He reaction rate calculated for Pd (UQ — 230 eV) is by a factor of about 1040 larger than the results obtained by Koonin Nauenberg 3 for the deuteron molecule. Thus, the electron screening effect in metals seems to provide the largest contribution to explain the results of cold fusion in the electrolysis experiments. On the other hand, since the observation of the excess heat production is probably connected to the fusion of 4 He (Ref. 4) with the rate by about a factor of 107 larger than the neutron emission, there should obviously exist an additional phenomenon leading to a further increase of nuclear reaction rates at room temperature. In our opinion, however, the remaining factor 107 might be achieved within classical nuclear physics without any unusual assumptions. An example for such an approach could be a thin resonance in the 4 He nucleus lying close to the d + d reaction threshold. Supposing a nearly single-particle width of this resonance for the deuteron channel and simultaneous quenching of the nucleon channels, one can explain major experimental results concerning the cold fusion. The deuteron width of the resonance can be expressed by the i?-matrix formula:
r d = 2P d fc d | 7d | 2 ,
(io)
where P d and fcd are the penetration factor and the wave number in the d + d channel, respectively, and |7 d | denotes the reduced resonance width. If the d + d channel has the largest partial reduced width, the total resonance width will drop for sub-Coulomb deuteron energies because of the decreasing penetration factor, causing to the same extent an increase of the resonance-maximum cross section by
236
many orders of magnitude. Furthermore, the hypothetical resonance could change the reaction branching ratios within the resonance width of a few eV in favor of those supposed for the cold fusion. In addition, the small width of a resonance would also explain the problems connected to the reproducibility of cold fusion experiments. Small local changes in the lattice structure can lead to differences in the energy of the reacting deuterons of order 1 eV and hence decide whether the reaction will be enhanced by the resonance or not. For other heavy metals we also expect large enhancement factors. However, alteration of the screening energy by a few tens of eV results in changing the reaction rate at room t e m p e r a t u r e by many orders of magnitude. Therefore, in the search for a suitable material for the cold fusion, an important aim of future experiments should be to distinguish which screening contribution - the valence-electron polarization, the core-electron polarization or the cohesion screening - is enhanced in metallic environments. On t h e other h a n d a material enabling large fusion rates at room t e m p e r a t u r e should also ensure a high deuteron density and a relatively low deuteron binding energy in the lattice. T h e latter condition is necessary in order to set deuterons easily into movement, which further increases the reaction probability by many orders of magnitude. Thus, P d seems to be an ideal material for study nuclear reactions at room t e m p e r a t u r e . Summarizing, the electron screening effect in metallic environments enhances t h e d + d fusion rates at room t e m p e r a t u r e by about a factor of 10 4 0 compared to the previous theoretical prediction. If the hypothesis of a thin resonance in the 4 H e nucleus is right, we could also explain an additional enhancement of 10 7 needed for the observed heat excess in the heavy water electrolysis experiments. Moreover, the characteristics for the cold fusion branching ratios could be also clarified. A first evidence for such a possibility is the experimental observation of the target material dependence of the neutron to proton ratio in the d + d stripping reactions presented in this conference as well. 2 7
References 1. 2. 3. 4. 5. 6. 7. 8.
9. 10.
M. Fleischmann, S. Pons, and M. Hawkins, J. Electroanal. Chem. 261 (1989) 301. S.E. Jones, et at, Nature 338 (1989) 737. S.E. Koonin and M. Nauenberg, Nature 339 (1989) 690. A. De Ninno, et al, in Proceedings of the ICCF-10 (Cambridge, MA, 2003). S. Szpak and P.A. Mosier-Boss (Ed.), Technical Report 1862 (Office of Naval Research, San Diego, CA, 2002). M.C.H. McKubre, Proceedings of the ICCF-10 (Cambridge, MA, 2003). M.C.H. McKubre and F.L. Tanzella, Proceedings of the ICCF-7, Vancouver, Canada, 1998. K. Czerski, A. Huke, A. Biller, P. Heide, M. Hoeft, and G. Ruprecht, Europhys. Lett. 54 (2001) 449; Proceedings of the International Conference on Nuclear Asrophysics "Nuclei in the Cosmos", July 6-11, 1998, Volos, Greece, Edited by N. Prantzos and S. Harissopulos (Editions Frontieres), p. 152. K. Czerski, A. Huke, P. Heide, and G. Ruprecht, Europhys. Lett. 68 (2004) 363. H. Yuki, et al, JETP Lett. 68 (1988) 823.
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11. 12. 13. 14. 15. 16. 17. 18. 19. 20. 21. 22. 23. 24. 25. 26. 27.
J. Kasagi, et al, J. Phys. Soc. Jpn. 71 (2002) 2281. F. Raiola, et al, Eur. Phys. J. A 13 (2002) 377. F. Raiola, et al, Eur. Phys. J. A 547 (2004) 193. A. Huke, K. Czerski, and P. Heide, This conference, ICCF-11 (Marseille, France, 2004). K. Czerski, A. Huke, and P. Heide, Nucl. Phys. A719 (2003) 52c. S. Ichimaru, Rev. Mod. Phys. 65 (1993) 252. U. Greife, et al, Z. Phys. A 351 (1995) 107. G. Grosso and G.P. Parravicini, Solid State Physics (Academic Press, NY, 2000). S. Moroni, D.M. Ceperley and G. Senatore, Phys. Rev. Lett. 75 (1995) 689. D.E. Penn, Phys. Rev. 128 (1962) 2093. F.E. Salpeter, Aust. J. Phys. 7 (1954) 373. J.F. Ziegler, J.P. Biersack, and U. Littmark, The Stopping and Ranges of Ions in Solids (Pergamon Press, New York, 1985). K. Czerski, et al, Nucl. Instr. Meth. B 193 (2002) 183. J.F. Ziegler and J.P. Biersack, code SRIM, http://www.srim.org. J.H. You, et al, Phys. Rev. B 43 (1991) 7293. S.E. Jones, et al, Proceedings of the ICCF-10 (Cambridge, MA, 2003). A. Huke, K. Czerski, T. Dorsch, and P. Heide, This Conference, ICCF-11 (Marseille, France, 2004).
LOW MASS 1.6 MHz S O N O F U S I O N REACTOR*
ROGER STRINGHAM First
Gate Energies, P.O. Box 1230, Kilauea, HI 96754, E-mail:
[email protected]
USA
We are using one of the most remarkable pulsing systems that nature offers for producing transient high-energy densities and I have been fortunate enough to be involved with it for over 20 years. Over time, we have increased the frequency of our piezo cavitation drivers and are now at 1.6 MHz and find that our results are the same. Even better, the Q x /reactor g, the energy density, is drastically increased when compared to our 40 and 20 kHz piezo s y s t e m s . 1 - 3 The cost is decreased by at least an order of magnitude and the durability is greatly increased. All Q values in this paper are dQ/dt J / s or W. The systems differ in several ways because of the 40 times increase in frequency. These 1.6 MHz systems produce more sonoluminescence (SL), and more but smaller bubbles and an energy density in the collapsing bubble system that is the same magnitude as the 40kHz systems. 4 , 5 . In one cycle those small bubbles, initially a few 100 nm in diameter, that are resonance size for the 1.6 MHz input will grow isothermally. After the acoustic wave passes into its positive pressure phase the bubbles collapse violently keeping a portion of their energy. In the final stage of collapse the energy densities are literally astronomical. The collapse process produces from the bubble a jet that implants deuterons into a target foil. The time frame for this 1.6 MHz system is 40 times faster than for the 40 kHz system. The number of deuterons (protons) in the jet drops from 10 9 to 10 5 but the deuteron high density remains the same. The 1.6 MHz low mass (LM), device (weighing 20 g) produces the same excess heat, Qx, as the 40 kHz system (weighing 3 kg). The calorimetry is a D2O or H2O flowthrough system measuring its T; n and T o u t with a DT value probably a little lower than the true value. The flow of D2O is measured at 60ml/min or 1 ml/s. The total errors in the Qx measurements are in the order of 2 W. These values range up to 40 W depending on acoustic input, temperature, pressure, cavitating liquid, and target.
1. Introduction Over 15 years ago in 1989, the author heard about the experimental work by Fleischmann and Pons at the University of Utah and within a few days the author was using cavitating D2O with a Pd foil target. The author saw evidence of foil melting and possible excess heat generation. Three years later after filing patents, the initial three individuals, Dick Raymond, Larry Klein, and myself invited Russ George and Steve Wolff with help from Tom Benson and together started EQuest Sciences. After a year or so we produced helium four, tritium, and Q x . In 1998, EQuest *ICCF 11, Marseille, France; 31 October to 5 November 2004, Jean Paul Biberian, Chairman. 238
239
was dissolved and transformed into First Gate Energies with Dick Raymond still president. We were producing excess heat using a 40 kHz system in amounts very similar to what we are producing today with our LM 1.6 MHz device.1 We moved our laboratory from Mountain View, CA to Kilauea, Kauai, HI, in 2002. Most of our efforts here have been directed to the LM 1.6 MHz sonofusion device. We have limited resources so have lowered our goals to cutting costs and doing calorimetry experiments with the measurement of Q x production. At this time we cannot afford to look for the products of Q x production - the expensive analysis of helium and associated products. These products have been found in the past 2 ' 3 in our lower frequency reactors. The investigation was undertaken to advance sonofusion technology and to find better and more compelling data showing Q x production. (1) There are more transient cavitation bubbles (TCBs), formed per second. (2) Smaller TCB bubbles are produced. (3) The smaller bubbles have less energy but the same energy density at the final stage of the collapse process. (4) There is less target damage due to reduced number of deuterons in the implanting jet. (5) The advantage of incorporating the sonoluminescence (SL), emission data from the sonofusion reactor is its application as a tool. The SL emission is coincidental with the jet plasma formation and deuteron concentration that is implanted into the target. So we have accomplished the above and found several more advantages using the higher 1.6 MHz frequency. (1) The data is much more reproducible. (2) The Qx generation is now commercially competitive. (3) These small LM devices can be ganged together resulting in a large and cost effective high-density energy source. (4) Our confidence level in our technology has greatly increased. The physical phenomena of the TCB and stable cavitation bubble growth and collapse has been well documented 4 but not understood in the physics sense. When compared to the 20 and 40 kHz systems the short time frame of 0.6//s for the 1.6 MHz frequency that includes the bubble's complex growth and collapse mechanism is scaled to fit.5 The path of the birth and death of a TCB in the cavitating liquid during one cycle of 1.6 MHz pressure swing, going from low pressure involving the rapid bubble expansion into the high pressure acoustic compression, follows. The initial infant bubble that is selected by the system's parameters to become a TCB for one acoustic cycle is in a parameter controlled environment. The parameters that control the TCBs in the cavitating water are temperature, pressure and Qa input (see Fig. 1). Initially, among all the bubbles in the low pressure zone is the infant TCB bubble population of resonant size which couples with the 1.6 MHz acoustic input, Qa, of an appropriate voltage. With the temperature and pressure of the water and Qa working together in the LM SF reactor and piezo creates an operating resonance (see Fig. 1). The infant bubble grows rapidly isothermally and collapses as a TCB during one acoustic cycle. In a 1.6 MHz time frame the collapse is much more rapid and potentially more energetic but with perhaps one ten thousandth the particles (105 particles in the implanting jet). The energy densities are at least the same as the 20 kHz systems and the jet formation is assumed to be
240
similar along with the target implantation. 1 these three parameters.
3
These phenomena are controlled by
Frequency = 1.6 MHz
—
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Rn = 2000 nm
flj = 200 nm -flf = 20 nm Time
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Infant bubble reservoir
~ 0.625 j"S Isothermal bubble growth
Adiabatic bubble collapse
TCB jet formation 100 ps
Figure 1. A schematic of the growth and collapse of a bubble in an intense 1.6 MHz acoustic field producing TCBs as the acoustic wave progresses through a cycle. The time period for this process is less than 0.6 /J,S. The infant bubble at a radius of Ri originates in the low-pressure portion of the oscillating acoustic field where the Ri expands rapidly and isothermally and upon reaching the high pressure portion of the acoustic field the bubble growth slows reaching a maximum radius Rg. At this point, with its newly gained mass, the bubble starts its implosive and accelerated collapse path to radius R{. Here a portion of the collapse bubble contents which are now dissociated into a low-energy high-density plasma produce a jet and SL. The SL is the only tool we have that communicates the state of the bubble plasma. This collapse process is considered pseudo adiabatic because much of its original mass is lost at the bubble interface. As the pulse of SL photons created by TCB collapse is emitted, with the formation of a jet, the remaining bubble contents become the high density micro accelerators. Some of these accelerated and z-pinched deuteron or proton ions are implanted into target lattices. These final processes are sub-picosecond in duration.
There are several scenarios that describe the bubble collapse and the SL emission and several physical dilemmas that do not fit. For example, the SL pulse length and the relation between the SL emitting cavity and its wavelength are two of these dilemmas. 6 It is clear that in our experiments we see a correlation between Q x and SL emission (see Fig. 4a and b). The temperature factor that we have worked with to this point is from 25 to 80° C. The pressure of Ar is one atmosphere saturation and there are 4 atm of pressure developed in the reactor via the restricted water flow through the small reactor orifices. There was more than a 10-fold increase in SL when the initial Ar was increased from one to two atmospheres
241
with no corresponding increase in Qx. This is very interesting and is explained by the Ar concentration being responsible for SL not Q x - So to use SL as a tool we must consider the Ar concentration levels which should be the same in Qx comparison studies. We want to engineer the LM SF reactor by doing some material improvements and expect to operate the LM SF reactor at higher temperatures. 2. Calorimetry The calorimetry is simple and conservative. We look at the data generated at steady-state temperature conditions with the Qi pulsed one minute on and one minute off to help clarify the magnitude of the radio frequency (RF), interference during the thermocouple measurements. The contribution of RF to the temperature measurements of Tin and T out was at most +0.2°C. The effect is more pronounced in the TC for the oscillator and transformer (O&T) calorimetry with about 0.5°C increase. The DT (T out — T;n) measurement is of the circulating water through the low mass sonofusion (LM SF) reactor. The other half of the calorimetry measurement is the water flow rate through the 1 ml volume of the LM SF reactor. The flow meter was placed just before the bubbler and regularly monitored (see Fig. 2). The flow rate values for all runs were between 54 and 60 ml/min. A volume calibration of the flow rate of 54 ml/min (measured at the bubbler) show that the volume of water passed per minute is 60.1 ml/min. This is 12% higher than the flow-meter measured value at a flow of 54 ml/min. For example, the LM SF reactor has a flow rate, F, of 1 cm 3 /s and a Tin and a T out through its 1 cm 3 volume. DT xF xk = QQ and is the basis for our calorimetry. Prior to each run the circulation system was turned on and T in and T out were measured and their values were steady and nearly equal (Fig. 3). Then the pulsing acoustic oscillator was turned on (duty cycle) and the data gathering was continued to the end of the run. Data reduction using the collected wattmeter and TC data produces the following calorimetric relations. All Q values in this paper represent d Q / d i J / s o r W. Qi: Watts in from wattmeter. Qo&t: The total watts lost to the oscillator box calorimetry with Joule heater (JH), for calibration. Qa = Q\ — Qo&zt- The acoustic watts into reactor. QQ: The total watts out of reactor. Qx = Qo — Qa.'- The watts of excess heat. The total watts out (Q0), equals Qa plus Q x , where Q x = DT x F x 4.184 - Q a , and where F is the flow rate in ml/s. The acoustic watts input, Qa, is determined from a Lucite closed box calorimeter inside the air circulating light box which houses the reactor and PMT, photomultiplier. The Lucite calorimetry box contains the oscillator and transformer, O&T, and is calibrated against the input of a 15 W J heater to find the steady-state heat lost to the O&T. The heat lost by the O&T is Qo&t and is that portion of Q\ that is not Qa. A linear plot of JH watts-input
242 Air in & out
• Flow meter Co-olant water bath HX • Lexan T window Piezo
Oscillator 1.6 MHz Calorimetry box
W Duyt cycle
|
Wattmeter
Variac Low mass sonofusion reactor
PM"T Target >a power in Water in
Figure 2. The experimental set-up for gathering data from the reactor - lower left inset. It is made up of a circulation system, a power input system, an SL measurement system, a calorimetric system, a calorimeter for the heat loss of the oscillator and transformer, and a d a t a gathering system. The circulation system has the primary task of removing heat from the low mass SF reactor and the measured DT and flow rate for the calorimetry. The circulation system includes a pump, a coolant bath, a 1 ml LM SF reactor, a flowmeter, and an Ar bubbler. The power input, Qi, had the option of being pulsed or continuous wave cavitation, D, and t h a t power to the wattmeter, W, and the 1.6 MHz LM reactor is controlled by a variac, V. The SL emission is collected by the P M T and counted in a black box environment. The calorimetric system has two parts. The first part is the measurement of the LM SF reactor DT (Tout — Tj n ) and the water flow rate in the black box. The second part is the transformer and oscillator heat losses measured in a calorimetry box calibrated with a Joule heater, JH, also located in the black box with its forced air circulation. The set-up for data gathering consists of a thermocouple system measuring the critical temperatures and a calorimetry box for measuring the steady-state temperature of the transformer and oscillator with its Joule heater that provides for the partition of Q\ into Q a and Qo&t- The bubbler keeps the circulating water, Ar saturated and the coolant bath keeps the Ti n close to ambient temperature. The data collection system samples the temperature every 5 s. Lower left inset is the reactor detail showing the 1 ml reactor volume with the placement of the target foil in the reactor window for a baffled P M T SL photon emission counting.
vs. the calorimeter steady-state DT for O&T is used to determine Q0&t values for Q^ The total input, Qi, was divided between Qo&t and Qa and relates to the efficiency, E, of the acoustic input, the ratio of Qa/Qi- E varied between 0.33 and 0.23 for these experiments. The time for the transformer to reach steady state was 3 h because of its high mass. This required more experimental time. The time for the LM sonofusion reactor to reach a practical steady state was 5 min.
243
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Figure 3. An abbreviated form of a data sheet, where the data were logged every 5 s. This is a data sample of 8 min near the last of run of Series B cavitated with Pd foil #2 as a target, in D2O, and under 2 atm Ar. This run was typical of the data collected. The first characteristic to note is the shape of the H&C curves and the one minute duty cycle shown by T C #2. The second, note the temperature R F interference shown by TC # 0 is no more than 0.3°C but the oscillator & transformer shown by TC # 5 has an RF interference of close to 2.0°C. Note that the temperature in the light box T C # 7 is constant and does not show RF interference as does the coolant bath temperature, TC # 6 . The DT is measured in the off mode and produces a Q0 of 42 W. Qi measured by the wattmeter is partitioned by E to give Q a .
For example, a LM SF reactor weighing 20 g generates data for its calorimetry at steady state. The reactor has a mass water flow through it of 1 ml/s and with a DT of 15°C. From DT x F x k we calculate the Q0 = 55 W. We know from Q 0 & t and E how to partition a 50 W Q; that determines the value of Qa. Subtract 35 W, the calorimetric value of Qo&t, from 50 W Qi to give the 15 W for Q a . Subtracting Qa from Q 0 leaves a Q x of 40 W. The analysis of the data shows the importance of Newton's cooling law when applied to the heating and cooling of water flowing through the LM SF reactor. The matching cooling and heating curves [T = Tsse~aAt/CM and T = T ss (l -aAt/CM^ JI _ j^g-fct] j t data are the result of the pulsed acoustic e or seen n ne input into circulating water. (Being pulsed, the reactor system does not reach a final steady state but cycles between a high and a low value approaching its steady-state temperature value.) The constant k that is the exponent {a A/CM) can be determined from the data where a is the heat transfer coefficient, A is the surface area of the reactor, C the reactor's heat capacity, and M is the reactor's
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SL Relative photo emission (b) Figure 4. The pulsed d a t a collected in two different systems; system A is the Pd target foil with cavitating D2O and 1 atm of Ar and, system B is the CuBe (98.1/1.9) with cavitating H2O and 1 atm Ar. (a) and (b) The difference between relative intensity of SL (photon emission in lOOOcounts/s) with the intensity 10 times greater for H2O, the B system as expected. 8 - 8 (a) The excess heat production, Qx, is eight times greater in A than B. (b) The acoustic input, Q a , does not vary in A and B with respect to D2O and H2O.
245
mass. The T ss is the steady-state temperature and T is any temperature on that particular heating curve. The heating and cooling curves, H&C, can be constructed mathematically that closely match the curves produced by the data. One could justify the use of that constructed Tss in the DT calculation. This would add around 15% to the DT values determined in the pulsing mode. (In the pulsing mode the heating curve reaches a point well up on the heating curve but is cut off by the duty cycle before reaching its true steady state, Tss.) The pulsed low mass, LM, system comes close to a steady-state temperature and we use that conservative value for the Q0 calculation. In these experiments most of the heated mass is not the LM SF reactor. Most of the heat content is from the mass of water flowing at 1 ml/s at its DT. The remaining mass of 20 g is that of the LM reactor (the momentary container of circulating water) has a three times longer time constant for its H&C curves than the circulating water. The H&C curves due to the LM reactor can be seen in the data with the circulation off. To maintain a DT of 10°C for the 20 g reactor one looks at the initial slope (DT/time) from the cooling curve data of the 20 g LM SF reactor. And from the H&C curves it requires 1W input to maintain a DT of 10°C in the static reactor. When one looks at the pulsed data of a 10°C DT of circulating water that produces 42 W of QQ (DT x F x k) that number overwhelms the reactor's 1W maintenance value. (The LM SF reactor with several smaller H&C curves with their associated mass, heat capacity, and longer time constant are used in the above calculation.) Q is the heat in joules per second or watts for the values below. The error for a typical Q0 measurement of 50 W, where watts = DT x F x k is as follows. To produce DT from the input Qi from the wattmeter and the measurement of Qa by the subtraction of <50&t from Q; is the path to Q a and the DT determination. The errors in the wattmeter measurement were in the order of ± 1 W in 100 W and in the Q 0 & t calorimetry measurement ± 2 W and in the TCs ±0.2°C in 100°C. The calculated error in Qa input and DT is then ±7%. The error in the calibrated flowmeter measurement is ± 2 c m 3 / s for 60cm 3 /s is 3.3%. So the error for Q0 is ±8%. The calculation of (X is Qo ~ Q& and the error for Qx measurement is ±10.4%. The measurements are on the low side for Qx because of unaccounted convection heat losses to the environment during the experiment which increase as DT increases so the measurements of Q0 and Q0&t are conservative. These are main sources of error. 3. Experimental Water was circulated through the sonofusion reactor's 1ml volume at a rate of l m l / s . using an FMI pump with a 0.635 cm ceramic piston and sleeve. The cavitation liquid was circulated via the pump through to the 0.382 cm inside diam. stainless steel cooling coil 150 cm long exchanging the circulating water's heat and exchanging it to an ambient 21 coolant water bath. The water is then passed through a 10//m filter then to the 0.05 cm inside diam. input reactor orifice (input T;n measured with a thermocouple). A residence time for the circulating reactor
246
water of I s . to produce the DT of 0-12°C and with a Q a of 0-15 W means a Qx from 0 to 40 plus watts with the 100/xm Pd target foil and D 2 0 (system A). The hot water left the reactor through a 0.05 cm inside diam. output reactor orifice (output T out measured with a TC) and out of the light box and into the flow meter (see Fig. 2). The circulation continues to the Ar bubbler then back to the pump. We used two different target foils, Pd 100 /nm thick with cavitating D2O with 1 atm Ar (system A) and CuBe (98.1/1.9) 125 /jm thick with cavitating H 2 0 with l a t m Ar (system B) which produced about 1/8 Qx of the system A. Both systems were pulsed with a duty cycle of 1 min on and 1 min off. The Q\ power to the O&T was regulated by a variac from 30 V that produced no SL (only background counts of 100s _ 1 ) to 140 V with 90kcounts/s of SL emission [(kcounts are lOOOcounts/s registered by the Systron-Donner counter/timer from the Hamamatsu 3 HC 125 03 PMT (see Fig. 2)]. The 2-cm diameter sealed Lexan window of the sonofusion reactor was 90% covered with 1 x 2 cm target foil between the PMT and piezo. The target foil was placed 1 mm in front of the window and 2 mm in front of the piezo in the 1 ml of reactor liquid. Even with the small volume and foil blockage of the window a maximum of 100 kcounts/s was observed in system B. The SL Kcounts increased with the increase of Qi from the variac voltage. The counter registered a count rate for each second of cavitation foil exposure. It was pointed out that the count was only a relative photon emission rate 6 as photons are emitted in 100 ps pulses that swamp the PMT. The SL was the only connection we had to the high-speed transient phenomena occurring in the TCB collapse process. The relation of SL and Qx gave us an observational tool to the high density low energy plasma and deuteron or proton production in the 1.6 MHz sonofusion reactor. This was a great aid in adjusting the critical parameters of temperature, Ar pressure, and acoustic input for Qx reproducibility. The input temperatures for these experiments were steady-state temperatures at Tin which was near ambient. There were some complications from a contribution from H&C curves other than water and are discussed in the calorimetry section. Tout was controlled by Qa and Q x , which produced Q0, so it varied from near ambient to 15° above depending on Q\. The running steady-state temperature was at Tout of the sonofusion reactor and the heat disbursing system. The temperatures were measured with TT-K-40 thermocouples and the data logged by an Omega Measurement Computing - PCI-DAS-TC with 16 TC channels. There were two types of runs, pulsed and continuous. The pulsed data were naturally cooler being in the on-mode for half the time. The continuous wave experiments agree with the pulsed runs but we are not sure about the possible RF interference (see Fig. 4). The Ar pressure was kept at 1 atm by the slow bubbling of Ar into the D 2 0 or H 2 0 bubbler (see Fig. 2), and this was not changed during the experiments so the external pressure was always 1 atm Ar for all runs. The parameter that controlled the Q x production was Qa/Qi- The input from the line voltage was controlled by the variac and passed this power through a wattmeter, a 100 W Ohio Semitronix Wattmeter, and into a transformer with 50 V RMS output to a 70 DC volt rail
247
feeding a 1.6 MHz oscillator which produces the Q a powering the reactor piezo. The oscillator and transformer, O&T, were in a Lucite calorimetry box along with the calibration JH where the Q0&t losses were determined. The Q a and E could then be determined (see Section 2). The Qi is varied via a variac from 4 to 50 W (the SL threshold is 4W). In system A, when Q\ is adjusted to 50 W, the SL is 100,000counts/s and in system B 10,000 counts/s. 6 ' 8 The character of Qa produced from our oscillator used in these experiments included a varying voltage of the 1.6 MHz signal carried in a 120 Hz envelope. The maximum voltage amplitudes of a 50 W Q; (150 V peak to peak that includes a family of lesser voltages) produces a maximum Q a at 15 W. This allows, as we have done earlier experiments, a voltage amplitude that varies from 0 to the maximum voltage for a particular Qi setting. The Q a input of a multi voltage system shows the mechanical resonance of the system to choose its coupling voltage even though it may be small. The Q a maximum signal can be varied from 0 to about 150 V peak to peak. The data show that at Q[ of 4W there is no SL and no apparent Q x above the error level. By increasing Q; to the oscillator from this 4 W point there is an increasing SL and The reactor system was dynamic; the water circulated through the reactor at a measured rate, and differed from a static reactor system where the water remains in the reactor without movement. In the static system the heat must be removed by exterior contact with a flowing heat exchange media. We have used both systems in the past and they both produced Q x . The dynamic system was chosen for its quick response to heat removal. We used the SDS 200, a 200 MHz oscilloscope, with a 5 GS/s sampling rate to observe the 1.6 MHz input signal Qa and the SL PMT voltages. The PMT output voltage response was split with a SL event counter that measured the rate of photon emission from the LM SF reactor and oscilloscope.
4. Results There were two systems studied. System A was the D 2 0 , Pd, Ar and system B was the H2O, CuBe, Ar. The water circulation was basically l m l / s and the external pressure of Ar was one atmosphere. The controlling parameter was the acoustic input Q; that was partitioned between Qa and Q0&t which determines the E and equals Qa/Qi- The Pd target foil produced the highest Qx/Qa and the CuBe (98.1/1.9) target foil in H 2 0 produced 1/8 the Q x of the Pd foil in D2O. Both foils appeared untouched by exposure to cavitation. This was a good result as both Cu and Pd suffered damage when exposed to 20 and 40 kHz cavitation processes. The durability of the foils and the low mass of the 1.6 MHz Q x producing systems have the characteristics needed in a commercial system. The low running temperatures between 30 and 45° C and the low pressures are much less than the 20 and 40 kHz systems with running temperatures well over 100°C.
248
During the experiments the systems malfunctioned several times primarily when the water circulation system leaked or plugged causing the reactor to overheat and fail. Sometimes we only needed to fix the leak but on several occasions we lost the piezo when its vapor deposited electrode peeled off the surface or the transistor in the oscillator burned out. The reduced data collected from these systems is shown in Figs. 4 and 5. 5. Interpretation and Conclusions The advancements of our sonofusion technology over the last year has grown at a rapid rate. It now is plausible to discuss the possibility of sonofusion becoming an economically commercial energy source. Increasing the cavitation frequency has solved several problems that we have encountered in our past work - size, cost, energy density and durability. The size has been reduced from 5 kg to 20 g and the cost from $15,000 to $150. The excess heat produced per gram of LM SF reactor has been increased about 500 times and the duration life-time of a cavitation exposed target foil has been extended to a year or more but needs more testing to verify this fact. The relation between Qx and SL appears that they are coupled together for a particular system. The H2O systems produce more SL than do the D2O systems. So within a particular system SL is a good predictor for Qx- Figure 5a and b shows these relationships and demonstrate the utility of SL as a tool. A problem with this tool requires the alignment with the PMT and the careful sizing and placement of the target foil. Also the slow rise time, 70 ns, of the PMT response, is not compatible with the pico second pulse time. However, the somewhat obstructed path of the emitted SL photons moderates that problem. An interesting note on one run where the Ar pressure was increased from the usual one to two atmospheres of Ar produced 10 times more SL but the same Q x . 6 ~ 8 (see Fig. 4a and b). This phenomena was the result of substantial mechanical pressure increases in the LM SF reactor brought about by its small in and out orifices. Here in the reactor the running pressure did not change so the Q x did not change but the amount of Ar in the D2O was doubled and produced a tremendous change in SL emission with no change in the experimental set-up. QQ is measured by a conservative process of DT X F x k = J/s and when this number is equal to Qa ±2 W then there is no Qx. But if it is larger, which it will be if Qa is more than 4 W, then Q0 — Q& = Qx is a significant number between 3 and 40 W. This number depends on the value of Qa and as it increases so does Qx- When using the oscillator to drive the piezo there was a limit to the Q a produced as the efficiency, E, {Qa/Qi) as Q\ pushed the oscillator to failure. To produce more Qx we look to appropriate changes in the controlling parameters that include increase in pressure, temperature, and acoustic input. These improvements would involve the different reactor materials and improving the heat removal system. These small LM SF reactors can be ganged together to form a high energy density array producing
249
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(b) Figure 5. (a) Q x for similar conditions is 2-8 times greater with the D2O Pd system than the H2O CuBe system. The excess heat increases with the increase of Q a . (b) The multiplication factor, ME, that indicates the advantage in cost when producing low-grade heat using Q; + Q x to heat water for use as a source for hot water or for space heating in buildings. The ME times the power cost — an ME of 2 gives two times the power/$.
250
Q x that can be transformed into more useable forms of energy. We looked at two different cavitation pulsed systems. The system A, consisted of a Pd target foil, D2O, and Ar at 1 atm. The system B, consisted of a CuBe target foil, H2O, and Ar at 1 atm. The systems A and B are the same in every aspect except for the water. When the SL emission count from the PMT is recorded the H 2 0 is much larger than for D 2 0 . The system A is deuterated, the system B is protonated, and the nuclear paths are quite different after the high-density low-energy plasma target implantation. The implanted deuterons or protons may follow one of these paths D + D -> He4 + heat or P + P -» D + heat or P + D -> T + heat. No long-range radiation was found, only heat indicating some transient coherence in the implanted species. 2 ' 3,7 The pulsed data system A shows that as Q a increases so does Q x to a more than a 2/1 ratio (Q x /Qa) at the higher Qi values. System B shows a much lower increase of Q x as Q a is increased although it does appear to be real with a ratio of about 1/2. If one prefers to call system B a zero for a reference value, it gives all the data a foundation as no true zero has been found to date (see Fig. 5a). System A which produces a power multiplication effect, ME, as high as 1.7 becomes a useful tool for showing the economic advantage of the LM SF reactor water heating capabilities. The whole system including the oscillator and reactor are submerged in a tank of moving water. This allows the complete recovery of Q; plus Q x and their conversion into heat. This ME can be expressed as (Qi + Q x )/Qi and is 1.0 with no Q x production with an input Q; of 50 W, a Q a of 16 W and a Q x of 38 W the ME is 1.7 (see Fig. 5b). There is a substantial amount of work to be done to make sonofusion a replacement for a hydrocarbon-based economy and we look forward to that day. We have good continuous cavitation data that shows a four times better result for A system than for B system. One of the first tasks is finding by-products that are associated with the Q x production to place next to the Q x evidence. We are currently making improvements at a rapid pace in our sonofusion technology. Make the E, oscillator efficiency, a value approaching 1.0 where it is now 0.3. Increase the Q*/Qa ratio to 10 where it is now 3.0. Find new and better thermoelectric devices, TEDs, for the direct conversion of heat to electricity. Make the reactor more robust through the application of material technology so reactors can endure higher temperatures and pressures. Perform a marriage of steam technology with the sonofusion reactor. Look for target materials that are improvements over what we have today. The above are a few of the areas that we are currently investigating. We are now developing the idea of ganging the unit LM SF reactors together to form large heating devices. A practical size to build is a 4-unit device that is being tested with higher temperatures and pressures to produce at least 160 W of Q x with a much more efficient Q a /Qi of 50% or better. We are developing the calorimetry for this 4-unit system, which should have an ME of 2.3. A Qa of 15, a Qj of 30 and a Q 0 of 50 and for a 4-unit system 120 W for Qi: 200 W for Q 0 , and 60 W for Q a —> ME of 2.2. If we gang 32 of these 4-unit systems together a 10 kW device results (see Fig. 6).
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OUCDiCI OpfOOHD
Figure 6. A 4-unit piezo driven LM SF reactor. Ganging 32 units together produces 10 kW. Such a device delivers low-grade hot water at 80° C.
6. Summary We have today an infant technology that will grow at a very fast pace. Sonoluminescence is a fascinating subject and its study forms the basis of the SF technology. A paper 9 that gives many good references on SL of the single bubble can also be applied to the multibubble systems. Also see the references of.7 We can represent the utility of the sonofusion reactor as a device that can act as a power multiplier using the multiplier effect, ME, to measure the advantage over today's power costs (see Fig. 5b). There is one piece of important information missing; evidence of the other products associated with Q x production. So we go back to our old data from our 20 kHz system that reported the products of 4 He and 3 T (Ref. 2) and look for some of these products in the new analysis, by Francesco Celani, of our new target foils and we thank him for any results he may find. The Q x watts/(gram of reactor) is 2 and we expect that improvements will follow. If, for example, Q{ — 40 W and the Qa/Qi is 0.5 and Q x is 40 W, then the total watts output for one LM sonofusion unit is 80 W. This 20 g LM reactor can be used as a powermultiplier, ME, of value 2.0. If we have four LM reactors working together as a system the total output is 320 W and 25 of these 4-unit systems working together produces 8000 W with a reactor mass of 2 kg. When 1000 units are ganged together we can produce 80,000 W that would cost $300/day ($0.17 for a kWh). However, this system has a ME of 2 and the cost for Q; would be $150/day. With a 1000
252 unit reactor the Q x t h a t is produced would be worth $55,000/year and the initial cost for a sonofusion reactor might be $20,000 making the cost benefit for the first year $35,000. If the 40,000 W for Qi are solar generated, then we are looking at an added initial cost t h a t would be compatible with our sonofusion reactor with longt e r m dollar savings. T h e total heat production is Q\ + Qx with a cost reduction of 50% for low-grade heat used in building's utility heating. This is all possible with the sonofusion technology we have today and this technology is continually improving.
Acknowledgments I would like to t h a n k the individuals t h a t helped us get this 1.6 MHz system to the point it is in today: Dick Raymond, Richard America, Kip Wallace, Lynn Marsh, Julie Wallace, Ted Mill, Fran Tanzella, and Mike McKubre. References 1. R. Stringham, in Proceedings of the International Symposium on IEEE Ultras, 5-8 October 1998, Vol. 2 (Sendai, Japan), p. 1107. 2. R.S. Stringham, in Proceedings of the ICCF-8, 21-26 May 2000 (Lerici (La Spezia), Italy), pp. 299-304. 3. R.S. Stringham, in Proceedings of the ICCF-9, 19-24 May 2002 (Beijing, China), p. 323. 4. M.P. Brenner, S. Hilgenfeldt and D. Lohse, Rev. Mod. Phys. 74, 425-484 (2002). 5. K.R. Weninger, C.G. Camara and S.J. Putterman, Phys. E. Rev. 63, 016310-1 (2000). 6. G. Vazquez, C. Camara, S.J. Putterman and K. Weninger, Phys. Rev. LETT. 88 (19), 197402-1 (2002). 7. R.S. Stringham, in Proceedings of the ICCF-10, 24-29 August 2003 (Boston, USA, to be published). 8. R.A. Hiller and S.J. Putterman, Phys. Rev. Lett. 75 (19), 3549 (1995). 9. M.P. Brenner, S. Hilgenfeldt and D. Lohse, Single-bubble sonoluminescence, Rev. Mod. Phys. 74, 425-484 (2002).
R E S E A R C H INTO CHARACTERISTICS OF X-RAY EMISSION LASER B E A M S F R O M SOLID-STATE CATHODE M E D I U M OF H I G H - C U R R E N T GLOW D I S C H A R G E
A L E X A N D E R B. K A R A B U T FSUE
SIA "LUTCH", 24 Zheleznodorozhnaja Street Podolsk, Moscow Region 142100, Russia
X-ray emissions ranging 1.2—3.0keV with dose rate up to l.OGy/s have been registered in experiments with high-current Glow Discharge. The emissions energy and intensity depend on the cathode material, the kind of plasma-forming gas, and the discharge parameters. The experiments were carried out on the highcurrent glow discharge device using D2, H2, Kr, and Xe at pressure up to lOTorr, as well as cathode samples made from Al, Sc, Ti, Ni, Nb, Zr, Mo, Pd, Ta, W, Pt, at current up to 500 mA, and discharge voltage of 500-2500 V. Two emission modes were revealed under the experiments: (1) Diffusion X-rays was observed as separate X-ray bursts (up to 5 x 10 5 bursts a second and up to 10 6 X-ray quanta in a burst), (2) X-rays in the form of laser microbeams (up to 10 4 beams a second and up to 10 1 0 X-ray of quanta in a beam, angular divergence was up to 10 — 4 , the duration of the separate laser beams must be r = 3 X 1 0 ~ 1 3 - 3 X 1 0 ~ 1 4 s, the separate beam power must be 10 7 -10 8 W). The emission of the X-ray laser beams occurred when the discharge occurred and within 100 ms after turning off the current. The results of experimental research into the characteristics of secondary penetrating radiation occurring when interacting primary X-ray beams from a solid-state cathode medium with targets made of various materials are reported. It was shown that the secondary radiation consisted of fast electrons. Secondary radiation of two types was observed: (1) The emission with a continuous temporal spectrum in the form of separate bursts with intensity up to 106 fast electrons a burst. (2) The emission with a discrete temporal spectrum and emission rate up to 10 1 0 fast electrons a burst. A third type of the penetrating radiation was observed as well. This type was recorded directly by the photomultiplier placed behind of the target without the scintillator. The abnormal high penetrating ability of this radiation type requires additional research to explain. The obtained results show that creating optically active medium with long-living metastable levels with the energy of 1.0-3.0 keV and more is possible in the solid state.
1. Introduction Experiments were carried out previously to define a possible mechanism of high-energy phenomena in the solid-state cathode medium during high-current glowdischarge. The experimental results showed that the character of the detected X-ray radiation essentially differed from the known X-ray emission types. It indicated the importance of research into the performances of the detected X-ray radiation from the solid-state medium of the cathode sample material of the high-current glow discharge. 253
254
Penetrating radiation passing through the discharge chamber walls (5-mm thick steel) was recorded during high-current glow discharge (Fig. I). 2 The experiments showed that it was the secondary radiation occurring when interacting with the primary X-ray laser beams from the solid-state cathode medium with the material of the chamber walls and construction elements and lead protective shields.1 The created 100% reproducible technology for generating the X-ray laser beams, which would allow research into the performances of the secondary penetrating radiation.
Figure 1. Various variants of the experimental device: (a) system of a PM-scintillator placed 21cm from the cathode, (b) system with the PM-scintillator placed 70 cm from the cathode, (c) system with the PM-scintillator - PM placed 70 cm from the cathode with superimposition of the cross magnetic field.
2. Experiment Method and Results The experiments were carried out with the device that produces high-current glow discharge using deuterium, hydrogen, Kr, and Xe. The cathode samples made of Pd and other metals were disposed on the cathode-holder above which a window for output of penetrating radiation was placed. The window was closed by 15 /jm Be foil for protecting the detectors against visual and ultraviolet radiation (Fig. 1). A periodic-pulse power supply was used for the glow discharge, with a rectangular current pulse. The duration of the discharge current pulses were 0.27-10.0 ms, period between impulses was 1.0-100ms. The discharge was carried out in D2, Xe, and Kr. The X-rays recording was carried out with use of the thermo-luminescent detectors, X-ray films placed above the cathode at various distances, and scintillation detectors supplied with photomultipliers. 1
255
Thermoluminescence detectors are not sensitive to electrical noise and allow registering the absorbed radiation dose quantitatively in absolute units of dose measurement. Thermoluminescence detectors (TLD) based on A1 2 0 3 crystal register penetrating radiation beginning from the background values of radioactive radiation of the environment. These were to measure energy intensity and to evaluate the average energy of a soft X-ray emission in the discharge. To determine the average energy a special cassette (seven-channel spectrometer) was used. Seven channels (holes) with a diameter of 5 mm each were made in the cylindrical body of the cassette. The detectors in the form of disks with the diameter of 5 mm and thickness of 1 mm were arranged in the holes. A set of the beryllium foils having thickness 15, 30, 60, 105, 165, 225, 225, and 300 /im (in the each hole the foil having the special thickness was arranged) was arranged on the side of emission input in the body holes. Two TLD detectors were arranged outside the camera for the registration of background value of the emission dose. A pinhole camera gives a spatial resolution of X-ray emission and an opportunity to determine where the radiation emerges from. The time characteristics of the penetrating radiation were determined with the scintillation detectors supplied with the photomultipliers (PM). The signal from the PM was transferred to a fast preamplifier with an amplification constant of
/ x-ray, 4x10
Photons/burst
6
3x106
(a) 2x106 1 x106 0 ' X-ray, i Photons/burst 3x106
\k.
Figure 2. Typical oscillograms of the X-ray emission signal from the system PM-scintillator covered with the Be foil with the different thickness: (a) with covered the 15 ^ m Be shield, (b) with covered the 30 |im Be shield. The Pd-D2 system, the discharge current — 150 mA.
256
k = 7 and then to the two-channel computer digital oscillograph with the limit resolution frequency of 50 MHz per a channel. Organic scintillators on the base of polymethylmetacrelate (PMMA) with luminescence time of 3-5 ns were used. The time resolution of the entire path from the PM up to an oscillograph (experimentally) was 70-80 ns. Electrical noise was observed only when passing the front and back fronts of the current impulses feeding the glow discharge (Fig. 2). Three various variants of assembling the discharge chamber with the channel for the radiation extraction was used (Fig. 1). In the first variant (Fig. la) PMscintillator was placed 21cm from the cathode surface. The channel diameter for extracting the radiation was equal 1.7 cm. In the second variant the PM-scintillator was placed 70 cm from the cathode, and the diameter of the channel for extracting the radiation was 3.2 cm (Fig. lb). To define the type of penetrating radiation, the third variant of the experimental assembly included the magnetic system consisting of a constant magnet and an elliptic iron magnetic circuit (Fig. lc). The axis of the magnetic system poles was 35 cm from the cathode perpendicular to the axes of the radiation extraction channel. The magnetic field induction in the gap between poles was 0.2 T. For the determination of quantitative registration characteristics the thermoluminescence detectors were calibrated in the gamma-emission fields. The experiments were carried out using the following systems of cathode plasma-forming gas: Pd-deuterium. The obtained results show that the doses obtained by the corresponding detectors decrease exponentially with increasing the thickness of Be foil. The main component of the X-ray emission energy is in the range of 1.0-2.5 keV, but there is a component with a higher energy too. X-ray intensity was registered for the different values of current and voltage. The procedure of recording and measuring was developed as applied to two modes of the X-ray emission: a mode of the diffusion radiation bursts, generation of X-rays as laser microbeams. The intensity of the luminous flux from the scintillator when it was in the mode of generating X-ray laser beams was approximately 1000 times as much as the intensity in the mode of the diffusion bursts. In this case, the amplification constant of the radiation recording system changed by changing the supply voltage of the photomultiplier and by changing the amplification constant of the oscillograph. Under some experiments the luminous-absorbing filter attenuating the luminous flux coming to the PM was installed between the scintillator and PM. Two types of the filters were used, that attenuated the luminous flux by 50 times and by 2500 times, respectively. The intensity of the X-rays (number of photons a second) coming to the detector was determined by dividing the energy radiation power absorbed by the detector by the energy of an X-ray photon. Further the intensity falling to one detector was given to 2p solid angle. For the PM-scintillator the relative intensity of the X-rays was determined as the total of the amplitudes £ A ; of all the X-ray bursts within the time interval of
257
I s (Fig. 1). Then the relative intensity was given to a physical magnitude by the intensity value measured by the TLD detectors. The experiments using the PM-scintillator and shields made of the beryllium foil with thickness of 15 and 30 /*m gave the assessment of the X-rays energy value of Ex-ray ~ 1.0-2.5 keV (for different cathode materials, Table 1) that matched to the TLD detectors results well. 'x- ray, 4x106 • 3x106 2x106 1 x106 0 /(mA), 200 *
Photons/burst
(a) ! , , , . » *• •
;L •
!
_T^
0 A f = 10 n s . ' X-ray,
Photons/burst
t^s)
(b)
Af=10us
f(ns)
Figure 3. Typical oscillograms of bursts of the diffusive X-ray emission (PM-scintillator) during passing the discharge current. Ta-D2 at 175 mA. (a) PM-scintillator 21cm from cathode (as in Fig. la), (b) PM-scintillator 70cm from cathode (as in Fig. lb).
to Cn 00
Table 1. Material of cathode Glow discharge voltage (V) Glow discharge current (mA) X-ray energy during passing the discharge current, Ex-ray (keV) X-ray energy without current, _Ex-ray (keV) X-ray energy flow density, ip ( x l O - 4 W / c m 2 ) Number of X-ray pulses per second, Np ( x l O 5 pulses/s) Max energy of one X-ray pulse, i ? m a x ( x l O - 1 0 J) Number photons in one pulse, n (xlO 5 )
1650 130
Sc 1540 130
Ti 1730 170
Ni 1650 150
Mo 1420 210
Pd 1650 138
Ta 1600 138
Re 1520 125
Pt 1650 138
Pb 1610 138
1.54 1.68 1.2 3.8 1.2 0.50
1.26 1.5 1.7 3.7 1.5 0.74
1.45 1.46 3.18 6.0 1.9 0.83
1.91 1.96 1.2 3.4 1.5 0.49
1.48 1.33 1.36 2.7 1.5 0.63
1.98 1.71 1.4 4.0 1.3 0.41
1.62 1.62 2.13 5.1 1.4 0.55
1.36 1.38 0.74 2.2 1.1 0.87
1.47 1.75 1.9 4.4 1.6 0.68
1.36 1.45 1.7 4.4 1.3 0.94
Al
259
The dependence of changing the radiation intensity on the distance was determined using the experimental devices according to the diagrams in Fig. la, b. Magnification of the distance between the PM-scintillator detector and the cathode from 21 up to 70 cm resulted in reducing the radiation intensity more, than under the law l / r 2 (Fig. 3). Such result could be explained to the fact the radiation indicatrixes of the separate bursts had the elliptic shape with enough narrow angular orientation. The high intensity of X-ray emission allowed obtaining an optical image of the emission area. The pinhole camera with the hole with the diameter of 0.3 mm (as an optical lens) was used. The image shows that the cathode area with the diameter of 9 mm and especially its central part has the largest luminance (Fig. 4). The X-ray laser beam generation occurred under precisely fixed parameters and conditions of glow discharge.
(a)
(b)
Ncathode
Figure 4. The image of the X-ray cathode obtained using the camera obscura (pinhole camera). The objective with 0.3-mm diameter closes by the 15 /mi Be shield. With Pd—D2 and the discharge current of 150 mA, and the exposure time - 1000 s: (a) voltage is 1350 V, (b) voltage is 1850 V. The image is positive.
(1) The generation occurred only when periodic-pulse current was supplied. It did not occur with direct current, although X-rays as bursts of diffusion radiation did occur with direct current. (2) Some critical parameters of occurring the generation by the gas pressure of PGD in the discharge chamber and by the voltage of the discharge (7QD- The generation occurred at PQD(^GDcrit, UGD) ^GDcnt- A small change in the discharge pressure or voltage led to the occurrence of generation (the change in pressure was A P Q D = 0.2-0.3 Torr, and in voltage AUGD — 30-50 V). (3) These parameters were different for various cathode materials (Fig. 5). For example, when using Pd cathode, the X-ray laser generation occurred at pressure being twice as much as when using Ti cathode. (4) The parameters of occurring the X-ray laser generation depended also on the plasma-forming gas (Fig. 6). (5) When operating, the generation intensity gradually decreased (obviously
260
because of degradation of the cathode surface) and stopped in the course of time. This phenomenon was especially clear for cathode materials with a large coefficient of a material sputtered in the discharge plasma (e.g., Al, Pd, and Pb).
Photons/beam
X-ray. 1.2 x 1 0 8 0.8 x 10 8
(a)
0.4 x 10 s 0
*
Photons/beam
' X-ray.
I "11
8
1.2 x 10 (b)
0.8 x 10 8 f0.4 x 10 8 ' x - r a y | Photons/beam
1
1.2x1080.8 x 10 s 0.4 x 10 8
- I
,. 1 II 'I ' X-ray.
Photons/beam
!!
(c) ml''
ii:.,.
l
!
1.2 x 10 8 0.8 x 10 8
A t = 200 us
f(us)
Figure 5. The typical oscillograms of bursts from X-ray laser beams (PM-scintillator) in a D2 discharge for different kind of cathode samples: (a) Al, (b) Sc, (c) Pb, and (d) Ta. Assembly is by Fig. l a (the distance from the cathode to the detector is 21cm). *Pulse peaks are selected via a discriminator amplifier.
The X-rays as laser beams consisted of the separate beams, presumably, having a small diameter (up to 10 6 -10 10 photons in a beam). These magnitudes were obtained in assumption that the system of the PM-scintillator operated in the linear area, taking into account the magnitude of reducing the amplification constant of the path when recording the X-ray laser radiation. The X-ray laser beams emission occurred during the discharge burning and within up to 100 ms after turning off the current. At the specific parameters of the discharge the generation of the X-ray laser beams was observed only some ms later after turning off the discharge current (up to 20-30 beams after each current pulse). The time oscillograms type of the generated beams depended on the type of the plasma-forming gas (Fig. 4) and type
261
' X-ray> . Photons/beam " ] [ ' " '
1.2 x 1 0 8 -
; :<,
,t.'
Pd-D
I
' X-ray 1.2 x 1 0
Photons/beam
*
8
0.8 x 1 0 8 0.4 x 1 0 8 0 /(mA) ,
100 0
(b)
\ I \f< i J'"? .•'.i.'.iii.J. '
m|
(c) V J
Pd-Kr
__h—.„—^~-___
ml
m2
f(HS)
Af=100p,s
Figure 6. Typical oscillograms of bursts from X-ray laser beams (PM, scintillator) in the discharge for different kind of gases (a) D2, (b) Xe, and (c) Kr. Assembly is by Fig. l a (the distance from the cathode to the detector is 21cm). The cathode sample is Pd, current - 50 mA. *Pulse peaks are selected via a discriminator amplifier.
of the cathode materials (Fig. 5). In this case the amplification constant of the path of recording the radiation was enough large and the upper part of pulses was cut off by the amplifier discriminator. The estimation of the X-ray laser beams divergence was carried out under the experiments with use of the experimental devices according to the diagrams in Fig. la, b. The magnification of the distance from the cathode up to the system of the PM-scintillator from 21cm up to 70 cm resulted in inappreciable reducing the signal (Fig. 7). These results proved to be true when using 50-multiple optical niters (Fig. 7). The experiments with superimposition of the cross magnetic field showed, that radiation had two components (Fig. 7c). The X-ray laser beams were not diverged in the magnetic field and recorded by the PM-scintillator. The other part of the radiation did not hit on the detector. Hypothetically, this part of the radiation was fast electrons with the energy of £0.5 MeV. The fast electrons beams can be formed when interacting the primary X-ray laser beams with the walls of the channel for extracting the radiation. The real form of the radiation pulses was observed
262 x-ray.
Photons/beam
1.2 x 10! 0.8 x 10s -
(a)
0.4 x 108 0 /(mA) 200 •
-tj-
' x-ray.
ml
^**4^2
Photons/beam
8
1.2 x 10 0.8 x 108 -
(b)
s
0.4 x 10 0 /(mA) 200
.i...l J.—iu_
o E-f
X-ray
isr-f^p2.
Photons/beam
8
1.2 x 10
0.8 x 10s
(»in,
0.4 x 108 0 /(mA). 200
;_| '
ST-jVa^_ A t = 200 us —4
I—
/(us)
Figure 7. The typical oscillograms of bursts from X-ray laser beams (PM-scintillator) in the discharge for different kind of assemblies. The cathode sample is Ta, D2, current - 100 mA. (a) Assembly is by Fig. l a (the distance from the cathode to the detector is 21 cm without a cross magnetic field), (b) Assembly is by Fig. l b (the distance from the cathode to the detector is 70cm without a cross magnetic field), (c) Assembly is by Fig. l c (the distance from the cathode to the detector is 70cm with a cross magnetic field). * Pulse peaks are selected via a discriminator amplifier.
using the luminous-absorbing filter (Fig. 8) reducing the luminous flux from the scintillator to the photomultiplier by 2500 times. The track images of the X-ray laser beams were obtained using the X-ray film placed above the cathode at various distances. The diameter of the laser beam tracks was 6-10/xm at a distance 100 mm from the cathode and up to 20-30/im at 210 mm (Fig. 9). High radiation intensity and the process of the photo emulsion solarization gave the positive tracks image. The angular divergence of each beam was estimated up to 10~ 4 (based on the results of measuring the track diameters at various distances from the cathode).
3. Secondary Penetrating Radiation The experiments were carried out with the device of the high-current glow discharge1 with use of H2, D 2 , Kr, and Xe at pressure up to lOTorr, and the cathode samples
263
:-ray^ 6x10 ! 4x109 2x1090 /(mA) 200 0
(a) • .i....
^f,
rMj'Jju':.
A f = 100 ns •**!—t-
f(ns)
6x109 4 x 109
(b)
2x109 0
A. i-'l'l3«AlWvWArf«^^ J ^ J > m ^ < ^^_
/(mA) 200 0 A f = 100 ns t(ns)
Figure 8. The typical oscillograms of bursts from X-ray laser beams (PM-scintillator with optical filter) in the discharge for different kind of assemblyes. (a) The cathode sample is Ta, (b) the cathode sample is Mo, current, 100mA; D 2 . (a) Assembly is by Fig. 7a (the distance from the cathode to the detector is 21cm). (b) Assembly is by Fig. 7b (the distance from the cathode to the detector is 70 cm). *Pulse peaks are selected via a discriminator amplifier.
made of Al, Sc, Ti, Ni, Nb, Zr, Mo, Pd, Ta, W, and Pt at current up to 500 mA, and the discharge voltage of 500-2500 V. The pulse-periodic power supply of the glow discharge with the pulses duration of the discharge current of t = 0.3-1.0 ms and period of T = 1.0-100 ms was used. The targets as the shields made of various materials foil (Al, Ti, Ni, Zr, Yb, Ta, and W) with thickness of 10-30 mm and of 1.0-
Figure 9. The increased negative image of the flare spots of the roentgen laser beam tracks for the different distances from cathode, the roentgen film (Kodac and XBM) covered with the 15/im Al shield. The system P d - D 2 , the discharge current - 130mA; the exposure time - 1000s; (a) for 100 mm from the cathode surface, (b) for 210 mm from the cathode surface. The image is negative.
264
3.0 mm were arranged at a distance of 21 and 70 cm from the cathode (Fig. 10a, b). The scintillation detector supplied with the photomultiplier was used for recording the secondary radiation. The device with a channel for extracting the radiation with the length of 70 cm and the magnetic system creating a cross magnetic field relatively to the radiation axis at a distance of 35 cm from the cathode was used for defining the type of the secondary radiation (Fig. 10c).
(a, b)
(c)
Figure 10. Schematic representation of an experiment with X-ray targets (secondary penetration radiation research). PM-scintillator system. 1, cathode sample; 2, anode; 3, 15 /jm Be foil screens; 4, scintillator; 5, photomultiplier; 6, magnetic bar (magnetic induction between magnetic poles is about 0.2 T); 7, X-ray targets made a foil of various materials.
The procedure of the secondary penetrating radiation registration and calibration of the detector was similar to the procedure of registration the primary radiation beams. 1 Under the experiments the recording of the time radiation spectrums was carried out within the time between the back and forward fronts of the discharge current (being free of the discharge current). The radiation type was defined with the device with a channel for extracting the radiation with the length 70 cm when being free of the cross magnetic field and the imposed magnetic field was available (Fig. 10b, c). When free of the magnetic field, significant attenuation of the PM-scintillator signal was not observed when increasing the distance from the cathode to the detector from 21 to 70 cm (Fig. 11a). Superimposition of the magnetic field with an
265
'ei. beams, electrons/beam _ - * v
J 1' 1;
1.2 x10 8 0.8 x10
8:
|
1 1 1
0.4 x10 8 0 /(mA) 200 : 0 3lectrons/beam ' el. beams'
|—k.
i
i T1
._
if
ii
II i
j l
f
r
i
|
i
i
f
i
30707-08
„
IYI
1.2 x10 8 0.8 x10 8 0.4 x10 8 0 /(mA) 200
o
T1
•
^~_
k_
.1 i
30707-20 in*
Af=100us*4-4 -
— 0 *
Figure 11. The typical oscillograms of bursts from secondary penetration radiation beams (fast electrons) in the discharge for different kind of assemblies. The cathode sample is Ta; current, 100 mA; D2. (a) Assembly is by Fig. 7a (target arrange at a distance of 21cm from cathode without superimposition of the cross magnetic field), (b) Assembly is by Fig. 7c (target arrange at a distance of 21 cm from cathode with superimposition of the cross magnetic field), secondary penetration radiation (fast electrons) don't registered. *Pulse peaks are selected via a discriminator amplifier.
induction of 0.2 T led to complete disappearing of the signal in the PM-scintillator (Fig. l i b ) . Thus, the secondary radiation was the flux of the charged particles (presumably fast electrons) with a small angular divergence. W h e n increasing the distance from 21 t o 70 cm, t h e primary X-ray laser beams kept an ability to generate the secondary radiation when interacting with the targets made of various materials (Fig. 12). These results were the additional confirmation of the fact t h a t the X-ray laser beams had a small angular divergence. T h e type of the oscillograms of the primary radiation bursts was defined by the cathode material. T h e secondary X-ray radiation of two types was observed. (1) Radiation with a continuous time spectrum as separate bursts with intensity up to 106 photons per a burst. This emission began 0.5-1.0 ms later after turning off the discharge current. (2) Radiation with a discrete time spectrum and radiation intensity up to 10 9 photons per a burst. Distribution of the bursts by the time of this radiation was defined by the target material. T h e generation of the secondary penetration radiation is supposed to occur from solid medium of the lead shield. T h e results of recording the radiation bursts were used for the time spectrums construction. T h e dependence of the radiation bursts amount on the time interval between the back front of the discharge current impulse and forward front of the radiation bursts was under construction. T h e time spectrum of the primary X-ray laser radiation had a discrete character. T h e time spectrum of the primary X-ray
266 / x-ray. Photons/beam 1.2 x 10 8 0.8 x 1 0 8 0.4 x 1 0
8
IL
0 /(mA) 200 0 / (el.beamsi electrons/beam
f
(a)
r
1.2 x 1 0 8 0.8 x 10 8 0.4 x 10 8 0
!l
el.beams; electrons/beam
1.2x108 0.8 x 10 8 0.4 x 10 8 0 A t = 200 us
HP+-
?(us) Figure 12. The typical oscillograms of bursts from (a) primary (X-ray laser beams from cathode) and secondary penetration radiation beams (fast electrons) in the discharge for different kind of target materials. The cathode sample is Ta, D2; current, 180 mA. Assembly is by Fig. 2b (target arrange at a distance of 70cm from cathode), (a) primary penetration radiation from cathode, (b) Al target of 1.4-mm thickness, (c) Yb target of 1.8-mm thickness. Pulse peaks are selected via a discriminator amplifier.
was a function of the cathode material. Separate bursts were recorded within 85 ms after turning off the current. The time spectrum of the secondary radiation also had a discrete character, but the type of this spectrum was a function of the target material. Also this secondary radiation is registered using the X-ray film arranged behind the lead shield (Fig. 13). A third type of the penetrating radiation was observed as well. This was radiation recorded directly by the photomultiplier placed behind of the target without the scintillator (Fig. 14). In this scheme, the target was arranged between the shield with the thickness of 3 mm made of plastic and the PM detector. The type of the secondary radiation was defined by the detector material. This emission began 20min after turning on glow discharge current and emitted after turning off the discharge current of 20min and more (Fig. 14). An abnormal high penetrating ability of this radiation type requires additional research. 4. Discussion The features of the X-rays recorded in these experiments are as follows: • The X-rays leaves the solid-state medium of the cathode material.
267
Figure 13. The X-ray film exposed by the secondary penetration radiation from the lead screen with the thickness of 2 mm. The system M0-D2, current 220 mA, the exposure time - 720 s. 1, X-ray from cathode; 2, 15 /jm Al shield; 3, 2 mm lead target; 4, X-ray film; 5, area of X-ray film behind lead shield, it is the photoemulsion solarization presumably; 6, area of X-ray film behind 15 jjira Al shield only. The image is negative.
• The intensity of the X-rays increases 5-6 times when increasing the discharge voltage by 1.3-1.4 times. • The quantity of the X-rays energy is essentially not changed in this case. • The X-rays emission occurs within 100 ms after turning off the discharge current. The obtained results are the direct experimental proof of existing the excited metastable energy levels with the energy of 1.5-2.5 keV in the solid of the cathode sample. Presumably, these excited metastable levels are formed in the volume of separate crystallites. These excited metastable levels exist for the time of AT mst (up to 100ms and more). Then the relaxation depopulation of these levels takes D, mGy/s (dose rate)
0 «4* H + •
A
a ? 1
0.01
400
t (s)
20 |im Mo target 30 urn Ni 35 urn W 10nmTa 25 |im Zr 50 urn Nb 100 urn Al
800
(after GD switch off)
Figure 14. The third type secondary penetration radiation dose rate dependence upon the time after turning off the discharge current. The cathode sample is Ta, D2; current, 100mA; voltage, 2000 V. 1, 15/im Be foil shield; 2, scintillator; 3, X-ray targets made of foil of various materials; 4, photomultiplier.
268
place, being accompanied with the emission of the X-rays and fast electrons. These beams generation occurs from the solid-state cathode medium presumably for one passing in the mode of super luminance. In this case the duration of the beams should be of K r n - 1 0 - 1 3 s . Understanding the mechanism of these level of formation will require additional research. T h e existence of one of the two physical phenomena can be assumed: (1) Excitation of the interior L, M electronic shells without ionization of the outer electrons. (2) Vibrational deformation of the electron-nuclear system of the solid ions. T h e core of electronic shells is displaced relative to a nucleus with forming a dipole (an optical polar phonon). T h e frequency of the formed phonon is much greater t h a n the plasma frequency in a metal.
5.
Conclusion
Experimental research into this fundamental phenomenon has allowed us to create what is essentially a new type of device: the X-ray solid-state laser with a wave length of the radiation of 0.6-0.8nm, duration of separate pulses of 1 0 _ 1 1 - 1 0 _ 1 3 s and beam power in pulses up to 10 7 W. T h e results show t h a t creating optically active medium with long-living metastable levels with the energy of 1-3 keV and more is possible in the solid state.
References 1. A.B Karabut, Research into powerful solid X-ray laser (wave length is 0.8-1.2 nm) with excitation of high current glow discharge ions, in Proceedings of the 11th International Conference on Emerging Nuclear Energy Systems (Albuquerque, New Mexico, USA, 29 September-4 October 2002), pp. 374-381. 2. R.B. Firestone, Table of Isotopes, Eighth Edition, Vol. 2, Appendix G-1 (Wiley, New York, 1996). 3. R.C. Elton, X-ray Lasers (Academic Press, New York, 1990).
C H A R G E D PARTICLES FROM Ti A N D Pd FOILS
LUDWIK KOWALSKI Montclair State University, Upper Montclair, NJ, USA STEVEN E. JONES Brigham Young University, Provo, UT, USA DENNIS LETTS 12015 Ladrido Ln, Austin, TX, USA DENNIS CRAVENS Cloudcroft, NM 88317, USA
After familiarizing himself with the use of CR-39 detectors, about a year ago, the first author asked Steven Jones to send him a TiDj; foil, similar to that described at the Tenth International Conference on Cold Fusion.1 It was an attempt to detect 3MeV protons with the CR-39 chips. The idea was to develop an experiment suitable for student-oriented cold fusion projects. That is how the first author became a cold fusion researcher. After receiving the foil he sandwiched it between two CR-39 detectors for the period of 55 days. The area of each detector was one square inch. The exposure started 3 days after the sample was prepared (by keeping the titanium foil in deuterium gas at high temperature and pressure). The number of tracks counted on the face of the CR-39 detector that was applied to Jones' foil turned out to be 225. The opposite side of the same CR-39 detector (exposed to air) was used to count tracks due to our background. The number of background tracks turned out to be 132. Such results, if generated by a Geiger counter, for example, could be used as evidence of charged nuclear particles being emitted from the foil. The difference 225 — 132 = 93 is 4.9 times larger that the standard deviation of 18.9 (calculated as the square root of the sum of 225 and 132). A Montclair State University student, Marcee Martinez, was then asked to count the tracks again. First she "trained her eyes" by observing a CR-39 chip with tracks from alpha particles. Then she started counting "similar tracks." Her result was 165 for the signal and 124 for the background. This time the difference, 41, is 2.4 times larger than the standard deviation. Are conventional standard deviations, 19 and 17 (as above), appropriate indicators of uncertainty? They are probably not. A human being counting tracks must 269
270
frequently decide to either count or not to count a particular track-looking spot. The uncertainty associated with counting, the error of rejection, must be added to conventional standard deviation. The conventional standard deviation becomes negligible when the number of counts becomes very large but the error of rejection remains a constant fraction of the total number of counts. Suppose the counting situation is such that hesitation happens in 10% of cases and that the total number of counts is 900. In that case the error of rejection is probably close to 45 (5% of all counts). The conventional standard deviation (the square root of 900) is 30 and the sum becomes 75. The result should be reported as 900 ± 75, rather than as 900 ± 30. Richard Oriani 2 found a way to practically eliminate the error of rejection. But his method is more labor-intensive than the method we used. Instead of two detectors, one for the signal and one for the noise (background), as we did, he uses the same detector for both. This is accomplished by etching a single detector twice: before the experiment and after the experiment. After the first etching the surface is photographed through a microscope, field by field. In that way the preexisting background is recorded. The second etching takes place after the experiment and the same fields are photographed again. Then the photos are compared, again field-by-field. Only tracks that appeared after the experiment are counted. By his method the net signal of 132, e.g., would indeed be much more convincing. Fortunately, this was not a problem to worry about in another project involving track detectors. That project resulted from correspondence with Dennis Letts. He has a team of scientists investigating excess heat produced in electrolytic cells. Knowing about their apparent electrolyte boil-off,3 the first author asked for a chance to look at a possible "nuclear signature." Three palladium cathodes: Pd613, Pd-616, and Pd-615 were sent to the first author and he exposed them to the CR-39 detectors. The technique was the same as for the TiD x foils; the cathodes were sandwiched between pairs of detectors for several weeks, detectors were etched, and tracks were counted, under the microscope. The results were: (a) about 500,000 tracks on the two detectors sandwiching Pd-613, (b) about 11,000 tracks on two detectors sandwiching Pd-616, and (c) no tracks above the background for the Pd-615 cathode. These numbers are rough estimates, errors by the factor of two, or so, are not important in this particular context. Only then was the first author informed that the Pd-613 generated an unusually high amount of excess heat, the Pd-616 generated much less excess heat, and Pd-615 generated no excess heat at all. He was also informed that all three cathodes were cut from the same sheet of pure palladium and that the electrolyte used in the cells was prepared at the same time and kept in a container. The only difference was that several drops of an additive, labeled "sauce," were added to the electrolyte in which the Pd-613 cathode was used. That additive was known to contain a tiny amount of uranium (Fig. 1). After learning about this the first author asked for a sample of this sauce. Several drops of it were placed on a sheet of plastic and dried under a lamp to produce a
271
Figure 1. The photograph taken through a microscope, shows tracks over the area of the detector equal to 1.30 X 1.00 m m 2 .
layer of a dark residual. The CR-39 was at once deposited over that residual. At the same time another CR-39 was applied to the most active side of the Pd-613 cathode. Three weeks later the detectors were removed. They immediately revealed a large number of tracks. In fact the maximum track density at the cluster from the Pd-613 was essentially the same as three weeks earlier. These facts are consistent with the idea that excessive tracks were due to the contamination of the electrolyte to which the "sauce" was added. The very large difference between track densities from Pd616 and Pd-615, on the other hand, could not be blamed on contaminations because m these cases the electrolyte (and other materials) were exactly the same. The Pd616 produced excess heat and generated nuclear tracks; the Pd-615 did not produce excess heat and it did not generate nuclear tracks, above the natural background level (Fig. 2). Nuclear Signature Seems to be Real: It is important to emphasize that the "contaminating sauce" was not added to the electrolyte in which the other two cathodes (Pd-616 and Pd-615) were used. And yet the number of tracks due to the Pd-616, roughly 11,000, was found to be about 100 times higher than the number of tracks due to the Pd-615. This indicates that nuclear particles were detected at the surface of the Pd-616 cathode, long after the electrolysis. A skeptic might suspect that another alpha-radioactive contaminant (not the "sauce") might have been accidentally added to the electrolyte in which the Pd-616 cathode was used. If this were the case then both surfaces of the Pd-616 cathode would produce about the same number of tracks. In reality one side of the Pd-616 produced 8000 tracks while the other side produced 3000 tracks. How can this be explained? The electrolytic
272
Figure 2. The photograph through a microscope, shows tracks over the area of the detector equal to 0.25 X 0.19mm 2 .
cell was essentially mirror-like symmetric (a small cathode near the center and a spiral platinum anode, parallel to the walls of the beaker). Furthermore, clustering of tracks was discovered on the more active surface of the Pd-616 cathode. The tracks due to the Pd-613 cathode, by the way, were also distributed very unequally. One side produced nearly 500,000 tracks while another side produced only about 4000 tracks. Most of the 500,000 tracks were found in a cluster whose area was only a small fraction of the cathode area (see Fig. 2). It is difficult to explain strong clustering in terms of the contamination of the electrolyte. A more natural explanation is to assume that a very high concentration of tracks in a small area (about 2 or 3 mm) coincided with the spot at which heat was generated during the experiment. A tentative conclusion is that uranium contamination, in the case of Pd-613, was responsible for only a small fraction of what was actually observed. The first author agrees with the second author that excess heat demonstrations, designed to convince that something highly unusual (cold fusion) is taking place, should always be accompanied by attempts to display nuclear signatures. After all, there are many non-nuclear ways to generate excess heat, especially at the power level below one watt. A complete examination of all chemical processes taking place in a setup (to rule out chemical origin of excess heat) is much more demanding than using a nuclear detector of some kind. Cold fusion effects, if they are nuclear, must generate nuclear reaction products, either radioactive or stable. On May 2005 Ludwik Kowalski sent an e-mail message to Dennis Letts. He wrote: "I am going to galley proof our ICCFll presentation in Marseilles. This puts me in an awkward situation. If I were reporting on my own work I would add a short paragraphs, something like this: 'No additional experiments were conducted
273
to confirm observations reported 6 months ago. T h e unexpected delay is due to . . . ' B u t in this case I was only a messenger; you are real players. A reader is likely to be interested in the current status of our investigation. I think t h a t it is not right to report positive results only and keep negative results hidden. Do you agree? . . . " T h e following reply was received several hours later. "No additional experiments were conducted to confirm observations reported 6 months ago. T h e unexpected delay is due to the fact t h a t experiments seldom work on a schedule. The MOAC had to be modified slightly to re-store design stability and precision. Also, we have not observed laser-triggered excess power since August 2003. Of course I agree [with your last statement] - since changing metals at the end of 2004, my success rate has been zero. This is compared to a success rate of 87% during the years of 2000-2004. Other t h a n changing Palladium stock, I don't know what has caused the sudden loss of the laser effect. Experiments have been conducted in a high quality calorimeter (MOAC), in a moderate quality calorimeter (my Avanti) and on the open bench. T h e laser effect has not re-appeared under any of the above calorimetric conditions. Experiments are being conducted now to re-establish the laser effect or to explain why it stopped working. You may use this information in any way you wish, including an addendum. W i t h regard to reporting negative results, consider this: Cravens and Letts discovered the laser effect in September 2000 and reported the positive results publicly in August 2003. We spent 3 years testing the credibility of our result before reporting publicly. We anticipate behaving in a consistent manner now - we have negative results b u t we're not in a rush to report until we're sure t h a t we have negative results and t r y to provide some reasons why the results are negative. I believe t h a t reporting results formally by 2007 will be consistent with our previous work and should not be considered 'keeping negative results hidden'." References 1. S.E. Jones et al., Charged-particle emissions from metal deuterides, in Proceedings of the 10th International Conference on Cold Fusion, 2003 (Cambridge, MA, USA). This paper can be downloaded from the library at http://www.lenr-canr.org. 2. R.A. Oriani and J.C. Fisher, Energetic charged particles produced in the gas phase by electrolysis, in Proceedings of the 10th International Conference on Cold Fusion, 2003 (Cambridge, MA, USA). This paper can be downloaded from the library at http://www.lenr-canr.org. 3. D. Letts and D. Cravens, Laser stimulation of deuterated palladium: past and present, in Proceedings of the 10th International Conference on Cold Fusion, 2003 (Cambridge, MA, USA). This paper can be downloaded from the library at http://www.lenrcanr.org.
CR-39 TRACK D E T E C T O R S IN COLD F U S I O N E X P E R I M E N T S : REVIEW A N D PERSPECTIVES
A. S. ROUSSETSKI P. N. Lebedev Physical Institute, Russian Academy of Sciences E-mail: [email protected]
1. Introduction Earlier experiments 1,2 have showed emissions of DD-reaction products (3-MeV protons) and energetic charged particle emission (a-particles) during exothermic D(H) desorption from the Pd/PdO:D(H) heterostructures. The occurrence of these emissions was confirmed by independent experiments using both Si-surface barrier and CR-39 plastic track detectors. 3 ' 4 Over the last few years, the CR-39 track detector has become a popular method to measure charged particle emissions in cold fusion experiments. The use of CR-39 is quite simple and cheap, but this technique demands some special conditions. As shown below, the observance of these conditions allows the researcher to not only detect charged particles, but also to identify their types and estimate their energy spectrum. On the other hand, when these conditions are not met, the method can fail, mainly because of problems with radioactive nuclides contained in the surrounding materials (electrolyte, air, cathode, etc.), mechanical defects, and the development process after etching. The necessary conditions for correct CR-39 measurement include the following: - purification of CR-39 detector surface, - low density of background tracks before measurements, and protection of CR-39 from external radioactive contamination, - correct calibration procedure, - control of background during the measurement and the use of "clean" materials (without radioactive nuclides), - protection of detector surface from mechanical and thermal influences, high intensity UV radiation, - in some tests, shielding foils with known stopping ranges identify particle types, - correct etching conditions in each measurement. Access to purified track detectors along with knowledge of track characteristics produced by various types of particle allow the use of CR-39 chips in long-duration experimental exposure during and after electrolysis with Pd and Ti cathodes. We 274
275
used purified CR-39 detectors produced by Landauer Inc. (USA) and Fucuvi Chemical Industry Co. (Japan) with very low-background track density (N^ < 20cm - 2 ) to detect the emissions with very low intensity (10~ 4 —10 -3 c m - 2 s _ 1 ). 2. CR-39 Track Detector CR-39 is a polymer (Ci2H 18 0y) with a density of ~1.3g/cm3. When a charged particle crosses the detector surface it causes radiation damage along trajectory. This zone of structure damage may be increased to 10~ 4 — 10~2 cm by etching in a chemical reagent. We used optimal etching conditions for CR-39 detector: 6N solution NaOH at 70°C over 7h. V = V T / V B = f{dE/dx) is the etch rate ratio (where dE/dx is the stopping power of particle, Vrand VB is the track and bulk etch rates). A track is formed if VT > VB. If VB = VT, dE/dx = (dE/dx)s is the threshold stopping power. The critical angle of detection 6C is determined as the minimal angle between the particle trajectory and detector surface when track formation is still possible: 8C = arc sh^Ve/Vr). It is easy to shown that if detector crossed by particles in different directions the detection efficiency is determined as rj = 0.5 * (1 — sin# c ). 3. Experimental Technique The measurements were carried out using PAVICOM4 - a completely automated device for track detector processing. It consists of an optical microscope with a digital video camera; a sample holder stand with three-dimensional displacement provided by stepper motors with accuracy of 0.25 /mi; manual controls; and a personal computer for automatic measurements. We used a-sources and a cyclotron alpha beam (Ea = 2-30 MeV) to calibrate the CR-39. Figure 1 shows the photomicrograph of tracks from a-particle cyclotron beam (Ea = HMeV) normally incident on CR-39 detector. For proton calibration we used a Van de Graaf accelerator (Ep = 0.6-3.0 MeV). The results of the calibration - the dependence of track diameter from particle energy - are presented in Fig. 2 for a-particles, and Fig. 3 for protons. We used the following types of samples in our experiments. Electrochemically loaded Au/Pd/PdO:D x heterostructures were used for charged particle emission during deuterium desorption after electrolysis. Ti (30 /mi), Pd (30 /mi) cold worked foils and Pd/PdO heterostructures (50 and 100 /mi) were used for in situ measurements during electrolysis in a solution of 1M L12SO4/H2O (current density j = lOmA/cm 2 ). Pd (30 (an) and Pd/PdO (50/mi) samples with He implanted on
276
Figure 1. Tracks from o-partjcle cyclotron beam detector. Image size - 120 X 90 /im.
I 1 MoV) normally incident on CR-39
(/•;„
the surface 2 x 10 17 and 2 x 1016 at./cm 2 , respectively, were used to investigate the influence of He impurities on alpha-particle emission during electrolysis. The example of long duration background measurements with a 0.1 M Li2S04 solution is presented in Fig. 4. The main part of background tracks spaced in the range of diameters 8-12 fim. We can estimate the mean level of background a-emission as (fib) = 2.7 x 1 0 _ 4 s _ 1 c m - 2 .
Alpha calibration curves for Fukuvi and Landauer CR-39 detectors 13 12 11 10 — Fukuvi - Landauer
9 8
'U-
7 6 5
10
Figure 2.
15 20 E a (MeV)
25
30
Alpha-sources and cyclotron alpha.
277
Prolon calibration curves (or Land tier and Fukuvi CR-39 detectors 9
1
I
1
8.5 8 7.5 7 6.5 6 5.5 5 4.5 05
•V 1
1.5
2
- Landauer CR-39 •
2.5
3
Fukuvi CR-39
3 .5
Ep(MeV)
Figure 3. Proton calibration with Van de Graaf beam calibration (2-30 MeV) of CR-39. Accelerator (0.6-3.0 MeV).
4. R e s u l t s and Discussion The measurements with Pd/PdO (50/tm) sample after electrolysis showed that hifi.li energy charged particle emission lake place not only on the whole sample surface, but also it can concentrate in some small zones ("hot zones") with dimensions of a few hundred microns corresponding to places with maximum internal strains. The photomicrographs of "hot zone" (250 x 500//in 2 ) with ~10 3 tracks of a-particles and protons are showed in Fig. 5a,b. The distribution of track diameters for particles normally incident to the detector is showed in Fig. (i. We can see three peaks that corresponded to following particles and energies: d = G.O
Open CR-39 background, f = 335 h Open CR-39 background. (= 216 h Open CR-39 background. (= 118 h
10 Track diameter (um)
Figure 4.
I MIL 11
12
Example of background during electrolysis in 0.1 M L12SO4.
278
(n)
(b)
Figure 5. CR-39 measurement after electrolysis of P d / P d O i H ^ (50jitm). Shielding of CR-39 11 /im of Al. Photomicrographs of "hot zone" (250 X 500 /jm 2 ) with tracks of a-particles and protons. Image size — 120 X 90 fim.
6.5/xm (Ep = 1.4-1.7MeV), d = 7.0-7.6/xm (Ea = 9.2-14.0MeV), d = 7.8-8.6/xm (Ep = 5.6-7.8 MeV). The distribution of track diameters for the entire detector surface (not just in the "hot zone") is presented in Fig. 7. We observe the same peaks in this distribution. This means that the charged particle emission in the "hot zone" is the same as the rest of the sample, but the emissions are concentrated in space (and, possible, in time). We estimated the mean intensity of charged particle emission (protons and a-particles, without "hot zone") during all time of exposition (5h) as (n) = 6 x 10~ 2 s" 1 c m - 2 . a-Particles emitted from one point on the sample surface. We observed such events both after electrolysis and during long duration electrolysis measurements. Examples of these events with Au/Pd/PdOiD^, (40 /iin) and PdHe
I H Pd/PdO:Hx, S = 250 x 500 (im, CR-39/5.0 Jim Al Exothermic H-desorption Burst of emissions (photo)]
20T J
18-'
1614-
6.5
Figure 6.
7.0 7.5 8.0 Track diameter (fim)
9.0
Distribution of track diameters in.
279
|Pd(bgr)CR-39.open,l = 48h I Pd/PdO:Hx(lg). CR-30. open, r= 5.0 h I (Pd/PdO:Hx(lg) - Pd(bgr))
30
25
•f 20
I
& g
15
*
10-
6.0
6.5
7.0
J
7.5
3.0
8.5
9.0
Track diameter (urn) Figure 7. D i s t r i b u t i o n of track d i a m e t e r s on "hot zone" (250 X 5 0 0 / / i n 2 ) C R - 3 9 surface w i t h o u t "hot zone".
(30/nn. 2 x 1 0 , 7 a t . H e / c m 2 ) samples are presented in Figs. 8 a n d 9, respectively. In these cases we can t o estimate the energy of emitted a-particles, measuring their ranges from the point of emission to the end of tracks. Taking into account the thickness of detector shielding (50 and 6 0 / m i P E , respectively) and etched layer of CR-39 ( ~ 9 / m i ) . we can t o estimate the energies of emitted a-particles: EQi = En2 = 11.2 MeV; Ea3 = Eo4 = 9 M e V ; Ea5 = Ea6 = 8.3 MeV; Ea7 = lOMeV (see Fig. 8) a n d Eai = 9.2 MeV: Ea2 = 8.6 MeV; Ea3 = 9 MeV; Ea4 = Ea5 = Ea6 = 8.4 MeV (see Fig. 9). T h e energies of all these a-particles are more t h a n energies of n a t u r a l background and they can be identified as long range particles emitted from the sample surface under high internal strains. These events d e m o n s t r a t e the release of few tens MeV of energy concentrated in small volume of sample. If we suppose t h a t the energy concentrated in the region compared with dimension of the lattice, and released in a time period of 1 0 - 1 2 ~ 1 0 - 1 4 s , we get the power ~ 1 0 1 8 - 1 0 2 0 W / c m 2 .
5. C o n c l u s i o n (1) We formulated the necessary conditions for successful using of CR-39 detector in typical (•<']
280
Figure 8. CR-39 measurements after electrolysis of Au/Pd/PdOiDa;. Shielding of CR-39-50jtjm of P E . Image size - 240 x 180 fim. Seven a-particle emissions from one point on the sample surface.
Figure 9. CR-39 measurements during electrolysis of PdHe (30(im thick, 2 X 10 1 7 He/cm 2 ) in 1M L i 2 S 0 4 (j = 4 - 4 0 m A / c m 2 ) . Shielding of CR-39 - 60/im of PE. Image size - 120 X 90/urn. Six a-particle emissions from one point on the sample surface. d i m e n s i o n s of l a t t i c e . T h e s e i n d i c a t e t h e p o w e r d e n s i t y ~ 1 0 1 8 — 1 0 2 0 W / c m 2 , which
is
comparable
to
the
power
density
of
intensive
picosecond
laser emission.
References 1. A . G . Lipson et al, Fusion Technol. 3 8 , 238 (2000). 2. A . G . Lipson, B . F . Lyakhov, a n d A.S. Roussetski. In Proceedings of the ICCF-8, Ital. Phys. Soc. Conf. Proc. 7 0 (2001) 231. 3. A . G . Lipson, A.S. Roussetski, et al., Bulletin of the Lebedev Physics Institute Russian Academy of Sciences. 1 0 , 22 (2001). 4. A.G. Lipson, A.S. Roussetski, C.H. C a s t a n o , a n d J. Miley, Bull. Am. Phys. Soc. 4 7 , 1219 (2002). 5. A . B . Aleksandrov et al, Nucl. Instr. Meth. A 5 3 5 542-545 (2004).
E N E R G E T I C PARTICLE SHOWER IN T H E V A P O R FROM ELECTROLYSIS
R.A. O R I A N I University
of Minnesota, Minneapolis, MN 55419, E-mail: orianOOl @umn. edu
USA
J.C. FISHER 600 Arbol Verde, Carpinteria, CA 93013, E-mail: [email protected]
USA
Approximately 40,000 energetic charged particles were recorded in a pair of plastic detector chips suspended in the vapor over an active electrolysis cell. Particle track locations and orientations were revealed by examining the etch pits produced by chemical etching. Analysis of track orientations indicates that the shower originated in a compact source in the vapor between the chips. The total magnitude of the shower is estimated to have been 150,000 particles and its duration is estimated to have been a few seconds. A previously unknown type of nuclear reaction is indicated.
1. Introduction For over a decade, beginning with Fleischmann and Pons, 1 there have been claims of unusual experimental results suggesting room temperature nuclear reactions of a new kind. They include generation of excess energy above input energy during electrolysis, production of helium and tritium, generation of energetic charged particles, transmutation, and other essentially nuclear phenomena. The bibliographies prepared by Storms 2,3 provide overviews of this work. The nuclear claims have not been generally accepted by the physics community. Yet research in this area continues, directed to finding and demonstrating results of sufficient magnitude and clarity that skepticism can be overcome. Because energetic charged particle phenomena are among the clearest indicators of nuclear processes, we have concentrated our efforts in this direction. Using CR-39 plastic detectors in electrolysis experiments we have observed particle tracks consistent with energetic alphas. Initially, we immersed the detectors in the electrolyte. 4,5 We observed an excess of particle tracks over those in control chips similarly exposed without active electrolysis. Our results were variable with an overlap between the track densities observed for active chips and for control chips, but after many repetitions of the experiment statistical analysis showed a highly significant correlation between active electrolysis and energetic particle generation. Although these results were convincing to us they still left room for doubt by the larger community. 281
282
We next supported detector chips in the vapor above the electrolyte. In most experimental runs we obtained densities of tracks that exceeded the background of incidental radon tracks by an average factor of about three. 6 But in five runs we found the remarkable result of a factor of a hundred above background. One such shower originated in the vapor between a pair of chips and generated tens of thousands of recorded tracks. Describing and interpreting these tracks is the subject of this paper. 2. Experimental Procedure The experimental setup is identical with that employed in earlier experiments 4 ' 5 except that the detector chips were suspended in the vapor above the electrolyte. The electrolysis cell is an open-ended vertical glass cylinder 10 cm long and 1.6 cm inside diameter with a sheet of palladium clamped to the lower end and sealed by O-rings. The palladium serves as cathode. The upper end of the cell is partially closed by a stopper and the cell is partially filled with an electrolyte having an initial composition of 2.3 g Li2S04 per 100 cm 3 H2O. A 2-mm diameter titanium rod supported by the stopper bears two pairs of 0.1-mm diameter hooks on which CR-39 detector chips are suspended. A platinum wire spot-welded to the rod ends in a horizontal pancake spiral that serves as the anode. A nickel disc that nearly fills the cross-section of the cell is supported by the rod above the surface of the electrolyte. It serves to mitigate carry-over of mist from the electrolyte to the detector chips suspended above it. It also blocks charged particles originating in the electrolyte from impinging upon the detector chips. In the experiment here described two pairs of chips were hung edge down, members of each pair being roughly parallel to each other and about 8 mm apart. Electrolysis was conducted for three days during which time the detector chips were surrounded by O2 + H2 vapor. Energetic particles that entered the chips from the vapor produced latent tracks of internal damage along their trajectories. After electrolysis the chips were etched in 6.5 N KOH for approximately 20 h at 60°C. The etching process attacks damaged material along latent tracks more rapidly than it attacks undamaaged material, generating pits that mark the intersections of particle tracks with the surface of the chip. 3. Track Numbers and Orientations Here, we analyze the pattern of tracks from a shower in the vapor between a pair of detector chips. We begin with the chip having the higher track density. After etching to develop latent tracks, the side that was exposed to the shower was photographed in a mosaic of 270 photographs. A representative photograph is reproduced in Fig. 1. From these photographs a montage of 1044 rectangular images (4:3 ratio of sides) was obtained by subdividing each photograph into four equal images and discarding those few images that extended beyond the edges of the chip. Etch pits were counted in each area where counting was possible. Counting
283
was not possible where the chip had a hole for its support wire, had identification numerals laser-inscribed by the manufacturer, or in four images that had damage of unknown cause. Images that could not be completely counted were retained if more than half of the image was available. Their count numbers were adjusted upward assuming an equal density for the missing part of the image as for the measured part. Overall about 90% of the chip surface was counted.
°
O
«°
/"
cP c % 3
°
o
°.00"Q
Figure 1. Etch pits on the surface of a CR.-M9 plastic detector chip .suspended in the vapor over an active electrolysis cell. Each pit marks the location of a track of damaged material where a charged particle has penetrated the chip. A roughly conical pit has developed during etching because the etchant attacks the damaged material of the track more rapidly than it attacks the adjacent undamaged material. The area shown measures approximately 0.29 mm X 0.22 mm. The mean diameters of the darker circular pits are approximately 24 /an.
We counted 29,800 etch pits in the portion of the chip available for counting, and estimate by interpolation that another 3300 particles passed undetected into unavailable areas, giving a total of 33,100 charged particles impinging upon or passing through the 1044 images. By analyzing the shadow cast by the support hook we estimate that an additional 240 particles were stopped by the wire and did not reach the detector chip. Adding these the final total is about 33,300 charged particles impinging on the area of 1044 images.
284 A
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Figure 2. Distribution of etch pits on the surfaces of CR-39 plastic detector chips suspended in the vapor over an active electrolysis cell. (A) The more heavily pitted chip. Density in pits per image is indicated by the color scale for a mosaic of 1044 images that span the approximately 8-mm 2 surface. Outlined images could not be counted and etch pit densities were interpolated for them; those in the upper portion of the chip correspond to the support hole and those in the lower portion correspond to laser-inscribed identification numbers. The solid contour lines are spaced at 10 pits/image and range from 10 pits/image along the right side to 110 pits/image near the peak. The dashed contour line denotes 3 pits/image. Arrows indicate mean orientations of tracks having elliptical etch pits. Arrow lengths are proportional to the mean cosines of the angles between individual track projections on the surface of the chip and the corresponding arrow orientation. (B) The facing chip at a distance of about 8 mm. A 2 mm supporting rod ran vertically between the detectors. The smoothed contour lines are spaced at 3 pits/image and range from 3 pits/image on the left to 30 pits/image at the peak. The area of low etch pit density over much of the detector lies in the shadow of the supporting rod. It indicates that the shower originated in a small volume close to and nearly behind the support rod. The edge of the shadow is not parallel to the edge of the detector chip, suggesting that the chip was canted with respect to the rod or that the active volume moved sideways as it rose.
A smoothed contour plot of the density of etch pits is shown in Fig. 2A. The units are etch pits per image. (Because the area of an image is about 6.3(10)~4 cm2 one must multiply by 1600 to obtain etch pits per cm 2 .) The solid contour lines are spaced at 10 pits/image and range from 10 pits/image along the right side to a maximum of 110 pits/image near the lower left corner of the chip. From its maximum the density of pits falls to below 10 pits/image near the right side of the chip, reaching a level of 3 pits/image at the dashed contour line. This is the etch pit density we customarily find in chips exposed to the vapor in experiments where we do not see a massive shower such as the one under discussion. The dashed contour line thus marks a boundary beyond which no shower particles left tracks capable of producing pits upon etching. In addition to its prominent position along the right side of the chip this boundary comes close to the lower left corner of the chip. (The image at the lower left corner of the chip contains 10 pits. The 10 pits/image contour line should pass through it, although this is not shown in the figure because the
285
contour algorithm requires more than a single data point to determine a contour segment. The gradient of pit density suggests that the 3 pits/image contour line then lies just beyond the corner of the chip.) Also shown in Fig. 2A is an indication of the directions of the tracks near the perimeter of the densely pitted area. Track orientations can be determined from the shapes of the etch pits as described more fully below. Eight areas were selected around the perimeter and one near the center of the chip, each consisting of four contiguous images. Within each such area the orientations were determined for those etch pits for which a clear measurement was possible. Where necessary the microscope was focused at several levels from the surface into the interior of the plastic to aid the determination. Each pit with a measured orientation was assigned a unit vector in the direction of the track as seen in its projection on the surface of the chip. These vectors were added to obtain the mean track direction, and the cosine of the angle between each constituent vector and the mean track orientation was determined. The mean cosine provides a measure of the extent to which the vectors are aligned. When the mean cosine is near unity the constituent vectors must be nearly parallel. When the mean is near zero the constituent vectors must tend to point equally in opposite directions. The arrows in Fig. 2 indicate the mean orientation of the tracks in each area, and their lengths are proportional to the mean cosines of the track projections along these directions. Clockwise beginning at the lower left corner the mean cosines and (in parentheses) the numbers of tracks from which they were determined, are 0.956(35), 0.387(43), 0.726(30), 0.453(49), 0.686(20), 0.925(30), 0.838(20), 0.798(72); and for the central arrow they are 0.331(58). We see that in the lower left corner of the chip, and along the lower contour lines on the right side, the tracks are strongly aligned pointing away from the central region of high track density. On other parts of the perimeter the tracks also tend to align pointing away from the central region but with more scatter as indicated by the smaller values of mean cosine. It is clear that the tracks originated somewhere in the vapor above the densely pitted surface of the chip. But they cannot have arisen from a stationary source because the extended region of high track density does not have rotational symmetry. Working back from the boundary determined by the dashed contour line, we can obtain a rough idea of the height of the particle source above the surface of the chip. During etching a roughly conical pit develops because the etchant attacks the damaged material of the track more rapidly than undamaged material. Etching causes the vertex of the cone to move into the plastic more rapidly than it causes the surface to recede. The vertex points in the direction that the energetic charged particle traveled as it entered the plastic. The axis of the cone coincides with the track of travel and the shape of the etch pit depends on the orientation of the axis and on the half-angle of the cone. When the axis is nearly perpendicular to the surface the intersection of the etch pit with the surface is nearly circular. It becomes increasingly elliptical as the orientation of the axis tilts away from the perpendicular.
286
Now consider the etching process when the damage trail makes only a small angle with the surface of the chip. Consider a spot on the damage trail inside the chip. This spot lies closer to the surface than to the beginning of the damage trail where the particle entered the plastic. As the etching process proceeds the surface of the chip etches toward the spot at a steady rate. Etching proceeds along the damage trail at a faster rate but it has farther to go. At a critical angle, equal to the half-angle of the cone, the surface and the apex of the cone reach the spot at the same time. For damage trails with angles smaller than the critical value relative to the surface of the chip the surface gets there first and no etch pits can form. All shower particles must have been generated near enough to the chip that none of them left an etchable track beyond the dashed boundary in Fig. 2A. This implies that beyond the boundary none of them made an angle as large as the cone half-angle with the chip surface. Measurement and analysis of cone angles indicates a half-angle of about 19° as described below, so we can deduce that all particles were generated below a sloping surface that rises from the boundary at a slant angle of 19° in the direction opposed to the arrows in the lower left corner and along the right side of the chip. The tent-like roof suggested by these rafters reaches a height of about 1 mm from the chip surface in the neighborhood of the peak, indicating that the source of energetic particle generation did not extend above this level. It reaches a height of about 3 mm near the upper edge of the chip suggesting that the particle source moved away from the chip or grew in diameter as it progressed upward toward and past the support hole. We envision an active volume having an initial diameter of a fraction of a millimeter that began emitting particles in the vapor about 1 mm from the chip near its lower left corner, just touching the tent-like roof, then moved upward along the chip in a wandering path occasionally touching and defining other portions of the roof along the way. Because the densely populated area extends beyond the dimensions of the chip in some directions, only a rough estimate can be made of the total number of charged particles generated in the shower. We estimate that about 50,000 etch pits would have been counted had the chip been sufficiently extended, and considering that tracks making angles less than 19° with the surface do not produce etch pits we estimate about 150,000 charged particles as the total number in the full 4ir steradians of the shower. The second chip is slightly larger than the first. It was photographed in a mosaic of 285 photographs, from which a montage of 1140 images was obtained by quartering each photograph. Following the same procedure as with the first chip we found that a total of about 10,700 charged particles left etch pits in the detector chip or passed undetected into areas unavailable for counting. A contour plot of the density of etch pits for the second chip is shown in Fig. 2B. A portion of the chip exhibits a maximum in track density roughly opposed to the peak density in Fig. 2A. In this area the variation of track density with position mirrors that in Fig. 2A with track density values that are about one-third as great. The rest of the chip shows a very low level of track density, comparable with the background level in Fig. 2A,
287
that we interpret as lying in the shadow of the 2-mm rod from which the chips were suspended. It appears from the orientation of the boundary of the shadowed region that the chip was hung in a canted orientation with respect to the support rod, or perhaps that the active volume moved sideways as it rose between the detector chips. Because the shower originated in the vapor above a relatively warm electrolyte we expect convection currents that would carry away the vapor near a chip in a matter of seconds. The fact that we observe a somewhat confined and well-defined volume in which the particles originated suggests that the duration of the major part of the shower did not exceed a few seconds. The arrows in Fig. 2A and B provide aggregate measures of the orientations of particle tracks in selected small target areas. Each aggregate includes tracks that produced elliptical etch pits for which track orientations could be determined. Tracks having nearly circular pits, for which no orientations could be established, were necessarily omitted. If we consider a target area directly under a distant source, such that a perpendicular from the source to the plane of the target lies within the target, tracks formed in the target can make only small angles with the perpendicular. The more distant the source the smaller the angles will be and the more nearly circular the etch pits will be. Depending on the size of the source, its distance from the target area, and the ability of microscopic examination to detect small differences from circularity, it can turn out that no orientations at all can be established in a target area directly under the source. In this event orientations can be determined only if the target area lies off to one side of the source. Figure 3 summarizes individual orientations for the six target areas indicated by arrows in Fig. 2B. Tracks in target areas A-C on the left-hand side of the heavily pitted portion of the chip point to the left, away from the heavily pitted area, indicating that the responsible particles came from the direction of the heavily pitted area to their right. For these target areas track orientations were obtainable for an average 62% of all etch pits. The patterns of tracks are quite different in the three targets on the right-hand side of the chip, for which orientations were obtainable for only 27% of etch pits. Tracks in target area F in the lower right are confined to a pair of narrow angular spreads pointing upward and downward. The upward-pointing tracks correspond to a source below the target and the downwardpointing tracks correspond to a source above the target. We interpret these tracks as originating in a compact source that moved upward in the vapor approximately 7 mm distant from the chip at the beginning of its trajectory. Before the source reached a position above the target area the tracks were directed ahead of it in the upward direction. After it had passed the target the tracks were oriented behind it in the downward direction. When the source was directly overhead all tracks were nearly perpendicular to the target, the etch pits were nearly circular and their orientations could not be determined. The track orientations in target area E indicate that the compact source passed nearly over this area as well, but slightly to the right beyond the edge of the chip. The orientations in target area D suggest that the source continued its motion along
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Figure 3. Individual orientations for tracks that produced elliptical etch pits in target areas A - F in Fig. 2B. As described in the text the pattern of tracks in areas D - F indicates that a compact source of energetic particles drifted in the vapor in the general direction from F toward D, passing over and progressively to the right of these target areas.
more or less the same trajectory. In each of the images D-F where there is a clear division into two distinct spreads of orientations, the upward-pointing tracks were generated earlier than the downward-pointing ones. Because the activity of the source had a short lifetime, we expect the number of upward-pointing tracks in each target to exceed the number of downward-pointing ones, reflecting a decline of activity between the times at which the leading and following tracks were formed. The data are consistent with this expectation, recognizing that the compact source first became active near location F leading to a shortfall of upward-pointing tracks at that location from what would be expected had the source become active farther away. The patterns seen in Fig. 3 have counterparts in the data from Fig. 2A, but because the compact source was much closer to the first chip than to the second, the angle subtended by the source as seen from a target area in Fig. 2A was large enough that particles originating from the perimeter of the source produced oriented tracks at a location even when the center of the source was directly over that location. These tracks from a nearby overhead source add clutter to the record of a moving source that otherwise is so clearly evident in Fig. 3 for a more distant source.
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4. Particle Track Analysis Etch pits arise from various causes. Some result from alpha particles from decay of radon in the air or from superficial damage to the plastic detector and others from the energetic particle tracks that are the subjects of this analysis. Track pits initially are conical in shape with the vertex located on the track and the axis of the cone aligned with the track. The conical shape arises because damaged material along a track etches away more rapidly than the surrounding undamaged material. At first the depth and diameter of a pit increase proportionately as etching proceeds, but when the end of the track is reached the etching rate in the track direction slows to that of undamaged material and the point of the cone rounds out. The pit has "bottomed out." The portion of the pit near the surface of the plastic continues for a time to retain its conical shape and its diameter grows at an unchanging rate. Then as the surface of the plastic etches away to the depth of the end of the track the pit completely loses its conical shape and it progressively approaches the shape of a nearly circular dish. Pits from superficial damage bottom out very soon because the damage extends only a short distance into the plastic. They become shallow circular dishes shortly after etching begins. Examination of tracks produced by radon from a pitchblende source indicates that the track lengths for radon alphas are only slightly longer than the depth of plastic that is removed by the etching process. Tracks that are nearly perpendicular to the surface of the detector produce sharp-pointed pits, but tracks that make a modest angle with the perpendicular bottom out because the surface etches down past their far ends. Bottoming out is particularly pronounced when tracks from radon alphas are etched a second time. After the second etch all pits are circular or nearly circular dishes with diameters nearly twice that of single-etched tracks. One such pit is visible at the top of Fig. 1. In order to eliminate background events and to distinguish between families of etch pits, we employ various combinations of the following data restrictions. Let R be the ratio of the major axis to the minor axis of a pit. By imposing the restriction R > 1.1 to remove circular and nearly circular pits we can eliminate most of the pits that arose from sites of superficial damage, and also the pits that were formed in the initial etch and then were etched again after electrolysis. By imposing the restriction i? < 1.5 we retain only those pits whose geometric mean diameter is a good approximation to the diameter of a circular pit of the same energy impinging normal to the chip surface. By imposing a restriction to include only those etch pits that are observed under the microscope to be sharp-pointed cones we retain only pits that have not bottomed out. And conversely by imposing a restriction to exclude pits with sharp-pointed conical shape we retain only pits that have bottomed out. In the following analysis we always apply the restrictions 1.1 < R < 1.5 and we sometimes additionally apply restrictions relating to the presence or absence of sharp-pointed conical pits. We expect that some of the tracks recorded in the shower chips were caused by alpha particles from decay of radon in the laboratory environment. The magnitude
290
of such contamination was explored in a number of control runs in which detector chips were suspended in the vapor over the electrolyte in the absence of electrolysis.6 The chips were etched to reveal pre-existing tracks, and then they were photographed in tagged areas that could be identified later, were mounted in the inactive cell, exposed for three days, removed, etched and photographed again to reveal the tracks associated with influences of the laboratory environment during the initial photography, mounting, exposure, and etching procedures. The densities of etch pits from tracks formed during these procedures amounted on average to 150 ±70pits/cm 2 . In searching for tracks from radon contamination of the shower chips we first photographed, counted, and determined the shapes and mean diameters of all etch pits on the back side of the primary shower chip in Fig. 2A. The back side was shielded by the chip itself from the shower on the front side. The mean etch pit diameters are shown in Fig. 4A. Before applying the restrictions 1.1 < R < 1.5 to remove nearly circular and strongly elliptical pits the peak near 17/on contained about 160pits/cm 2 . This density lies within the range of control densities previously noted. Hence we conclude that the 17/xm pits indicate tracks from radon in the laboratory environment during photography before electrolysis and that they provide a standard for pits on the shower sides of both chips. Measurements of etch pit dimensions on the shower sides of the chips give quite different results. First, we examine the etch pits on the second shower chip in the shadow of the support rod which covers half the area of the chip. Here we expect alphas from radon decay as observed on the back side of the primary shower chip, and possibly other particles from decay of a few long-lived products of the shower reaction that may have drifted to where their decay products could reach the shadow region. Figure 4B shows the size distribution of these etch pits in the shadow region. Two peaks are evident, one near 17/xm corresponding to the peak in Fig. 4A and a new peak with larger etch pits near 24 /im having no counterpart in Fig. 4A. Microscopic examination shows that the larger etch pits have bottomed out near the end of the etching process, but to a lesser extent than the pits that result from double etching of radon alphas. We can analyze the two peaks by considering the three-dimensional shapes of the pits. In Fig. 5, we retain only those pits that are observed not to have bottomed out. Specifically, they must have the shapes of sharp-pointed cones. This restriction removes the family of larger etch pits, and the remaining distributions (Fig. 5A and B) for sharp-pointed conical pits are statistically indistinguishable. Both clearly reflect contamination by alpha particles from radon decay. Next, we turn attention to the family of larger etch pits that have just begun to bottom out. In Fig. 6, we plot distributions of pit sizes where now we retain only those pits that are observed to have bottomed out (i.e. they must not have the shapes of sharp-pointed cones). Figure 6A shows the distribution for pits on the shaded area of the chip in Fig. 2B, and Fig. 6B shows the distribution for pits on the front surface of the primary shower chip in Fig. 2A. These distributions
291
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are statistically indistinguishable, strongly suggesting that the family of larger etch pits identifies tracks of charged particles emitted from precursors whose lifetimes are sufficiently long that a few have drifted into the region between the support rod and the shadowed area of the second shower chip. We now can confirm the 19° value of the half-angle of the shower pits whose trajectories bounded the location of the shower source. From Fig. 5 the mean diameter of the radon alpha tracks in the peaks of the distributions is 17.4 ± 1.0 /xm. From Fig. 6 the mean diameter of the new tracks in the peaks of their distributions is 24.1 ± 1.2 fira. Comparing the diameter of the new tracks to that of radon alpha tracks the ratio is (24.1 ± 1.2)/(17.4 ± 1.0) = 1.4 ± 0.1. Analysis of the etching process leads to a relationship between the half-angle 9 of a conical etch pit, the pit diameter D at the surface of the detector chip, and the depth of etching S of the flat surface, D/S = 2(1— sin 6)/ cos 8. Sharp-pointed conical pits from radon alphas occasionally are found on surfaces perpendicular to the detector chip such as the edges of the chip and the edges of laser-inscribed numerals. The side views of these pits facilitate measurement of cone angles, and suggest a half-angle 9 = 36° for
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Figure 5. Etch pit sizes on the two chip surfaces of Fig. 4, subject to the data cut 1.1 < R < 1.5 as in that figure and additionally restricted to include only sharp-pointed conical pits that have not bottomed out. (A) Back side of the primary shower chip in Fig. 2A. (B) Shadowed area on the front side of the secondary shower chip in Fig. 2B.
radon alphas. Substituting this value of 8 in the equation gives (D/S)iadon = 1.02. Because the new alphas have diameter 1.4 times as great we have (£>/5) new = 1-43 corresponding to 9 = 19°. Particle identities and energies can be determined using methods described by Fleischer et al.7 We first consider the relationship between etch pit half-angle and particle energy for protons and the corresponding relationship for alpha particles. Quantitative relationships for CR-39 plastic were provided by Fleischer.8 The shower particles cannot be protons because there is no energy for which protons produce tracks with 19° half-angles. For alpha particles the energy corresponding to a 19° half-angle is 2.0 MeV, suggesting that the shower particles could be alphas. Energies also can be deduced from measurements of etch pit diameters. Roussetski et al.,9 in support of their research on the emission of charged particles in various systems, have determined etch pit sizes for alphas having a wide range of accurately known energies. Their calibration curve for diameter D corresponding to energy E is well fit by the relationship D35E = constant over the energy range 1.85 < E < 7.19MeV. From this relationship we have E2/Ei = (L>i/D 2 ) 35 .With D2/D1 = 1.4 ± 0.1 this gives E2/Ei = 0.31 ± 0.04 for shower particles interpreted as alphas relative to radon alphas. Radon decays to stable 2 1 0 Pb in a cascade of reactions including three that generate alpha particles: 222 Rn —> 2 1 8 Po + a,
293
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Etch pit sizes on two chip surfaces subject to the cuts 1.1 < R < 1.5 and additionally to exclude sharp-pointed conical pits. The remaining pits have bottomed out. (A) area on the front side of the secondary shower chip in Fig. 2B. (B) Sample of the front the primary shower chip in Fig. 2A.
2 i s P o —„ 2i4p b + ^ a n d 2i4p 0 —> 2 i o p b + a T h e g e a l p n a s h a v e energies 5.5, 6.0, and 7.8 MeV, respectively, and are expected with equal frequency. Taking the mean value E\ = 6.4 MeV we find that the energy of the shower particles would be E2 = (0.31 ± 0.04) (6.4) = 2.0 ± 0.3 MeV if they were alphas. This confirms the determination from half-angle analysis. It is unlikely that nuclei with higher charge and mass would have sufficient range in the vapor to reach the detector chips and form etchable tracks, and hence in view of the available evidence we tentatively identfy the shower as 2 MeV alpha particles.
5. Conclusions Our observations furnish compelling evidence for a nuclear process that generated a shower of charged particles in an oxygen-hydrogen vapor. It appears to have consisted of a rapid reaction that generated a cloud of unstable intermediate particles whose decay products were the observed shower particles, tentatively identified as 2 MeV alpha particles. We can think of no explanation for this phenomenon in terms of conventional nuclear theory, and believe that an extension of the theory is required.
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Acknowledgments We thank M. E. Fisher for assistance in data presentation. References 1. M. Fleischmann, S. Pons, M. Hawkins, J. Electroanal. Chem. 261, 301 (1989) and 263, 187 (1989). 2. E.K. Storms, J. Sci. Exploration 10 (2), 186 (1996) (full text in http://www.scientificexploration.Org/jse/articles/storms/l.html). 3. E.K. Storms, Infinite Energy 4 (21), 16 (1998) (full text in http://pwl.netcom.com/~storms2/review5.html). 4. R.A. Oriani and J.C. Fisher, Jpn. J. Appl. Phys. 4 1 , 6180 (2003) and 42, 1498 (2003). 5. R.A. Oriani and J.C. Fisher, Trans. Am. Nuc. Soc. 88, 640 (2003). 6. R.A. Oriani and J.C. Fisher, in Proceedings of the 10th International Conference Cold Fusion, 2003. 7. R.L. Fleischer, P.B. Price, and R.M. Walker, Nuclear Tracks in Solids, (University of California Press, Berkeley, CA, 1975). 8. R.L. Fleischer, Private communication. 9. A.S. Roussetski, A.G. Lipson, and V.P. Andreanov, in Proceedings of the 10th International Conference Cold Fusion, 2003.
NUCLEAR REACTIONS P R O D U C E D IN A N ELECTROLYSIS CELL
OPERATING
R. A. O R I A N I University
of Minnesota, Minneapolis, MN 55419, E-mail: orianOOl Qumn. edu
USA
J. C. F I S H E R 600 Arbol Verde, Carpinteria, CA 93013, E-mail: [email protected]
USA
We report the results of experiments in which CR-39 plastic particle-detection chips were exposed in various environments within and surrounding operating electrolysis cells. Because CR-39 detectors record only particles with energies in excess of about 0.2 MeV the detected particles must have arisen in nuclear reactions. Evidence for such reactions was found in deuterium gas behind a palladium cathode that served as part of the cell enclosure, in air behind a similarly disposed nickel cathode, in air beyond the glass wall of the electrolysis cell, and in oxygen gas above the anode when anode and cathode were placed in separate arms of a Utube cell. These results, augmented by earlier work indicating nuclear reactions within the electrolyte and in the hydrogen-oxygen gas over the electrolyte, cannot be understood in terms of conventional nuclear theory.
1. Introduction Energetic charged particles can be detected by the damage tracks they generate when penetrating various solid materials. 1 When the surface is attacked by a suitable etchant damaged material is removed more rapidly than undamaged material and etch pits are formed where tracks intersect the surface. In our studies we employ detector chips that are commercially available for recording alpha particle tracks from radon decay. After appropriate calibration, analysis of etch pit sizes, shapes, and cone angles can indicate the types and energies of the responsible particles, which can be protons, alpha particles, or more massive ions. In prior work tracks of particles having energies of a few MeV have been observed in CR-39 detector chips immersed in various electrolyte solutions in operating electrolysis cells, indicating that nuclear reactions have occurred in these electrolytes. The systems studied have included D20/Li 2 S04 as electrolyte with palladium as the cathode, 2 H 2 0/Li 2 S04 electrolyte with palladium as cathode, and H 2 0/Li 2 S04 electrolyte with nickel as cathode. 3 Nuclear tracks were also found in detector chips suspended in the oxygen-hydrogen gas above an H 2 0/Li 2 S04 electrolyte using palladium or nickel as cathode material. 4 In all these experiments controls were carried 295
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out with detector chips immersed in the electrolyte solutions or suspended in the vapor above the solutions as appropriate, but in the absence of electrolysis, for the same length of time as the duration of the electrolysis experiments. The density of etch pits was observed to be on average greater for chips exposed during active electrolysis than for chips exposed in control experiments. The probabilities that the results from the electrolysis experiments and those from the controls could have arisen by chance from a single population ranged from 10~ 4 to 10~ 10 . Thus we demonstrated that a nuclear reaction of some sort in the electrolyte or in the vapor over the electrolyte can indeed accompany the electrolysis of either heavy or ordinary water using either palladium or nickel cathodes. Beyond this we have observed clusters of tens of thousands of nuclear tracks on detector chips in the H2 + O2 + H2O vapor above the electrolyte of an operating electrolysis cell.5 Analysis of one such event has shown that the tracks were caused by high energy charged particles that originated in the gas a few millimeters from the surface of the closest chip. The reaction produced a shower of about 150,000 alpha particles with energies of approximately 2 MeV of which we recorded about 40,000 on a pair of opposing detector chips. Figure 1 shows the pattern of etch pits on the more heavily pitted chip in a region having about half of the maximum track density. Figure 2 plots the variations in track density over the surfaces of the two opposing detector chips. It is evident that the particle source lay between the chips and closer to the more heavily pitted one. These experimental results cannot be explained by nuclear physics as currently understood, nor can the generation of excess energy during electrolysis first observed by Fleischmann et al.6 An extension of nuclear theory is required. The present work
Figure 1. Etch pits on a detector chip supported in the O2 + H2 + H2O vapor over an active electrolysis cell. 5
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Figure 2. (a) Contour plot of the density of etch pits on the surface of the detector chip in Fig. 1. Density in pits/image is indicated by the color scale for a mosaic of 1044 images that span the approximately 8 mm 2 surface. Outlined images could not be counted and etch pit densities were interpolated for them. The solid contour lines are spaced at 10 pits/image and range from 10 pits/image along the right side to 110 pits/image near the peak. Arrows indicate mean orientations of the tracks in various locations, (b) Contour plot of the density of etch pits on the detector chip facing the chip in Fig. 2a at a distance of approximately 1 cm. Here the solid contour lines are spaced at 3 pits/image and range from 3 pits/image on the left to 30 pits/image at the peak.
was carried out to further extend the range of electrolysis phenomena that must be explained by any successful theoretical treatment. 2. Detectors Below the Cathode Electrolyses were carried out in a small tubular glass apparatus shown schematically in Fig. 3. The cathode, either palladium or nickel sheet, was clamped between O-rings fitted into a flanged joint whose lower half connected to a gas-handling and vacuum system. The anode was a platinum wire spiral. All electrolyte solutions had the approximate concentration of 0.02 g Li 2 S0 4 per ml of either D 2 0 or H 2 0 . By means of the gas-handling system the lower surface of the cathode could be maintained in an atmosphere of air or deuterium. CR-39 plastic detector chips obtained from the Fukuvi Chemical Industry Company, Japan, were etched in 6.5 N KOH for about 20 h at 65°C, the standard etching procedure for all controls and experiments. They then were examined at 100 x for pre-existing nuclear tracks including those produced by alpha particles from radon in the laboratory air. A pre-etched chip then was placed below and parallel to the cathode sheet, and in some instances pre-etched chips were also placed in the vapor above the electrolyte in the cell. The detector chip situated below the cathode was enveloped either by air or by deuterium gas at one atmosphere pressure. In experiments with palladium cathodes and light water for the electrolytic solution the air below the cathode was admixed with hydrogen gas by permeation of hydrogen
298
To power supply Thermocouple
Detector chips Nichrome ; wire heater Ni disc
Pt anode Detector chips
—3sr
Cathode
To vacuum and, gas-handling system Figure 3. Schematic diagram of the linear electrolysis cell employed for detection of energetic charged particles in the vapor above the electrolyte, outside the cell under the cathode, and outside the cell beyond the glass enclosure.
electrodeposited on the upper surface of the cathode. Electrolysis usually was carried out for 3 days at various current densities ranging from 0.1 to 0.4 A/cm 2 , after which the chips were again etched and examined. The density of new nuclear tracks per unit area of detector chip was compared with that found in controls subjected to the same experimental procedure except for the absence of electrolysis. Markedly positive results were obtained in 10 of the 26 experiments of this kind that were carried out. In these ten the densities of nuclear tracks formed during electrolysis were far larger than in the controls. Etch pits were observed to form localized clusters suggesting that showers of particles had emanated from compact sources in the vapor near the detector chips. Figure 4 shows a cluster of pits on a chip suspended in air about 1.5 cm below a nickel cathode and employing Li2S04 in H2O as electrolyte. Figure 4 and all others are at the same magnification as Fig. 1. Arrows mark the directions in which energetic particles impinged on the detector chip, as revealed by microscopic examination of the etch pits. (Recall that pits that mark pre-existing tracks have been etched twice, and for this reason are nearly twice the diameters of pits that mark tracks that formed during the experiment. Several doubly etched pits are visible in Fig. 4 and others are visible in figures
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below.) It is apparent that the experimental particles have radiated outwardly from a source in the surrounding air just a few millimeters distant from the surface of the detector. They record a shower of charged particles that is qualitatively similar to the roughly 1000-fold larger shower shown in Figs. 1 and 2 for detectors suspended over the electrolyte.
Figure 4. Cluster of etch pits on a detector chip suspended in air under a nickel cathode. Arrows indicate the directions in which charged particles impinged on the chip. The electrolyte was IJ2SO4 in H 2 0 .
Figure 5 shows a sample of the extended distribution of etch pits that cover a detector chip suspended in air under a nickel cathode. Figure 6 shows a shower of etch pits on a chip that was held 1.5 cm under a palladium cathode, enveloped initially in air for about 1 day, then for about 2 days in deuterium gas that diffused through the cathode and displaced the air. Figure 7 shows another shower of etch pits on a chip that was enveloped in air for about a day then in deuterium gas for about 2 days. In cases where detector chips were placed below the cathode and also in the gas above the electrolyte large numbers of tracks appeared on the latter whenever significant numbers of new tracks appeared on the chips held below the cathode. We note that the tracks appearing on detector chips below the cathode could not have been produced by energetic charged particles arising within the cathode or on its wetted surface because the mean free path of such particles is too short to penetrate the 0.125 mm thickness of the cathode. The energetic charged particles must have arisen at the lower surface of the cathode or more likely within the gas below it.
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./ /
Fi gure 5. Sample of the extended distribution of etch pits covering a detector chip suspended in air under a nickel cathode. The electrolyte was Li2SC>4 in H2O.
3. Detectors Above the Anolyte An electrolysis cell in the form of a U-tube was devised, fitted with wire spirals within each leg to serve as electrodes, and with nichrome wire heaters surrounding the upper portions of the legs of the U-tube. The anode was made of platinum and the cathode was either platinum or palladium. The electrolyte was contained in the
V Figure 6. Shower of etch pits on a detector chip suspended under a palladium cathode in air lday, then in deuterium gas 2 days. The electrolyte was IJ2SO4 in D2O.
i. €
c
O
c
Figure 7. Shower of etch pits on a detector chip suspended under a palladium cathode in air 1 day, then in deuterium gas 2 days. The electrolyte was Li2S04 in D2O.
lower portion of the U-tube and extending upward to cover the electrodes in each leg. Detector chips were suspended in the legs above the level of the electrolyte where they were exposed either to the vapors generated in the anolyte at the anode or to the vapors generated in the catholyte at the cathode. T h e detectors were maintained at about 60°C by the nichrome heaters. Prior to carrying out electrolysis the detector chips were as usual etched and examined for pre-existing tracks. Electrolysis with 0.1-0.4 A / c m 2 current density was carried out for 2 or 3 days, after which the detector chips were again etched and examined. New nuclear tracks were observed in chips exposed above the anolyte as well as above the catholyte. Of fourteen experiments with chips surrounded by oxygen and water vapor above the anode, five produced new tracks in numbers much larger t h a n were produced in control chips held in the vapor above an electrolyte solution for 2 or 3 days without electrolysis. T h e successful experiments in O2 + H 2 0 over the anolyte all employed H 2 0 for the electrolyte. Figure 8 shows a small shower of etch pits on one of these chips.
4. D e t e c t o r s O u t s i d e t h e Cell We have in addition observed the production of nuclear tracks, in numbers significantly larger t h a n in controls, in detector chips placed in near contact with the outside surface of the glass cell wall at the level of the electrolytic solution. This phenomenon was seen in 6 of the 11 experiments of this type t h a t were carried out. Figure 9 shows some of the tracks produced in one of these experiments. T h e electrolyte employed H2O as solvent.
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\
\
Figure 8. Shower of etch pits on a detector chip suspended in the O2 + H2O vapor over the anolyte in a U-tube experiment. The electrolyte was IJ2SO4 in H2O
5. Challenges to Nuclear Theory We note here the sporadic nature of charged particle generation in our experiments. As stated in previous publications we infer that the cause for the difficulty of replication is our ignorance of the full range of experimental parameters that should be
c
. \ \
Figure 9. Etch pits formed near the center of a large shower on a detector chip mounted just beyond the outside surface of the glass wall of the linear electrolysis cell. The electrolyte was L i 2 S 0 4 in H 2 0 .
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controlled for nuclear reaction to occur. In addition, and probably equally important, is the strong probablity that detector chips may not be positioned sufficiently near to the location where reactions may have occurred. Our past work has amply demonstrated this possibility. Often one side of a detector chip bears a large number of new tracks while other side does not. We note also that the energy carried by the particles we detect is many orders of magnitude smaller than the total energy release as determined by calorimetric methods. Although we have presented strong evidence for nuclear reactions in the electrolyte and in various gases remote from the electrolyte, they cannot be the primary reactions that generate the reported excess energy. We presume that sustained primary reactions take place near the surfaces of the electrodes and that we observe transient secondary reactions associated with or triggered by products of the primary reactions. Yet in spite of the difficulty of replication and the modest energy represented by the observed nuclear tracks our experiments pose significant challenges to theory. We have shown that nuclear tracks can be generated during electrolysis in detector chips positioned within the electrolytic solution, in the H2 + O2 + H2O gas over the electrolyte in the straight-tube cell, in the O2 + H2O gas over the anolyte of the U-tube cell, in air below the cathode, in air just outside the glass wall of the electrolysis cell, and in deuterium gas below the cathode. These experiments indicate that nuclear reactions can be suported by oxygen and by deuterium, and that reactions can be triggered by unidentified agents that are able to pass through nickel and palladium cathodes and through the glass cell wall. Acknowledgments We thank M. E. Fisher for assistance in data presentation. References 1. R.L. Fleischer, P.B. Price, and R.M. Walker, Nuclear Tracks in Solids (University of California Press, Berkeley, CA, 1975). 2. R.A. Oriani and J.C. Fisher, Jpn. J. Appl. Phys. 41, 6180 (2003); Erratum 42, 1498 (2003). 3. R.A. Oriani and J.C. Fisher, Trans. Am. Nucl. Soc. 88, 640 (2003). 4. R.A. Oriani and J.C. Fisher, in Proceedings of the 10th International Conference on Cold Fusion (Boston, USA, 2003). 5. R.A. Oriani and J.C. Fisher, in Proceedings of the 11th International Conference on Cold Fusion (Marseille, France, 2004). 6. M. Fleischmann, S. Pons, and M. Hawkins, J. Electroanal. Chem. 261 (1989); Erratum 263, 187 (1989).
E V I D E N C E OF MICROSCOPIC BALL LIGHTNING IN COLD FUSION E X P E R I M E N T S
E. H. L E W I S E-mail:
P.O. Box 2013, Champaign, [email protected]; Web:
IL 61825, USA www.scientificrevolutions.com
There is evidence of microscopic ball lightning in several methods of cold fusion and transmutation. Thus far the experiments of Matsumoto, Miley, Shoulders, Savvatimova, and Urutskoev et al. have shown evidence of these objects that range in size from sub-atomic to about 1 mm in diameter. This article presents pictures and evidence collected by these groups, summarizes the evidence found by other groups, and discusses the significance of microscopic ball lightnings. The implications for atomic physics and physics in general are discussed.
1. Introduction During the last 13 years, the evidence for microscopic ball lightning in CF experiments has been building. Little objects that behave like natural ball lightning in many ways leave characteristic markings. Such markings have been found in Matsumoto's experiments since about 1991, Miley's experiments about 1996, Shoulders experiments about 1996, Savvatimova's experiments about 2000 and Urutskoev's experiments about 2001. I am not sure on the exact dates these markings were found. The markings are characteristically about 1 /im to 1 mm in diameter, and are usually either spots or long trail-like markings as though the ball lightning moved along the surface of something. Sometimes they are grooves or bore holes. Similar markings produced by plasmoids and EVs have been studied for decades, sometimes for fusion research; and through his experimental observations, Shoulders showed that the plasmoids studied by Bostick, Nardi, and other researchers are composed or EVs or are EVs. The significance of these objects for the field of cold fusion and transmutation in general is that these are a cause of transmutation and cold fusion reactions, but on a deeper level they point to the plasmodal identity of atoms. In this paper, the very similar markings found by these groups who did somewhat dissimilar experiments independently are discussed, compared and contrasted, and the general meaning of these objects to physics is discussed. Such markings are seen clearest in Matsumoto's Acrylite plastic sheets and in the clean targets used by Ken Shoulders. It seems that the X-ray films used by Savvatimova and the CR-39 sheets used by Urutskoev do not yield as clear markings. The trails may sometimes be millimeters long. In his early articles on cold fusion and transmutation, as part of the regular method of research on nuclear reactions, 304
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Matsumoto set up Acrylite plastic sheets coated with an emulsion that allowed him to capture the tracks of reaction products. He found strange and large markings and began to explain them by a theory called the Nattoh model, which is a type of Japanese bean pudding. He focused his experimental research on these objects creating the strange traces, especially after he learned about the idea of microscopic ball lightning, and published about six articles in Fusion Technology from 1991 to 1995 about photographs of these markings and their meaning. However, he was generally ignored and ridiculed, even by cold fusion researchers, and felt that he couldn't even get a hearing at cold fusion conferences. In 1993, he accepted the idea of microscopic ball lightning and started research on this idea specifically, but did not get his ball lightning articles published. In 1996, after an earthquake in Hokkaido where he lives, he noticed that microscopic tracks were left on plastic sheets and perhaps discovered naturally produced microscopic ball lightning. Here are two pictures of his tracks from his experiments.
Figure 1. Ring and track markings left on a sheet of acrylite plastic. 1 It is evident that at least one toroidal object about 50 fj,m wide slid and jumped around. If there were more than one such object, it was remarkably similar in size. Acrylite sheets were outside of a discharge container filled with water. The sheets of plastic were about 100 jira wide by 50 mm X 50 mm, and this sheet was one of a set of such sheets set in parallel with about a 3 mm gap in between each sheet. These emulsions were set outside a cylindrical glass cell which had an Acrylite bottom 1 mm thick. They were set outside this plastic bottom. This suggests that the plasmoid phenomena traveled through the Acrylite or the glass. One of the anomalous abilities of ball lightning is the ability to travel through glass and other insulators. This evidence points to the identity of these objects as microscopic ball lightning. It is possible that the object responsible for these markings on one side of one sheet of plastic also left similar markings close in size on the backside of the preceeding sheet. Tornadoes hop in a similar manner. The object was 50 fim wide.
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Figure 2. Ring and pit markings left on an electrode after discharge. 2 These markings are very similar to the markings shown previously by Nardi and Bostick of plasmoids. The markings are less than 50 fim wide. Matsumoto preformed electric discharging in ordinary and heavy water. The anode was a platinum pin and the cathode was a copper plate.
In 1996, a researcher working in Miley's lab investigated the microsphere experiments. These experiments involved little beads coated with thin layers of nickel or other elements about 650 A thick via a special, patented electrode sputtering technique. These pictures are from Nickel on plastic Run # 8 . This cell and the anomalous appearance of a wide range of elements has been described by Prof. George Miley in several articles. 3,4 In Miley's ICCF10 lecture, he said that this Run # 8 exhibited by far the most excess heat than the many other cells of this type. The electrolysis was performed in his laboratory at the University of Illinois. The pictures were taken by using a digital camera that was attached to a good optical microscope. The photographs in Fig. 4 were taken by Savvatimova5 of markings on X-ray film that were both inside and outside her discharge device. She used X-ray film to catch these BL markings. The objects in Shoulders' experiments that he calls EVs behave in ways similar to BL. They are a type of BL. Their special characteristics such as very fast travel may be due to the method of their production with the type of electrodes he uses. His method of getting the tracks shown here produces clear markings of the ball lightnings and their effects. He uses flat, clean materials, and sometimes coats his "witness plates" as they are called in this field with temperature sensitive material like wax in order to see how warm these objects are. Like many ball lightnings, the objects that left the markings in Fig. 5b might not have been warm at all, because in
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4
«. i
-;• M >•
(e)
W
(g)
Figure 3. These seven photographs are at a magnification of 200 X or 400 X and are of markings on the two Lexan casings, two microspheres, and the Ti anode and cathode of Run # 8 . (a) and (b) are of the post-run microspheres, (a) Two ring marks in the metal. The marks look like two rings of ball lightnings, like beads in a necklace, left little pits in the metal. These are much like most of Shoulder's ring markings, (b) One faint ring mark in the plastic bead where the metal had flaked off. (c) and (d) The titanium plate cathode and the titanium plate anode of the cell. These plates enclosed the microspheres in a Lexan plastic casing, (c) A very faint mark pointed out by the black line. It is about 18 )im wide, and is clearer in the original photographs, (d) A round ring mark in a pit that formed in the anode. The pits were interesting and deep.
308 Figure 3. (Continued) The pit itself is about 200 fim wide at the surface of the anode, but narrowed down to the white area that is about 100 /im in diameter. The ring mark is about 20 or 30 /an wide. Grooves and strings of little dots are visible as well. Ball lightning-like plasmoids often form little strings and rings. Tornadoes and ball lightning also form such lines or circles. See for example this link: http://www.ernmphotography.com/Pages/BalLLightning/OtherBLPages/fbparks/BL_Triple-Waterspout.html. (e-g) Ring marks on the casings. Two different casings were used for this run. (e) Ring mark in the plastic casing, in a photograph that was computer processed to make the edges more apparent, (f) Lexan Plastic Casing # 2 of Ni/Plastic Run # 8 . Magnification 200 X. Shows a group of small rings. The markings are seen from the outside of an intact casing. The picture shows the convex impression left by a microsphere that was in contact with the inside of the casing. The bead developed both ridges and ditch markings. To the left of the bead impression are the faint marks of rings that are about 20 /jm wide, (g) Lexan Plastic Casing # 2 of Ni/Plastic Run # 8 . Magnification 200 x. Shows a ring mark to the right of the bead impression. The picture shows the convex impression left by a microsphere that was in contact with the inside of the casing. The bead developed both ridges and ditch markings. A BL may have left a trail mark in the plastic or bored through. The ring mark is about 25 /jm in diameter. Details about the experiment and the markings are discussed in other articles. The photographs shown here were taken by E. Lewis of various components of Ni-Plastic Run # 8 in the Laboratory of Professor G. H. Miley at the University of Illinois at Urbana-Champaign in 1996. His cooperation in allowing this work is gratefully acknowledged.
1umm
Figure 4. X-ray film outside (A and B) and inside the vacuum chamber after deuteron irradiation in glow discharge.
other similar tests with aluminum oxide coated with wax, there was apparently no melting of the wax at all, although it is obvious the underlying material, aluminum oxide,6 moved as if there was a splash. Similar effects are seen around ball lightning and in lightning strikes sometimes, and in other electrical discharges experiments, and also happen during transmutation. What all this points to is a state of matter that needs to be understood. In this plasmoid state, the atoms act like ball lightning.
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(b)
(c)
Figure 5. (a) Ring Mark in Witness Plate. This is a typical type of ring marking (from Ref. 6). (b) Strike Marks on Lead Glass. These marks show the heatless motion of atoms (from Ref. 6). (a) and (b) are from the same article. Shoulders reports that there is no evidence of heat. This figure shows the effects of several ball lightnings hitting this lead glass surface, (c) Impact Site on palladium foil loaded with deuterium. Shoulders reports that chemical analysis of this spot showed many transmuted elements (from Ref. 6).
X-ray analysis of track
Energy (keV)
25
Figure 6. Impact Site X-ray analysis of the ball lightning strike shown in Fig. 5(c) (from Ref. 6). Shoulders reports that chemical analysis of this spot showed many transmuted elements.
In the next photograph, Fig. 5c, a chemical analysis was performed at the site of this type of atomic sloshing (motion), and a wide range of chemical elements are discerned, as is shown in Fig. 6. Recently, Urutskoev has published pictures similar to these as shown in Figs. 7 and 8. In Fig. 7 which is from his article published in 2002, "Observation of Transformation of Chemical Elements during Electric Discharge," 7 the marking looks much like the bottom two wispy lines in Savvatimova's picture in Fig. 4a. They look like some of the long trail tracks in Matsumoto's article as well.
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1 lOmcm
Figure 7. Trails like those shown by Matsumoto and Savvatimova. Figures 7 and 8 are from Urutskoev et al. (from Ref. 7).
a 500 mem Figure 8. A comet like trail. They wrote that markings like these had a very high energy. These may be like the type of BL markings that Matsumoto called "white holes." The white marking is about 1000 mem long, and remind me of some of Shoulders pictures of fast moving EVs. The authors attribute a nuclear-reaction origin to the object.
These pictures show similar markings. Rings or trails or combinations of rings and trails or blotches or pits. This is because the microscopic ball lightning objects may move on surfaces, as does ball lightning in nature. Or they may impact surfaces, leaving the pits. Sometimes as in nature, they leave deposits. Sometimes tornadoes and ball lightning leave grooves in the ground or in materials. In their article from 2002, Urutskoev mentioned finding markings like scratches. Dash has also written about and shown a picture of a scratch-like mark in an electrode. And Shoulders has shown pictures of such grooves. In nature, ball lightning sometimes bore tunnels in walls, and Egely8 has published descriptions of these. The existence of these objects presents cold fusion researchers and physicists in general both a cause and an effect of atomic reactions. They are a newly discovered type of particle. At a deeper level, they call into question the assumptions of nuclear physics and the QM paradigm atomic model. These objects are anomalous to QM theory in that this type of matter is energy. It points to the idea that atoms are structured like them. Research is needed to determine the effect of these ball lightning objects on time, gravity, magnetism, electricity, and atomic reactions. We need accurate determinations of the physical relationships in order for theory to develop further.
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In conclusion, thus far five groups working on three continents and one hemisphere have published the markings of tracks like t h a t of microscopic ball lightning t h a t were associated with successful t r a n s m u t a t i o n and cold fusion experiments t h a t exhibited unusually high t r a n s m u t a t i o n and excess energy. In fact, Savvatimova especially emphasized t h a t there was a correlation between the amount of t r a n s m u t a t i o n in a reaction run and the number of markings produced, and I think t h a t Miley's, Matsumoto's, Shoulders and Urutskoev's experiments also bear witness to such a correlation. I think t h a t people working in other continents and the other hemisphere will find such products and similar correlations. Some experiments may not produce these larger types of BL objects. B u t in all experiments anomalous to QM, the atoms themselves transform to a state like ball lightning.
Acknowledgments I would like to t h a n k all these researchers for their permission to reproduce these photographs.
References 1. T. Matsumoto, Observation of Tiny Ball Lightning During Electrical Discharge in Water, Manuscript Article, 1994. 2. T. Matsumoto, Experiments of One-Point Cold Fusion, Manuscript Article. 3. G.H. Miley and J.A. Patterson, Nuclear transmutations in thin-film nickel coatings undergoing electrolysis, in Proceedings of the Second International Conference on Low Energy Nuclear Reactions, 13-14 September 1996 (College Station, TX, USA). 4. G.H. Miley et al., Quantitative observation of transmutation products occurring in thin-film coated microspheres during electrolysis, in Proceedings of the ICCF-6, October 14-17 (Hokkaido, Japan). 5. I. Savvatimova, Reproducibility of experiments in glow discharge and processes accompanying deuterium ions bombardment, in Proceedings of the ICCF-8, 21-26 May 2000 (Lerici, Italy). 6. K. Shoulders, Charged Clusters in Action, Manuscript Article, 1999. 7. L.I. Urutskoev, V.I. Liksonov and V.G. Tsinoev, Observation of transformation of chemical elements during electric discharge, Annales Fondation Louis de Broglie 27 (4), 701 (2002). 8. G. Egely, Hungarian Ball Lighting Observations (Center Research Institute of Physics, Hungarian Academy of Sciences, 1987).
N E U T R O N EMISSION FROM D 2 GAS IN M A G N E T I C FIELDS U N D E R LOW T E M P E R A T U R E
TADAHIKO MIZUNO, TADASHI A K I M O T O , AKITO TAKAHASHI, AND FRANCESCO CELANI Division
of Quantum University,
energy engineering, Graduate School of Engineering, Kita 13 Nishi 8, Kita-ku, Sapporo 060-8628, Japan
Hokkaido
AKITO TAKAHASHI Emeritus
professor
of Osaka University,
Japan
FRANCESCO CELANI INFN-LNF,
via E. Fermi 40 00044, Frascati,
Rome,
Italy
We observed neutron emissions from pure deuterium gas after it was cooled in liquid nitrogen and placed in a magnetic field. Neutron emissions were observed in ten out of ten test cases. Neutron burst of 5.5counts/s were 1000 times higher than the background counts. These bursts occurred one or two times within a 300 s interval. The total neutron emission can be estimated from the counting efficiency, and it was 10 4 -10 5 counts/s. The reaction appears to be highly reproducible, reliably generating high neutron emissions. We conclude that the models proposed heretofore based upon d-d reactions are inadequate to explain the present results, which must involve magnetic field nuclear reactions.
1. Introduction There have been many reports of neutron generation during cold fusion experiments. 1_3 Although there have been a few negative reports, 4 most show some neutron emission. However, it seems hard to replicate, and reaction rates are very low. Shyam et al.5 reported on conventional light and heavy water electrolysis with a palladium electrode. They used 16 BF3 neutron detectors to increase the chance of detection. They observed a difference in neutron emission rates between light and heavy water electrolysis. The neutron count rate was slightly higher for heavy water. Shyam et al. conducted a series of experiments to detect production of neutrons from a commercial palladium-nickel electrolytic cell operated with 0.1 M LiOH or LiOD as the electrolyte, at a current density of ~80mA/cm 2 . A bank of 16 BF3 detectors embedded in a cylindrical moderator assembly detected neutron emission. A dead time filtering technique was used to detect the presence of neutron bursts, if any, and to characterize the multiplicity distribution of such neutron bursts. It was found that with an operating Pd-D20 cell located in the center of the 312
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neutron detection setup the daily average neutron count rate increased by about 9% throughout 1-month period, over the background value of ~2386 counts/day. This indicated an average daily neutron production of ^2220 neutrons/day by the cell. In addition, analysis of the dead time filtered counts data indicated that about 6.5% of these neutrons were emitted in the form of bursts of 20-100 neutrons each. On an average, there were an additional six burst events per day during electrolysis with LiOD over the daily average background burst rate of 1.7 bursts/day. The frequency of burst events as well as their multiplicity was significantly higher with D 2 0 + LiOD in the cell when compared with background runs and the light water control runs. Oya et al.6 used a precise method to determine the relationship between neutron energy and excess heat. They use flow calorimetry measure excess heat generation. They showed a clear relation between heat and neutron generation. Neutron energy was in the MeV order when the excess power was generated. The key parameters for the occurrence of the anomalous phenomena, especially excess heat generation and the emission of excess neutrons, have been investigated through a series of electrolytic experiments in Pd-LiOD (H) systems. Seven key parameters have been identified: (1) (2) (3) (4) (5) (6) (7)
purity of Pd cathode, shape and size of Pd cathode, processes of pretreatment of Pd cathode, electrolysis mode, electrolyte, purity of the medium, initial open-circuit voltage.
In the present work, a series of systematic experiments have been carried out with some fixed parameters. By controlling key parameters completely, an appreciable correlation between the excess heat generation and the excess neutron emission can be replicated successfully. We have sometimes seen neuron emission with a phase transition method. This typically occurs in non-equilibrium conditions. Chicea and Lupu 7 showed the neutron emission from Ti metal loaded by deuterium gas absorption. Chicea used a simple measurement system. The sample holder includes Ti powder. The Ti metal absorbed deuterium gas and sporadic neutron generation occurred. In several experiments, Chicea and Lupu loaded titanium samples with deuterium in gas phase, and the temperature of the samples was changed over a wide range, while neutron emissions were monitored. Neutron emissions were recorded in very low intensity bursts, but still significantly above the background. This revealed that low energy nuclear reactions in condensed matter can be produced at a low rate, which is occasionally high enough to become detectable. They observed very strong neutron emission occurred more than 10 times during 20 h. At times, the emission exceeded four times background counts.
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Jones et al.a used a similar method, and they reported neutron emission from Ti metal that absorbed deuterium gas. Jones' results are very clear, showing that neutron emission only occurs with deuterium gas, not hydrogen. They presented evidence for neutrons emanating from partially deuterided titanium foils (TiDx) subjected to non-equilibrium conditions. A previous paper presented data for complementary charged-particle emissions. Metal processing and establishing non-equilibrium conditions appear to be important keys to achieving significant nuclear-particle yields and repeatability. It is very important to confirm nuclear products to prove that cold fusion is, in fact, some kinds of nuclear reaction. Neutrons are especially suitable for this purpose. We have already published transmutations results from the electrolysis method. We have confirmed isotopic shifts in elements. We have also confirmed neutron emission during various methods of cold fusion. We have measured the neutron energy distribution during heavy water electrolysis with a Pd electrode with a closed-cell system. 9 The cell temperature and pressure can be raised to increase deuterium absorption. We observed a clear neutron energy peak at 2.5 MeV. This indicates a possible d-d nuclear fusion reaction. The reaction rate was estimated as 10 _ 2 3 /dd/s. We have used other methods to increase the probability of neutron generation. We used very high purity heavy water absorbed into a Pd wire. After the wire absorbed deuterium, hydrogen gas was admitted into the wire to stimulate the neutron generation reaction. 10 The neutron count, the duration of the release and the time of the release after electrolysis was initiated all fluctuated considerably. Neutron emissions were observed in five out of ten test cases. In all previous experiments reported, only heavy water was used, and light water was absorbed only as accidental contamination. Compared to these deuterium results, the neutron count when hydrogen is deliberately introduced is orders of magnitude higher, and reproducibility is much improved. Several analytical methods suggested some characteristic elements appearance in the electrolysis system after the neutron emission. After filling the Pd wire with deuterium in heavy water, we took the wire and immersed it in the heavy water system. Figure 1 shows the time change for input voltage, current and electrolyte temperature. At 3000 s, we changed the voltage from 32 to 85 V. Figure 2 shows the neutron emission during this voltage change. The neutron count was 100 times larger than the background count. The rate of neutron emission depended on the purity of heavy water. We can see neutron emission occurred at more than 90% of purity as shown in Fig. 3. We can say that we have to pay attention if you want to generate neutron emission. Because that the heavy water easily absorbs light water. The rate of neutron count was estimated as 1.5 x 10 _ 1 7 /dd/s. The rate was increased 106 by the conventional deuterium gas absorption method.
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Neutron burst.
2. Experimental The reaction cell was a Pyrex glass tube of 6 mm diameter, 3 mm inner diameter and 100 mm in length, filled with pure D2 gas. A coil wound around the tube supplied the magnetic field. This magnetic coil is made from 10,000 turns of 1.5mm diameter copper wire. Another Pyrex glass vessel of 50 mm diameter was put around the reactor tube, and filled with liquid nitrogen. The whole system was put in a stainless steel vessel 1.5-mm thick. The outer surface of the steel vessel is insulated with Styrofoam, and another layer of 1.5-mm thick stainless steel plates were placed on top of the Styrofoam insulation to prevent electromagnetic noise
316
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Dependence of neutron on purity of D2O.
from reaching the neutron measurement system. The vessel was filled with liquid N2 to cool the coil and the reactor tube. The magnetic field was 8 kg at the center of the reaction tube. Power for the magnetic coil was supplied by a stable direct current power supply through a resistive wire, to control the current. The magnetic field passes through the reaction tube along its length. The height of the coil is 100 mm; the same as tube length. The current passing through the coil was increased from 0 to 100 A, which gives the change of intensity of the magnetic field from 0 to 8 kg. Neutrons were measured with three external He 3 detectors placed around the cell, 20 cm from the vessel walls. The method seems rather simple. We filled the glass tube with pure D2 gas. The pressure was several atmospheres, typically 3 atm. The glass tube was then cooled by liquid nitrogen. After that, we supplied a magnetic field. The temperature was kept under -196°C. The magnetic field was periodically changed, and this produced a sporadic neutron burst. Figure 4 is a photo of the experimental system, power supply, and neutron measurement system. We used Aloka neutron survey meter TPS-451S and three He-3 detectors. The He-3 proportional detector has the energy sensitivity from 0.025 eV to 15 MeV. The sensitivity was calibrated using a standard Cf-252 neutron source. Figure 5 shows a schematic representation of the measurement system. The liquid N2 gas cooled the reactor tube. The maximum magnetic field was 10 kg in the center of the reaction tube. The current for the magnetic coil was supplied by a stable direct current power supply through a resistive wire. The magnetic field passes through the reaction tube along the length. The height of the magnetic coil is 100 mm, that is, the same as tube length. The current passing
317
Figure 4.
Photo of D2 gas experimental setup.
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Schematic representation of the D 2 gas experimental setup.
through the coil was changed from 0 to 100 A; changing intensity of the magnetic field was changed from 0 to 10 kg. Neutrons were measured with three external He 3 detectors, each 2 cm in diameter and 10 cm in length. They were placed around the cell, separated 20 cm from the
318
cell. All the detectors were surrounded by a cylindrical plastic neutron moderators, 12-cm diameter and 15-cm high. The detectors were inside the moderator, with the open end of the cylinder facing the cell. To reduce noise, the detectors were covered by electromagnetic shielding. After calibration, neutrons and noise were distinguished by covering one of the detectors with 0.5-mm thick Cd film. A neutron entering through the plastic moderator will lose energy and be absorbed by the foil, while electromagnetic noise easily passes through the Cd material. The detectors were calibrated with a standard Cf-252 neutron source (2.58 x 10 4 decay/s). The background count was estimated as under 0.008 ± 0.003 counts/s. A typical count under these conditions was 5 ± 1 count/s from the standard neutron source. This means the total counting efficiency is estimated as 0.0002. Figure 6 shows the typical neutron counting rate over 10 min after 3 atm of D2 gas filled the tube, a magnetic field of 8 kg was imposed, and the cell has been cooled in liquid nitrogen. The magnetic field was changed to 10 kg at 1200 s by increasing the current. About 20 s, a low-level neutron emission began, and after 50 s, a sudden neutron burst was observed. In this experiment, the reactor tube was filled the pure deuterium gas up to 3 atm, and the liquid N2 was put into the vessel holding the reactor tube, and the magnetic field was imposed in the last step. In other experiments, these steps were taken in a different order.
DD cluster reaction distance between cell and detector: 30 cm
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In this example cooling of the deuterium gas was continued for a considerable
319
time and neutron emission was sporadically observed when the electromagnetic field was changed. However, in other runs, neutron emissions were observed immediately after liquid N2 was added. Figure 7 shows the real time-representation for the previous graph. Neutron emission occurred very sporadically over a very short period. So, the rate of the neutron emission changed by the accumulation time. The real counts calculated by inverse time of each emission intervals is shown here. This demonstrates that the neutron emission is very strong and very high and it sometimes almost 1000 times higher than the background counts.
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Figure 8 shows the case of hydrogen gas at liquid N2 temperature under 8 kg of magnetic field. First, the tube was evacuated and the magnetic field was fixed at 8 kg. After that, at 220 s, hydrogen gas was introduced into the tube, and the hydrogen gas was removed at 3430 s. No neutron burst was observed during the time hydrogen gas was present in the tube. We can see there are no neutron emissions exceeding background counts during the test. Figure 9 shows another typical neutrons emission when the tube was first supplied the magnetic field and then cooled by liquid N 2 . Here, the neutron emission occurred immediately after liquid N2 was added. The count rate increased up to a peak within a few seconds and decreased a few seconds later. Total neutron emission for this brief period is estimated as 5 x 105. However, no more neutron emissions were observed after that, even when the input magnetic current was increased up to 100 A for 4000 s. In other examples, the total neutron count ranged from 104 to 105, and emissions lasted 1-4000 s. All cases were marked by a characteristic high
320
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321
Figure 10 shows the neutron count that was calculated in the inverse time for each neutron burst from previous figure. As shown here, the neutron burst occurred between 0 and 120 s.
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Figure 11 shows an example when the temperature was kept at room temperature, 20°C. Deuterium gas was kept in an 8 kg magnetic field. However, there were no neutrons above background. The neutron emission measurements under various conditions are shown in Table 1. The necessary conditions to make a neutron burst were: deuterium gas, a magnetic field and a low temperature. Neutrons were not generated when one of these conditions was not met. The generation of neutrons when the intensity of magnetic field was changed has not been measured systematically. We usually kept the intensity of the magnetic field constant to avoid noise from the current change and magnetic influence on the measurement system. Table 1. Gas Air Air Vac. Vac. H2 H2 D2 D2
Neutron emission measurements under various conditions.
Mag. field (kg) 8 8 8 8 8 8 8 8
Temperature (°C) 20 -196 20 -196 20 -196 -196 20
Maximum neutron count 0.016/s 0.01 count/s 0.01 count/s 0.009 counts/s 0.009 counts/s 0.013 counts/s 5 counts/s 0.015 counts/min
322
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We have no clear conclusion regarding the relationship between magnetic field intensity and the neutron emission. However, when a magnetic field was not supplied at all, neutrons were not emitted. We conclude that the magnetic field is necessary.Neutron emissions from the cooled D 2 gas following a change in a magnetic field are very difficult to explain by the models proposed heretofore, which involve d+d fusion reactions. These models assume that neutron emissions occur when deuterium gas alone is present; they suggest nothing about a magnetic field or low temperature; and they predict that emissions must be accompanied by excess heat and tritium production. 3. Results We have confirmed clear neutron emissions from pure deuterium gas after it is cooled in liquid nitrogen and then exposed to a magnetic field. The neutron count and duration of the emission fluctuated considerably. Repeatability was excellent, although the neutron count was sporadic. The reason neutrons are generated under such simple conditions is difficult to explain. However, Takahashi has suggested the d-d cluster fusion theory. In this theory, deuterium atoms take a unique arrangement in the metal crystal. It may be that deuterium gas under the low temperature and magnetic field locally arrange themselves in a similar array. Then some trigger reaction, such as local temperature change, change of magnetic field, or a fluctuation of the concentration of the deuterium gas induces the local change between the interactions of the deuterium atom, inducing a weak fusion reaction.
323
Moreover, the reaction may be triggered by particles such as a neutrino or muon from cosmic rays. However, these scenarios are still unclear. We need more experimental works to identify what the theory is most adequate. References 1. E. Choi, H. Ejiri, and H. Ohsumi, Application of a Ge detector to search for fast neutrons from DD fusion in deuterized Pd, Jpn. J. Appl. Phys. A 32A, 3964 (1993). 2. E. Choi, et al, Search for time-correlated fast neutrons from DD fusion at room temperature. Jpn. J. Appl. Phys. A, 35, 2793 (1996). 3. T.N. Claytor, D.G. Tuggle, and H.O. Menlove, Tritium generation and neutron measurements in Pd-Si Under high deuterium gas pressure, in Proceedings of the Second Annual Conference on Cold Fusion, "The Science of Cold Fusion". (Como, Italy: Societa Italiana di Fisica, Bologna, Italy, 1991). 4. E. Cisbani, et al., Neutron detector for cf experiments, Nucl. Inst. Methods Phys. Res. A, 459, 247 (2001). 5. A. Shyam, et al., Observation of high multiplicity bursts of neutrons during electrolysis of heavy water with palladium cathode using the dead-time filtering technique, in Proceedings of the 5th International Conference on Cold Fusion (Monte-Carlo, Monaco: IMRA Europe, Sophia Antipolis Cedex, France, 1995). 6. Y. Oya, et al, Material conditions to replicate the generation of excess energy and the emission of excess neutrons, in Proceedings of The Seventh International Conference on Cold Fusion (Vancouver, Canada: ENECO Inc., Salt Lake City, UT, 1998). 7. D. Chicea and D. Lupu, Low-intensity neutron emission from TiDx samples under nonequilibrium conditions, Fusion Technol. 39, 108 (2001). 8. S.E. Jones, et al., Neutron emissions from metal deuterides, in Proceedings of the 10th International Conference on Cold Fusion (Cambridge, MA, 2003). 9. T. Mizuno, T. Akimoto, and N. Sato, Neutron evolution from annealed palladium cathode in LiOD-D20 Solution. 10. T. Mizuno, T. Akimoto, T. Ohmori, A. Takahashi, H. Yamada, and H. Numata, Neutron evolution from a palladium electrode by alternate absorption treatment of deuterium and hydrogen, Jpn. J. Appl. Phys. 40, L989-L991 (2001).
E N E R G E T I C C H A R G E D PARTICLE EMISSION FROM H Y D R O G E N - L O A D E D Pd A N D Ti CATHODES A N D ITS E N H A N C E M E N T B Y He-4 IMPLANTATION
A. G. L I P S O N A N D G. H. M I L E Y University
of Illinois
at Urbana-Champaign,
Urbana, IL,
USA
A. G. L I P S O N A N D B . F . L Y A K H O V Institute
of Physical
Chemistry,
The Russian
Academy
of Sciences,
Russia
of Sciences,
Russia
A. S. R O U S S E T S K I P. N. Lebedev Physics
Institute,
The Russian
Academy
In this paper, we demonstrate reproducible emissions of energetic alphas and protons appearing in an energy range where both cosmic ray interference and possible alpha emissions from contamination (e.g., radon) is assumed to be negligible. We also show that He 4 doping of Pd and Ti cathodes leads to a significant enhancement of the energetic charged particles emission (ECPE). This measurement of the emissions of energetic (MeV) particles, in a region of low background interference plus their enhancement by He 4 doping provides very strong support for the existence of LENR processes in the crystalline lattice of deuterated metals.
1. Introduction The LENR and accompanying new physical effects in deuterated metals still do not receive necessary attention from the major scientific community, mainly due to a lack of reproducibility and their low intensity compared with the background. For instance, usually the detection of DD-reaction products in LENR experiments with deuterated metals (Pd and Ti), including neutrons and charged particles is accompanied by significant background counts, giving rise from cosmic rays and environment contaminations, especially in the energy ranges of interest. So, charged particles detected from DD-reaction (3.0 MeV p and 1.0 MeV t) show a very low intensity and appear at such energy range where the background counts are typically non-negligible.1'2 That is why, detection of energetic particles that could be easily distinguished from the background induced radiation is considered as highly desirable. Earlier we found that metal targets with a high hydrogen/deuterium solubility (Pd and Ti) underwent either by electrolysis, glow discharge deuteron bombardment or powerful pulsed laser irradiation demonstrate energetic charged particles emissions (ECPE), including alphas (9.0 < Ea < 15.0MeV) and protons/deuterons 324
325
[Ep(Ed) ~ 1.7(2.8MeV)].3 Based on the similarities between energy spectra of charged particles emitted in D/H Pd and Ti loading processes (Electrolysis, GD) with those emitted in the laser irradiation of TiH^D^) targets we have speculated that the ECPE from the Pd and Ti targets is determined by focusing of the energy applied during H-loading to the cathode in some specific lattice sites near surface (possibly the sites of a high internal strain) containing light nuclei (including He 4 ).On the other hand, the coherent energy transfer from DD-reaction sites in metal deuterides accordingly to Hagelstein4 would suggest the emission of alphas and protons in the same energy range as they were observed in our experiments. In this paper, we demonstrate reproducible emissions of energetic alphas and protons appearing in such energy range where possible cosmic rays and alpha contamination-induced particle radiation is assumed to be negligible. We also showed that He 4 doping of Pd and Ti cathodes leads to significant enhancement of the ECPE. The emissions of energetic particles, which are not peculiar to the natural background sources provides a strong support for existence of LENR processes in the crystalline lattice of deuterated metals. 2. Experimental In order to study ECPE from the metal hydrides both semiconductor Si-barier (SSB) and plastic track (CR-39) detectors were used. The ECPE during exothermic deuterium/hydrogen desorption from Pd foils loaded electrochemically was detected with Si-surface barrier detectors (ORTEC) of various efficiency calibrated with 241 Am alpha-source operated in vacuum 10~ 3 — 10~ 6 torr: SSB(l): S = 100 mm 2 , SSB(2): S = 900 mm 2 (the distance between the target and detector: d = 10-20mm). In order to suppress electromagnetic noise and provide twodimensional spectra for particle identification the dE-E SSB detector pair (dE-h = 20 /xm, E:h = 100 /xm, time gate A T = 20 ns) in air at ambient condition was employed (Fig. 1). To provide in situ detection of ECPE during electrolysis as well as after the D/H-loading we used purified (<20track/cm 2 ) Landauer (USA) CR-39 detector chips with area S = 2 x 1 cm2 attached to the cathode. Various metal foils and PE films were employed as a shielding (11-66/xm Al, 25-50 /jm Cu). Comparison of track diameters obtained with open and shielded CR-39 allow to identify charged particle accordingly to their stopping range in the shielding material (Fig. 2). In experiments with Pd/PdO doped with He4 another type of cell (with separated cathode and anode spaces was employed). After electrolysis detection of the ECPE from the Pd/PdO surface was carried out using additional mechanical loading of the samples (the load mass ~100 g) The effect of He implantation into Pd foil on the characteristics of EPC emissions was studied in situ during its electrochemical loading with hydrogen (Fig. 3). In this work, the 50/xm thick Pd/PdO heterostructure samples were used as a cathode. The complex cathode consists of large area (S = 4 x 2 cm 2 ) Pd/PdO substrate and smaller area Pd/PdO:He piece (S = 2 x 1 cm 2 ) tightly attached to the substrate from one of its side. The both
326
jsample
Al screen Figure 1.
The dE-E
detector pair diagram.
parts of cathode were cut from the same foil. The electrolysis was carried out in 1M L12SO4/H2O solution at current density j — 20mA/cm 2 . The CR-39 track detectors were applied to both the Pd/PdO substrate and Pd/PdO:He coating side. The background detectors were placed at the bottom of the electrolytic cell. The electrolysis duration was chosen as 230 h. The set of CR-39 detectors was calibrated by alpha-sources (1.9-7.8 MeV) cyclotron (alphas 9.0-30.0 MeV) and Van de Graaf accelerator (protons 0.5-3.0 MeV), accordingly to Ref. 3. After exposure in foreground and background runs the CR39 detectors were uniformly and simultaneously etched in 6M NaOH solution at
T - • Vessel AI203
Pd CR-39 (bgrj
" • Clamp _CR-39(fg) Electrolyte
CZ3-
CR - 39 (bgr)
Figure 2. Diagram of in situ E C P E detection with CR-39 track detectors (foreground CR-39 is attached to the Pd face of thin film Pd cathode on alumina substrate).
327
CR - 39 (fg)
Pt anode CR - 39 (fg) Pd/PdO:He Pd/PdO
CR - 39 (bgr)
a CR - 39 Pd/PdO He:Hx Pd/PdO:Hx Figure 3. Electrolytic cell with [Pd/PdO:He] - [Pd/PdO] complex cathode (upper figure) and attached background and foreground CR-39 detectors. Lower figure shows diagram of E C P E after electrolysis detection with the same cathodes.
t = 70°C during n = 7.0 h (removed layer is h = 9.2 fim). In order to obtain the proof for energetic particle detection, some calibration and Foreground detectors were subjected by 7.0 h, additional etching, such that total etching time was increased to r 2 = 14.0 h (h = 18.4 pm). This procedure allows unambiguously to distinguish ECPE tracks from the track-like defects (voids) at the CR-39 surface. In this work, electrochemically loaded foils of Ti, Pd/PdO and Au/Pd/PdOiD^. (1M L i 2 S 0 4 / H 2 0 ; 1 M NaOD/D 2 0; j = 20mA/cm 2 ) of 40-60 mm thick have been served as cathodes. In situ measurements with CR-39 track detectors were also performed with alumina/Pd (600nm), thin film cathode during electrolysis (1M L i 2 S 0 4 / H 2 0 , j = 10mA/cm 2 ). In order to explore a He 4 doping effect on ECPE yield during electrolysis, the Ti, and Pd/PdO foils were implanted from one side with He-4 ions using He-gun (total fluence F H e = 2 x 1016 4 He/cm 2 , E H e = 20keV. The stopping range of He-4 atoms in these foils is estimated as Rne ~ 20-30 nm. 3. Experimental Results Let us consider the typical SSB spectrum of charged particles obtained in vacuum with a reference pristine Au/Pd/PdO sample (that was not subjected to H/Dloading) for a long time of exposure. As seen from Fig. 4, it contains no counts at high-energy range above 8.0 MeV. The absence of counts at E > 8.0 MeV is complied with this fact that any known natural alpha-nuclides emit particles having energies which settled below 7.8 MeV (maximal alpha energy E ~ 7.8MeV for radon series). On the other hand, there
328
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are no energetic protons in the MeV range could be found in the spectra of comic particles at the surface of the earth because proton energy would be spent to neutron production in the atmosphere. That is why, in order to obtain a solid evidence for nuclear particle emissions in metal-hydrogen/deuterium system, the search in the energy range of E > 8.0 MeV is supposed to be highly desirable, solely, because the background events would not be covered the picture of possible ECPE. Much shorter exposure of Au/Pd/PdOiD^ sample in front of individual SSB-1 (low geometrical efficiency detector) in vacuum showed few counts at E = 9.1 MeV (Fig. 5). Notice that the similar result of high energy counts was obtained with Au/Pd/PdO:Ha; sample. The annealing of deuterium/hydrogen from the sample (at T = 400° C) resulting in spectrum, which is similar to the Background (Fig. 4). Application of high geometrical efficiency, large area SSB-2 detector in similar experiment with Au/Pd/PdO:D,j; sample in vacuum gives higher number of counts at E > 8.0 MeV already for the shorter time of sample's exposure in front of detector (Fig. 6). In order to identify type of high-energy particles emitted from the surface of Au/Pd/PdO:D(H).,. samples the dE — E detector pair was employed in air at ambient condition. The background experiment with reference Au/Pd/PdO sample showed two-dimensional count points (corresponding simultaneously to particle energy loss in thin dE and its stopping in thick .E-detectors) with coordinates (dE, E) at channel numbers N&E > 1000 ch. and NE < 600 ch. These channel numbers are corresponded to detection of alpha particles with energy in the range of 5.0 < Ea < 7.5 MeV or protons of 1.3 < Ep < 1.5 MeV and are anticipated in terms of natural radionuclide and cosmic background (Fig. 7).
329
Au/PdO:Dx, spontaneous D-desorption: T=300K, P=10"6torr, SSB:S= 100 mm2, f= 133,000 s
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Energy (MeV) Figure 5. A u / P d / P d O : D x after t h e electrolytic D-loading. Sample is in front of detector (d = 15mm). Foreground run, SSB-1 detector efficiency 3.3% (arrow marks the expected radon alpha edge).
The bands of alphas and protons in Fig. 7 are calculated accordingly to stopping powers of these particles in silicon. This result only confirms the results of background measurement with individual SSB-1 detector (Fig. 4), which showed
20 18H
Detector: SSB, e = 12%, vacuum: 10~3 torr
16
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Figure 6. Large area high efficiency SSB-2 detector: S = 900mm 2 , e = 12.0%. Foreground run. The counts with E > 8.0 MeV are collected for a shorter time than that with SSB-1.
330
dE/E Au/Pd/PdO Background run (dE/ETDC 750920 ch, gate 20 ns) •
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absence of any real ECPE at E > 8.0 MeV. Notice that real particles produce only two-dimensional poi with coordinates [E, dE). All one-dimensional events on the dE and E axis could be referenced to electronic noise. The events with dE coordinate N dE > 0 and E axis NE > 2000 ch. may be considered as a passage of very high-energy particle through the detector pair. In contrast, experiment with both Au/Pd/PdOiD^ and Au/Pd/PdO:H x heterostructure samples showed significant count number at the strip corresponded to energetic alpha-particle emission with E > 8.0 MeV. In Fig. 8, the data obtained for exposure of 18 Au/Pd/PdOiD^ samples (T,t = 550 h) in front of dE/E detector is presented. Taking into account geometrical efficiency of dE/E detection, the number of counts which are corresponded to calculated alpha strip for stopping power of used dE/E detector pair and have energy E > 8.0 MeV was found to be (Na) = (6.4 ± 1.2) x 10" 4 (s _ 1 ) in 4TT ster. Thus, the SSB measurement, confirmed by dE/E noiseless detection showed that Au/Pd/PdO samples loaded with deuterium/hydrogen emit energetic alpha particles in the energy range of approximately 9.0-14.0 MeV. If CR-39 technique is sensitive enough to detect low-intensity energetic alphas, then some signatures of ECPE should also be anticipated in experiments with plastic detectors. In order to check feasibility of CR-39 to measure ECPE we used the same Au/Pd/PdOiD^ samples loaded with deuterium to be exposed in the exothermic deuterium desorption regime. To enhance D-desorption the additional mechanical loading was applied to the sample with attached CR-39 detectors (Fig. 9a, b). In order to determine feasibility of ECPE in other metals (with low hydrogen solubility) and compare such results with ECPE from Pd/PdO samples in this experiment we
331
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E (channel) Figure 8. AE/E (SSB: AE = 20/u,m, E = 100 ^m) 2-dimensional spectra of charged particles from A u / P d / P d O i D s (after electrolysis): S i = 550h; (N Q ) = (6.4 ± 1.2) x l O " 4 ^ " 1 ) in Air ster.
also detected charged particles using Stainless steel, Cu and Al cathodes subjected to electrolysis. Measurements with CR-39 detectors showed presence of tracks with diameter ranging of 6.0 < d < 8.0 fim for Au/Pd/PdOiD^ system and total absence of tracks in those diameter range for St. steel, Al and Cu cathode exposed on the same
Au/Pd/PdO:D x (40 urn) t = 170 h, P= 80 g St. steel (100 nm), t = 275 h, P = 200 g Cu (50 urn), f = 275 h, P = 200 g Al (50 urn), t= 275 h, P = j?00 g
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Figure 9. a: CR-39 data on ECP emissions (8 < Ea < 16 MeV) in A u / P d / P d O i D j , (after electrolytic D-loading): (Na) = (5.6 ± 0.5) X l O - 4 ^ - 1 - cm _ 2 )/47r ster (compare with AE/E result). In Fig. 9b the diagram of experimental arrangement is presented.
332
manner. Accordingly t o our CR-39 calibrations 3 the tracks with diameter about 7.0 ± 0.2/tm are usually associated with energetic alpha particles in the range of 12.0 ± 3.0 MeV. T h e tracks with il = 6.2//in could be considered as a signature of 1.7 MeV protons or 2.8 MeV deuterons. Notice t h a t all tested samples showed presence of radon line at d = 8.0 / a n corresponding to alpha energy E = 7.8 MeV. Using Al and Cu samples results as the background counts one can calculate the yield of energetic (E = 12.0 ± 3.0 MeV) alpha particles, taking into account CR-39 efficiency with respect to critical angle of alphas. 3 This calculation gives the result (jY a ) = (5-6 ± 0.5) x 1 0 - 4 ( s - 1 c m - 2 ) in 4TT stcr. which is quite comparable with energetic alpha yield found from the dE/E detection data. Therefore, both SSB and CR-39 techniques allow to observe low intensity emission of energetic charged particles in Pd deuteride/hydride and show comparable results. T h e fast alpha-emission yield obtained in dE/E measurement has the same magnitude in CR-39 experiments confirmed by CR-39 detection. This observation gave rise t o our next step in E C P E study: application of CR-39 technique t o in situ electrolysis detection of E C P E using P d and Ti cathodes. Here we briefly remind some important results t h a t were obtained during in situ detection of E C P E in electrolysis experiment (the diagram is shown in Fig. 2) with the thin film P d cathode on top of alumina substrate. T h e background experiments showed proportional growth of track density vs. time for CR-39 immersed in electrolyte (Fig. 10). For large exposure time (/ > 10 days) two separate alpha peaks with track diameters located at 8.0 and 9.0/tm. respectively, were observed. The positions of these peaks are in good agreement with natural alpha background and are normally corresponding to ~ 7 . 0 MeV radon (8.0/(in tracks) and 5.0 MeV thoron (9.0/tin tracks) series of alpha.-nuclides contained in electrolyte. The foreground runs (f ~ 2.0 30 days) with electrolysis of Pd-thin film cathodes showed the appearance of unusual diameter tracks t h a t were not found in the back-
BB|Opon CR-39 background, t=335 h • • O p e n CR-39 background, / ." i<; h • • O p e n CR-39 background, .'-118 h
i 6
7
ii y
liu«
8 9 10 Track diameter (urn)
11
12
Figure 10. Background runs witli CR-39 detectors immersed in 1 M L12SO.1 electrolyte (the cell with magnetic stirrer).
333
ground detectors in the same electrolysis runs. Two significant peaks located at 7.0 and 6.0/an are observed in the foreground with open (not Cu-shielded) CR-39 (Fig. 11).
140120
| Foreground for open CR-39 I Background for open CR-39
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10
11
12
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Figure 11. The foreground (CR-39 attached to Pd face of the cathode) and background (CR-39 attached to alumina face of the cathode) runs with open CR-39 track detectors.
In the foreground runs using the same cathode and Cu-shielded CR-39, the 7.0 and 6.0//in peaks disappeared, but new peaks ranging from 7.5 to 11.4/nn occur (Fig. 12).
20
IForeground for Cu/CR-39 IBackground for Cu/CR-39
15-
o 10^
% 5
• 6
1 7
8
9
Track d i a m e t e r ( u m )
Figure 12. Cu foils.
The foreground and background runs with the CR-39 detectors shielded with 25/nn
Comparison of Figs. 11 and 12 shows that 6/an peak is completely disappeared due to Cu-shielding. while the broad 7.0/an peak shifted to the larger track diameters and split, to three narrow peaks (Fig. 12). Disappearance of 6.0/an peak with a shielded detector suggests it corresponds to a low MeV proton nature of this peak (Ep ~ 1.5-1.7MeV). There are no such changes in background CR-39 track
334
distribution. Rough reconstruction of Background alpha-particle energy spectrum, accordingly to calibration data showed only presence of anticipated radon and toron series of alpha nuclides in electrolyte (Fig. 13).
Alpha track energy distribution for background CR-39 (Pd/Alumina electrolysis)
Open CR-39 (bgr) •m— 25 mem Cu/CR-39 (bgr)
10
15
20
25
Alpha energy (MeV)
Figure 13.
Reconstruction of the alpha-particle energy spectrum from CR-39 background data.
In contrast, foreground CR-39 measurements during electrolysis of thin Pd-film indicate that fast alpha-particles ranging within 11.0-16.0 MeV (Na = (4.8 ± 1.0)* x 10" 4 /scm 2 ) and ~ 1.7MeV protons (7Vp = (28.6 ± 4.1)* x 10" 4 /scm 2 ) are emitted. The reconstructed alpha-energy spectrum based on Figs. 11 and 12, and CR-39 calibration data is presented in Fig. 14. The energetic alphas cannot be explained by the interaction of the background thermal neutrons with Li6 isotope in the electrolyte. This would give lower energy alphas with track diameters exceeding 14 fim that would be completely stopped by the Cu shielding foil. Thus, results of in situ CR-39 measurements during electrolysis showed low intensity, but reproducible ECPE of fast alpha particles and 1.7/2.8 MeV proton/deuteron. Earlier (Ref. 3) we have showed that ECP emissions from Pd and Ti loaded with deuterium or hydrogen demonstrate some similarities with ECPE induced by powerful laser striking the same targets. If some lattice mechanisms providing applied energy focusing have existed, then the ECP in electrolysis or D/H-desorption would be occurred similarly to laser induced processes via Coulomb explosion of "hot" spots beneath the surface of metal deuteride. The energy released in such a process could be transferred to the closest light nuclei (including, p, d and He4) captured in the lattice. In order to check a validity of such a process we performed a new series of experiments using Pd/PdO and Ti foils with increased surface He concentration. The in situ CR-39 measurements during electrolysis were carried out in the cell shown in Fig. 3.
335
Alpha track energy distributions for foreground CR-39 (Pd/Aiumina electrolysis) -Open CR-39
10 15 Alpha energy (MeV) Figure 14. Reconstructed foreground alpha-energy distribution for open and Cu-shielded CR-39 detectors: pay attention to a splitting of alpha "peak" in shielded CR-39 detector.
Experiments showed significant increase in ECPE yields in both He implanted Pd/PdO and Ti foils. The results of ECPE measurements with complex double [Pd/PdO:He] - [Pd/PdO] cathode are presented in Fig. 15.
60Pd/PdO:He side electrolysis Pd/PdO side electrolysis
5040300) XJ
20100
k
LL,. IL.. I j
-
i—•*
6
•»• 10
11
Track diameter (urn) Figure 15. Comparison of ECPE from the P d / P d O : H e and P d / P d O sides of the double cathode (with the background subtracting): E C P E enhancement factors: fc„ = 3.5 and kp =2.0.
As seen from Fig. 15, the ECPE in Pd/PdO:He sample is accompanied by alpha tracks of lower energy (d > 8.0 /zm) ranging from 7.5 to 2.5 MeV are also appeared on Pd/PdO:He detectors, the number of which is found to be at statistically significant level compared with the alpha background in this energy range. This result could be probably explained in terms of He4 distribution in the sample during electrolysis. The main part of lie-atoms is tightly bound at the surface and gives rise to energetic
336
Figure 16.
alpha enhancement. The other part of implanted He due to defect motion stimulated by electrolysis could diffuse in the bulk showing lower energy alpha-emission caused by energy losses in the Pd cathode. On the other hand, the measured enhancement of 1.7MeV protons at Pd/PdO:He side, probably attributed to a change in near-thesurface mechanical properties of the Pd/PdOiH^ sample caused by He implantation. The groups ("hot spots") of energetic alpha particles (Ea ~ 11-15MeV) are appeared at the CR-39 detector attached to the PdO:He face of the cathode. In Fig. 16a, b the microphotograph of such a spot with coordinates [-433, -2285] of 6-charged particle burst is presented (detector #Fg. 1-2/04). This pictures were obtained after the etching of the CR-39 detector during n = 7.0 h (16a) with following additional exposure of this detector in the 6M NaOH at t = 70° C during 7h (in total T2 = 14 h (b)). For comparison, the tracks obtained by the etching of the 11.0 MeV alpha-calibrated CR-39 detector (the alpha beam is in normal direction with respect to the surface of CR-39) during the similar time intervals
337
Figure 17. Similar results were obtained during in situ electrolysis of double T i / T i : H e cathode implanted with He-4 ions from one side (Fig. 18): T h e difference between the
35CM
l
I Ti/He side electrolysis •Ti side electrolysis
3025
.,>• 20 CO
\s 15
• o
>|0
10
rj
H
5-
lltiK 7
->.i-U—•
8" 9 Track diameter (um)
10
11
Figure 18. Results of in situ ECPE measurements with the double Ti:He/Ti cathode (with the background subtracting); ECPE enhancement factors: kn = 3.0 and kp = 8.0.
P d / P d O : H e and Ti:He energetic alpha-emission results consists of absence of low energy alpha "'tail" for Ti:He cathode. T h e protons emission enhancement factor for Ti:He face compared t o unimplanted Ti side was found t o b e as large as /,,, = 8. This is much larger t h a n t h a t for P d / P d O : H e (kp = 2) and could be a t tributed to difference in mechanical properties and hydrogen diffusivity in Ti and
338
P d . Despite some differences in P d / P d O : H e and Ti:He E C P E spectra during electrolysis, we found t h a t He 4 ion implantation is able t o enhance t h e E C P E emission at significant level.
4.
Conclusions
Thus, statistically significant number of energetic charged particles in the range, including alphas in the range of 9-16 MeV was detected b o t h with SSB and CR-39 track detectors techniques. T h e energetic alpha-particles accompanied by 1.7/2.8 MeV protons/deuterons are detected only in hydrogen/deuterium loaded metallic targets with a large "affinity" to hydrogen (Ti and P d ) . Notice, t h a t there are no background events was occurred in this energy range of our measurements. Earlier we also showed t h a t E C P E phenomenon has an essentially surface origin and observed only in metals with large hydrogen/deuterium solubility. No E C P emissions were found either in the "cosmic" Background or from the materials with a low hydrogen solubility: Cu, Al, St. steel, AI2O3(electrolysis), T a ( G D ) . All these findings provide a proof t h a t E C P E cannot be referenced to alpha-nuclide contaminations or secondary cosmic rays effects. In this study, we also found t h a t E C P E from the surface of P d / P d O and Ti cathodes could be significantly enhanced by He-4 ion implantation into a nearsurface layer. This discovery demonstrates t h a t presence of low amount of H e 4 in the metals with a high hydrogen solubility is strongly affected the energetic charged particle emissions. In order to obtain some clues to the mechanism of E C P E enhancement induced by He ion implantation we need to choose between two possible models: (1) Coherent energy transfer from DD-reaction sites to the light nuclei in the lattice with their immediate alpha-decay (Ref. 4) or (2) focusing of energy applied to the cathode during the H/D-loading into the some specific lattice sites near surface (the sites of a high internal strain) with further effective acceleration of the light nuclei (p, d and 4 He) by intratomic electric fields (Coulomb explosion). 3 To choose between the mechanisms new experimental d a t a on E C P E from P d / T i D / H loaded metals, involving He-4 and He-3 implanted cathodes are highly desirable. In any case, t h e occurrence of E C P E suggests anomalous energy release via the "active" lattice sites of non-equilibrium metal deuterides/hydrides.
References 1. A. G. Lipson, B. F. Lyakhov, A. S. Roussetski et al, Fusion Technol. 38, 238 (2000). 2. A. G. Lipson, A. S. Roussetski and G. H. Miley, Trans. Am. Nucl. Soc. 88, 638 (2003). 3. A. G. Lipson, A. S. Roussetski and G.H. Miley, in Proceedings of the ICCF-10 (Cambridge, MA, USA, 2003). 4. P. L. Hagelstein, in Proceedings of the ICCF-10 (Cambridge, MA, USA, 2003).
OBSERVATION OF N U C L E A R T R A N S M U T A T I O N R E A C T I O N S I N D U C E D B Y D 2 GAS P E R M E A T I O N T H R O U G H Pd COMPLEXES
YASUHIRO IWAMURA, TAKEHIKO ITOH, MITSURU SAKANO, NORIKO YAMAZAKI, AND SHIZUMA KURIBAYASHI Advanced
Technology
Research
Center,
Mitsubishi
Heavy Industries
Ltd.,
Japan
YASUKO TERADA Japan Synchrotron
Radiation
Research
Institute,
Japan
T E T S U Y A ISHIKAWA Coherent
X-ray
Optics Laboratory,
SPring-8/RIKEN,
Japan
JIROHTA KASAGI Laboratory
for Nuclear E-mail:
Science, Tohoku University, [email protected]
Japan
We have been studying low-energy nuclear transmutations induced by D2 gas permeation through Pd complexes ( P d / C a O / P d ) . We presented experimental results at ICCF9 and ICCF10. In this paper, we report recent progress. Transmutations of Ba into Sm were observed in two cases: with natural Ba on Pd complex samples (a definite result), and with mass 137-enriched Ba (probable). In these experiments, the atomic mass increase was 12 and atomic number increase was six. One of our experimental apparatuses was carried to SPring-8, which is the world's largest synchrotron radiation facility, located at Hyogo prefecture in Japan. Pr was confirmed several times by XRF at SPring-8. Some experiments were done to explore physical structure of the CaO layer. According to a D+ ion beam bombardment experiment performed at Tohoku University, the deuterium density of our Pd complex is one order larger than normal Pd. When we replaced CaO with MgO, we did not obtain any positive results. These results shed light on the role of the CaO layer in the Pd complex.
1. Introduction Anomalous low-energy nuclear transmutation reactions, such as the transmutation of Cs into Pr, have been observed on the Pd complexes, which are composed of Pd and CaO thin film and a Pd substrate. The reactions occur when the Pd complexes are subjected to D2 gas permeation. 1 " 4 Figure 1 shows a schematic of our experimental method. This method can be characterized by the permeation of D2 gas through the Pd complex and the addition of an element that is specifically targeted to be transmuted. 339
340
Permeation of deuterium is performed by exposing one side of the Pd complex to D2 gas while maintaining the other side under vacuum conditions. On the D2 gas side, dissociative absorption causes the D2 molecules to separate into D atoms, which diffuse through the Pd metal toward the vacuum side where they emerge from the Pd metal, combine, and are released as D2 gas. The second feature is the addition of an element targeted to be transmuted. Our sample is a Pd complex composed of bulk Pd on the bottom, alternating CaO and Pd layers, and a Pd thin film on top. After fabricating a Pd complex, Cs, Ba, Sr, or some other element is deposited on the surface of the top thin Pd layer. We can observe transmutation of the added Cs or Ba. In other words, with this composition, we can provide a deuterium flux through the Pd complex on which a target element is placed as a target to be ftransmuted. We perform in situ elemental analyzes of the given elements after D 2 gas permeation, by evacuating the D 2 chamber and using the built in X-ray photoemission spectroscopy (XPS) unit.
D2gas D Permeation
Cs,
Figure 1.
Schematic of the present method.
Let us briefly summarize the experimental results presented so far. The main experimental results are as follows:1-4 (1) Transmutation reactions of Cs into Pr were observed by D2 gas permeation for about lweek through Pd complexes. The D 2 gas pressure was about 1 atm and the temperature of the Pd complex was nearly 70° C. (2) Transmutation of Cs into Pr was demonstrated in more than 60 cases, with reproducibility close to 100%. (3) Transmutation of Sr into Mo was observed three times after D 2 gas permeation for 2 weeks. The isotopic composition of all detected Mo was different from the natural isotopic abundance of Mo. (4) The Pr was crosschecked by various methods such as XPS, TOF-SIMS (time of flight secondary ion mass spectrometry), XANES (X-ray absorption near
341
edge structure), XRF, and ICP-MS (inductively coupled plasma mass spectrometry). (5) Based on an analysis of the depth profile of the Pr, a very thin surface region up to 100 seemed to be active transmutation zone. (6) Experimental results suggested that the conversion rate from Cs into Pr, which is the ratio of detected Pr to Cs, was positively correlated with deuterium flux through Pd complex. In this paper, we describe the following recent progress and results: (1) transmutations of Ba into Sm, (2) confirmation of Pr by X-ray fluorescence (XRF) spectrometry at SPring-8, (3) some experiments relating to the role of CaO layer in the Pd complex. 2. Experimental The experimental method and setup are basically the same as before.1_4 Therefore, we shall omit a detailed description, and describe only the changed and improved points of the experiment.
Photoelectron energy analyzer X-ray gun
Pd complex with an elements (Cs, Sr, Ba, etc.)
Pd complex test piece *• Evacuation Chamber B
/~\
B-A gauge B-A gauge
D 2 gas
Ge detector
RP
(a)
(b)
Figure 2. Schematic view of experimental setup: (a) semi-in-situ measurement apparatus with XPS and (b) ex situ measurement apparatus without XPS.
Originally, we used an experimental apparatus with XPS (X-ray photoelectron spectrometry) shown in Fig. 2a. Elemental changes on Pd complexes were measured by XPS without taking them out of the vacuum chamber, to prevent contamination from outside of the chamber. It is necessary to evacuate the D2 gas during XPS measurement, because XPS does not work when the gas is present. This does affect the environment in the chamber; so strictly speaking, this should not be called an "in situ" method, although the Pd complexes are kept at the same position during experiments. It might be called a "semi-in-situ" method.
342
We introduced an additional permeation apparatus without XPS shown in Fig. 2b. Using this apparatus, only external ("ex situ") measurements are possible, with instruments such as ICP-MS, SIMS, and XPS. Figure 3 shows the experimental setup for in situ measurement at SPring-8. We developed this apparatus and carried to SPring-8, which is the world's largest synchrotron radiation facility, located in the west part of Japan. This setup enables us to observe elemental changes during D 2 gas permeation by XRF. In the case of SPring-8 experiments, Cs was deposited by the ion beam implantation method (voltage: 5kV, dose: (2.5-5) x 10 14 /cm 2 ). We permeated D 2 gas through a Pd complex with Cs for 10-14 days. D 2 gas pressure is about 170 kPa and the temperature was 70° C. XRF was performed during D 2 permeation in situ at the beginning and the end of the experimental runs. Detector , Be window
i-M—
Evacuation
3L - i7X„
C1 filter Fluorescence X-ray
SOR X-ray-
U'-vtf'r
Vacuum system
Evacuation
fhi-il'. i *..-
«h
(b)
Figure 3. Experimental set-up for the in situ measurement located at the SPring-8 synchrotron laboratory, BL-37XU beamline. (a) schematic of in situ measurement apparatus and (b) photograph of the equipment we brought to SPring-8.
3. Results and Discussion Let us describe Ba transmutation experiments. Natural Ba was deposited on some samples using the electrochemical method, in a 10 mM Ba(OH) 2 solution. On other samples, a special form of Ba with enriched 137 Ba was deposited, in a 7.3 mM Ba(N0 3 ) 2 solution. Applied voltage was I V and deposition time was 10 s, the same as the Cs and Sr experiments. Figure 4 shows XPS spectra for a Pd complex after deuterium permeation lasting 2 weeks, starting with natural Ba. The full XPS spectrum is shown in Fig. 4a. Peaks for Ba and Sm 3d and Sm 4d can be seen. Figure 4b shows the Sm 3d spectra. Measurements were performed twice to test measurement reproducibility. Clear Sm spectra were obtained in both measurements. In order to investigate the Sm isotopic distribution, we analyzed the detected Sm by SIMS. The natural abundance of Sm and the SIMS spectrum of the Sm
343
found on the Pd complex are shown in Fig. 5a, b, respectively. Natural Sm has seven isotopes; the most abundant is 152 Sm. The Sm spectrum on the complex was quite different. This clearly was Sm, as shown by the XPS spectra. Figure 5b shows data from a Pd complex with natural Ba on the surface after D2 permeation (marked "Used"), and for a complex that has not been permeated ("Unused").
200 400 600 800 1000 1200 1400
1070 1080 1090 1100 1110 1120 1130 1140
Binding energy (eV)
Binding energy (eV)
(a)
(b)
Figure 4. Detected Sm XPS spectra after D2 gas permeation through a Pd complex deposited with natural Ba; (a) full XPS spectrum and (b) XPS spectra for Sm 3d. (Measurements were performed twice to confirm measurement reproducibility.)
10° ,0
144
Sm
147
Sm
,48
Sm
149
Sm |15 °Sm
152
Sm
154
Sm
Ba
10* ,u
Used 3.2% .15.1% 11.3% 13.8% 7.5% 26.6% 22.5%
Sm natural abundance!
Sm
Unused
i38 B a 0
71.7%.
o 10J o O lO'
,
11.3%
'24%66^%
144 145 146 147 148 149 150 151 152 153 154 Mass number
10' 135
140
145
150
155
Mass number (b)
Figure 5. SIMS spectrum for detected Sm; (a) natural abundance of Sm and (b) SIMS spectra of detected Sm ("Used" indicates a Pd complex with natural Ba after D2 permeation, and "Unused" indicates a Pd complex with natural Ba that has not been permeated with D2).
Let us consider these spectra in Fig. 5b, using Table 1 that examines the effects of molecular ions. The 138 Ba signal for unused and used samples does not match.
344
Table 1.
Examination of molecular ions.
Pd
Pd 4 0 Ca
Ba
Ba 1 6 0
102 (1%) 104 (11%) 105 (22%) 106 (27%) 108 (26%) 110 (12%)
142 144 145 146 148 150
130 (0.1%) 132 (0.1%) 134 (2.4%) 135 (6.6%) 136 (7.8%) 137 (11.3%) 138 (71.7%)
146 148 150 151 152 153 154
We assume this is because the Ba deposition is not uniform. Pd 4 0 Ca molecular ion peaks are the same in the unused and used samples. Both 1 1 0 Pd (12%) 40 Ca, and 134 Ba(2.4%) 16 0 are candidates for mass 150, however their signals should be lower than 106 Pd(27%) 40 Ca and 138 Ba(71.7%) 16 0. The SIMS data shows that mass 150 for used sample cannot be explained by 1 1 0 Pd 4 0 Ca and 1 3 4 Ba 1 6 0. Next, we consider the effect of the 12 C ion. Mass 150 can be created by combining 138 Ba and 12 C. If 138 Ba 12 C is created, then 137 Ba 12 C (mass 149) and 136 Ba 12 C (mass 148) should appear. However, we do not observe any increase of mass 149 and 148 in the used sample. This indicates that BaC molecular ions have no effect on SIMS spectra. Therefore the large mass 150 in the used sample cannot be explained by 138 Ba 12 C formation. Based on these above SIMS considerations and XPS results, it seems clear that mass 150 in the used sample is derived from Sm. This strongly suggests that 150 Sm exists on the Pd complex after D2 gas permeation. In the case of the mass 137-enriched Ba sample, we could not obtain a clear XPS spectrum. However, we obtained SIMS data that showed an increase in mass 149. Figure 6 shows two SIMS spectra for Pd complexes with 137 enriched Ba after D2 permeation. An increase in mass 149 of about one order of magnitude was observed for both experiments 1 and 2. Table 1 shows that mass 149 cannot be created by Pd 4 0 Ca and B a 1 6 0 . 137 Ba 12 C also cannot be the cause of the increase, for the same reason. These facts imply that 149 Sm exists on the Pd complex, when we consider that Sm spectra were obtained by XPS using natural Ba. 149 Sm was probably detected after D2 permeation through the Pd complex. Figure 7 shows the mass correlation between the starting and final elements on the complex surface. If we put 138 Ba on the complex we obtain 150 Sm. And if we put 137 Ba on the Pd complex, we obtain 149 Sm, assuming the mass 149 increase of the SIMS spectra are caused by Sm. Observed transmutation reactions of Ba into Sm belong to the category of mass 12 (atomic number 6) increase reactions. Nuclear transmutation induced by our experimental method have also produced mass 8 (atomic number 4) increases, such as Cs —> Pr, and Sr —> Mo. The aim of Ba transmutation experiments is to investigate the mechanism of the present transmutation phenomena by the nuclear resonance scattering. 149 Sm is a Mossbauer isotope and its excitation energy is 22.5 keV. If we measure the Mossbauer effect of 149 Sm by synchrotron orbital radiation, we will obtain clear
345
(Enriched Ba^ D ->
(Enriched Ba)<
1000 "Ba
Pd Pd CaO
"Ba
Pd Pd CaO
100PcTCa
,a
,9
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Sm
100
Used Unused
BaO
O
10
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O 10
• .' |
I
J
|
,
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•)'! .
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Mass number
(a)
(b)
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F i g u r e 6. S I M S s p e c t r a for P d c o m p l e x e s w i t h 137 e n r i c h e d B a after D2 g a s p e r m e a t i o n ; s p e c t r u m for e x p e r i m e n t 1 a n d (b) s p e c t r u m for e x p e r i m e n t 2.
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4
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56
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Y#
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wmm**
element
ou
elements
Sm
500 5000, M + 12
/, ,.
*
Z+6
133 134 135 136 137 138 139 1500f
"
a
.-*
0 * 146
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148
149
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Ba «'
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6d
. 149
« ~* 56
1000; Given element
161
100
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150
,.„ Sm 62
80 ; 60
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elements FG. BG.
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134
F i g u r e 7.
135
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137
138
139
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149
150
151
M a s s c o r r e l a t i o n b e t w e e n t h e e l e m e n t s in t h e U n u s e d a n d U s e d s a m p l e s .
evidence of generation of 149 Sm and the information on the ultra fine structure relating to the electronic state and phonon of the generated 149 Sm. The authors are now examining and planning some experiments in collaboration with the researchers of University of Tokyo. Let us move to the next results: Pr confirmation by XRF and experiments with in situ measurement at SPring-8. Ex situ detection of Pr by XRF using SOR Xray at SPring-8 is shown in Fig. 8. All the permeation experiments in this figure
346
were performed in XPS apparatus. Data marked "Used 1" and "Used 2" are from samples after D2 permeation, and "Unused" data is from a sample that did not undergo permeation. The Pr-L lines are clear in both Used samples, while no Pr peak was seen in the Unused sample. Conversion rates from Cs to Pr are high, and Cs-L lines have almost vanished in the two Used samples. 12x103 10
o O
6~ 4-
• Used 1 Usedl
V^
• Unused L,
0
1
2
3
4
5
6
X-ray energy (keV) Figure 8. Ex situ detection of P r by X R F using SOR X-ray at SPring-8, Hyogo, Japan (Used 1, Used 2: data from Samples after D2 Permeation. Unused: data from a sample before permeation).
35 36
Cs-L a 1 Cs-L p1
200 -• Pr-L r
150
1
«
Is.*"
A. •«
100
sV-
•"••7
* *
•
Pr-L f
50 Energy (keV) Figure 9.
An example of Pr detection by in situ experiments at SPring-8.
The XRF spectrometry was performed using the experimental setup shown in Fig. 3, both during D2 permeation in situ and at the beginning and end of experiments. No Pr was observed in three Used samples.
347
Pr was detected in three Used samples with normal complexes, whereas no Pr was observed in an experiment without a CaO layer. Figure 9 shows a sample spectrum. Surface distributions of XRF spectra were observed using a 1-mm2 Xray beam. A clear Pr spectrum can be seen at the point 35 shown in Fig. 9. Pr spectra were obtained at some locations, however, no Pr was found in location 36. This indicates uneven distribution of Pr on the complex surface. The next topic is the role of CaO layer in Pd complex. Depth profiles of Cs and Pr were plotted in Fig. 10. Both TOF-SIMS and XPS analyzes were applied, as shown in Fig. 10a and b. Cs was injected into all the Pd complex samples by the ion implantation method. The relation between the sputtering time and the real depth was estimated in advance using a Pd thin film on Si substrate; thickness of the Pd thin film is known. These measurement shows that a 200 s in the case of TOF-SIMS and a 4min sputtering time in the case of XPS correspond to 10 nm. Figure 10a was already shown at ICCF10. Cs and Pr depth profiles for the Pd complex without permeation show normal results in Fig. 10. Cs decreases continuously from the surface and there is no Pr in the background samples. On the other hand, the depth profile estimated by XPS also supports that Cs transmutation reaction into Pr occurs in the near surface region up to 10 nm. We can see that there is Cs, which is the same order as given Cs, in the near surface area. Cs depth profiles for the foreground and background samples agree in the deep area. Figure 10 also shows that Cs atoms do not diffuse and migrate with D 2 gas permeation under our experimental conditions. Therefore, it is very difficult to imagine that the detected Pr was a concentrated impurity, and not a transmutation product. If we could assume that Cs transmutation occurred in the near surface region up to 10 nm, direct electronic effect on the region by CaO layer in 40 nm depth might be difficult. 100A 8.0x10 NoD After D
•
Pr '
a
, 1.2 |
0.8'
omi
Pr
*
. 0.0
1.0
•s 0.6 nJ 0.4, o
•
Q 2.0x10
%)P
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top
Js
S •-
»
«
*S
»
•
*
200 400 600 800 1000 Sputtering time (sec) (a)
0.2
4
10 nm « •
* w*
«
Unused Cs Used Cs Used Pr
* • «* '""."• m*
< o.o0
2
" »«
4 6 8 10 12 14 16 18 Spu Sputtering time (min)
(b)
Figure 10. Depth profile of Cs and Pr for samples after D2 permeation and without permeation; (a) based on TOF-SIMS measurement and (b) based on XPS measurement.
348 1000
800-
600 I-
> CD
400 h
200
0.01
Figure 11.
0.1
„„
,
/i D (10 22 /cm 3 )
1
10
Density measured by D+ ion bombardment experiment at Tohoku University.
D + ion bombardment experiment was performed at Tohoku University using a Pd complex. Low-energy D + ion beam from 2.5 to 10 keV irradiates the surface of metal and induce D(d,p)T reactions. Proton yield obtained AE-E counter telescope and its energy dependence enable us to estimate screening potential and deuterium density.5 Figure 11 shows that deuterium density of Pd complex(Pd/CaO) is one order larger than normal Pd. When we replaced CaO with MgO, we did not obtain any positive results. It means that MgO cannot work instead of CaO. Two cases out of two experiments using MgO show no Pr by ICP-MS measurements, although D2 gas flow rates were enough (2-3 seem) in both cases. On the other hand, almost every time Pr was detected if we use Pd complex with CaO. At present the authors do not have definite explanation for the role of the CaO layers. We cannot perfectly exclude out the possibility that CaO layers modified the electronic state of top Pd layer. However, it could be possible to consider that the CaO layers cause the increase of deuterium density according to the result of the bombardment experiment. Anyway, we should make clear how CaO layers work in further studies. A resonance nuclear reaction would give us precise depth profile deuterium near surface.6 Hydrogen depth profiles have already been established and measuring deuterium depth profile technique should be developed. We are planning with the researchers of University of Tokyo to utilize the 7Li and deuterium reaction.
349
There is no complete theory t h a t can explain the experimental results without any assumptions, however, some interesting models and theories have been proposed. 7 ~ 9 T h e observed t r a n s m u t a t i o n processes must belong to a new category of nuclear reactions in condensed matter. Therefore much more theoretical investigation is necessary. 4. Concluding R e m a r k s Transmutations of B a into Sm were observed natural B a as t h e starting material on P d complex samples, and possibly with mass-137 enriched Ba. This indicates t h a t we obtained a mass distribution of Sm depending on t h e starting isotopic distribution of Ba. One of our experimental apparatuses was carried to SPring-8 cyclotron facility, where it was used for in situ measurements, and where we obtained some P r signals by the X R F method. According to a D + ion b e a m bombardment experiment performed at Tohoku University, deuterium density of our P d complex indicated one order larger t h a n normal P d . Positive replication results were obtained not only in a gaseous environment 1 0 presented by Prof. A. Takahashi et at, b u t also in an electrochemical environment 1 1 performed Dr. F . Celani's team. Researchers at t h e Naval Research Laboratory are now planning a replication of t h e experiments t h a t produced transmutations of Cs into Pr. Acknowledgments T h e authors would like to acknowledge Prof. A. Takahashi, Prof. T. Okano, Prof. K. Fukutani, Dr. F . Clelani, Dr. K.S. Grabowski, Prof. M. Melich, Dr. G.K. Hubler, Prof. K. Okuno, Dr. Z. Yoshida, Prof. S. Tanaka, and Dr. I. Tanihata, for their valuable discussions. X R F experiments in this work were performed at t h e BL37XU in t h e SPring-8 with t h e approval of t h e J a p a n Synchrotron Radiation Research Institute (JASRI) (Grant No. 2004B0456-NXb-np). References 1. Y. Iwamura, M. Sakano, and T. Itoh, Elemental analysis of Pd complexes: effects of D 2 gas permeation, Jpn. J. Appl. Phys. 4 1 , 4642-4648 (2002). 2. Y. Iwamura, T. Itoh, M. Sakano, S. Sakai, and Kuribayashi, Low-energy nuclear transmutation in condensed matter induced by D 2 gas permeation through Pd complexes: correlation between deuterium flux and nuclear products, in Proceedings of the ICGF10, 24-29 August 2003 (Cambridge, USA), to be published, see http://www.lenrcanr.org/. 3. Y. Iwamura, T. Itoh, M. Sakano, and S. Sakai, Observation of low-energy nuclear reactions induced by D 2 gas permeation through Pd complexes, in Proceedings of the ICCF9, 19-24 May 2002 (Beijing, China), pp. 141-146. 4. Y. Iwamura, T. Itoh, and M. Sakano, Nuclear products and their time dependence induced by continuous diffusion of deuterium through multi-layer palladium containing
350
5.
6.
7. 8. 9. 10. 11.
low work function, in Proceedings of the ICCF8, 21-26 May 2000 (Lerici, Italy), SIF Conf. Proc. vol. 70, pp. 141-146. J. Kasagi, H. Yuki, T. Baba, T. Noda, T. Ohtsuki, and A.G. Lipson, Strongly enhanced DD fusion reaction in metals observed for keV D-1" bombardment, J. Phys. Soc. Jpn. 7 1 , 2881-2885 (2002). K. Fukutani, M. Wilde, and M. Matsumoto, Nuclear-reaction analysis of H at the P b / S i ( l l l ) interface - Monolayer depth distinction and interface structure, Phys. Rev. B64, 245411 (2001). A. Takahashi, Deuteron cluster fusion and related nuclear reactions in metaldeuterium/hydrogen systems. Recent Res. Dev. Phys. 6, 1-28 (2005). A. Takahashi, Mechanism of deuteron cluster fusion by EQPET model, in Proceedings of the ICCF10, to be published, see http://www.lenr-canr.org/. T.A. Chubb, Bloch nuclides, iwamura transmutations, and oriani showers, in Proceedings of the ICCF11, in press. T. Higashiyama, et al, Replication of MHI transmutation experiment by D2 gas permeation through Pd complex, in Proceedings of the ICCF10, in press. F. Celani, et al, Thermal and isotopic anomalies when Pd cathodes are electrolysed in electrolytes containing Th-Hg salts dissolved at micromolar concentration in C2H5OD/D2O mixtures, in Proceedings of the ICCF10, in press.
D E U T E R I U M ( H Y D R O G E N ) FLUX P E R M E A T I N G T H R O U G H PALLADIUM A N D C O N D E N S E D M A T T E R N U C L E A R SCIENCE
QING M. WEI, BIN LIU, YU X. MO, XING Z. LI, SHU X. ZHENG, AND DONG X. CAO Department of Physics, Tsinghua University, Beijing 100084, China XIAO M. WANG Institute of Plasma Physics, Chinese Academy of Science, Hefei 230031, China JIAN TIAN Life Science School, ChangChun University of Science and Technology, ChangChun 130022, China Deuterium (hydrogen) flux permeating palladium has been analyzed using mass spectroscopy (SRS RGA200) in a new apparatus. The "mass 6" component has been confirmed again. It is found that Langevin rate of Dg generation in the mass spectrometer plays an important role. However, "mass 6" component cannot be attributed to Dg only. The palladium plays an important role as well. The mixture of deuterium and hydrogen gas has been used to test the prediction of resonant tunneling theory as well.
1. Introduction Deuterium (and hydrogen) flux and condensed matter nuclear science has been an interesting subject since ICCF-9 (Beijing, China, May 2002).^ 3 During ICCF-10, (Cambridge, MA, USA, August 2003) the correlation between the deuterium flux and the heat flow was reported. 4 After ICCF-10, a deuterium flux experiment was conducted at Institute of Engineering Application Research, USA (IEAR) to detect the heat and the nuclear products. The preliminary experimental results were reported at The fifth Asti Workshop on anomalies in hydrogen/deuterium-loaded metals 5 (March 2004). It was reported that the temperature gradient in the radial direction of Pd disk was reversed when the deuterium flux was permeating through a thin palladium disk. The mass spectroscopy data showed that a "mass 6" component appeared in the deuterium gas permeating through the thin palladium disk. It is desirable to confirm this "mass 6" component and analyze this component. Particularly, the tritium production would be a test of the selective resonant tunneling theory, because the selective resonant tunneling theory predicts more tritium production if the mixture of deuterium and hydrogen gas were used instead of pure deuterium gas. 351
352
2. Confirmation of "Mass 6" C o m p o n e n t The mass spectrometer at IEAR was sensitive enough to detect the "mass 6" component in the deuterium gas passing through the thin palladium disk; however, that mass spectrometer worked only before and after the operation of the apparatus. An advanced mass spectrometer (SRS RGA200) was applied in this new apparatus at Institute of Plasma Physics, Hefei, China. This mass spectrometer was able to measure the "mass 6" component on-line along with other mass numbers. The new apparatus used a long thin palladium tube (<j> 3 mm x 0.08 mm x 140 mm) instead of the thin palladium disk used at IERA ( 20 mm x 0.1 mm) in order to increase the Pd surface area. An electrical heater was installed at one end of the Pd tube, and the other end of the thin Pd tube was blocked (Fig. 1). When deuterium gas was fed into the Pd tube, the deuterium flux permeating through the thin Pd wall was analyzed by a mass spectrometer (SRS RGA200) when the Turbo-molecular pump kept the pressure lower than 1 0 - 2 Pa.
Heater
RGA \iJLJJ
PKR251 \\f
I
Vacuum chamber
HV(015O)
\ C M ™p(450l/s) RP (4 l/s)
Figure 1.
Schematic of new apparatus.
353
Figure 2 shows clearly that "mass 6" component is one of the components growing with the deuterium flux. The upper line represents the "mass 4" component. It increased in steps because the heating power in the electrical heater increased in steps. The highest temperature near the heater was about 140°C. The occurrence of a "mass 6" component in the IEAR experiment was again confirmed in this experiment. In addition, this on-line measurement shows clearly that the "mass 6" component increases much faster than any of the other components (masses 1-5 and 7). The mass 7 component stays very low; hence, we can eliminate the possibility of lithium contamination here (the natural abundance ratio for Li-7 to Li-6 is more than 12). We have to distinguish the contribution from the D^ ion to the "mass 6" component from a possible T^ ion contribution in order to find the signal we are searching for. Mass 1-7 varies with time (D 2 + Pd, 2004-7-7)
: Me = 4 • 0.01 -.
I
• Me = 3-5 <Me = 2 " •Me=6" »Me = 1 1
•Me=5_
1E-5
- Me = 7 :
" *
1— ' 36000
I 38000
•
1 40000
•
1 42000
1
'
44000
1 46000
'
1
•—
48000
Time (s) Figure 2.
The confirmation of mass 6 component, and its rapid growth with deuterium flux.
3. Langevin Rate in Mass Spectrometer It is well known that the D 3 neutral molecule is unstable; hence, there is no way to ionize the D 3 neutral molecule inside the mass spectrometer to produce Djj". However, there was another process to produce the signal of Dij". Early in 1905, Langevin6 found that there was a large generation rate of D^" through the reaction: 7-9 D++D2^D++D-r-1.7eV
(1)
the D 2 ion inside the mass spectrometer may polarize the neutral D2 molecule and dissociate it. As a result, D^" was generated as a secondary process inside the mass spectrometer. Since it is an exothermic process, the cross-section of reaction (1)
354
might be much greater than that of the collision between two neutral molecules by a factor of 10-100. This Langevin rate explains observed "mass 6" component here and in early IEAR experiments, because the ionized D2 molecule might trap another neutral D2 molecule easier when the density of D2 molecule is getting higher and higher. This Langevin rate may be confirmed by two facts: (1) the "mass 6" persists while using the D 2 gas without Pd tube, (2) the quadratic dependence of "mass 6" on "mass 4". When D2 gas was fed directly into the mass spectrometer without permeation through a Pd tube, the partial pressure of various components decreased with time due to the pumping in the line of spectrometer. Figure 3 shows the changes of "masses 4, 2, and 6", respectively. The steps in Fig. 3 were caused by an interruption near 43000 s when the spectrometer was switched to another mode in order to measure the whole mass range (masses 1-200). Figure 3 shows that even if there is no Pd tube, the "mass 6" component might be as high as 10% of the "mass 4"component when "mass 4" is more than 0.03 Pa. Thus "mass 6" cannot be attributed to the occurrence of T j as expected.
1
40000
'
1
42000
*
1
*
1
44000 46000 Time (s)
•
1
48000
«
)
50000
Figure 3. Mass 6 appeared in mass spectrometer even if the deuterium gas has not been permeating through a thin wall of Pd tube.
Figures 4 and 5 show the dependence of "mass 6" on "mass 4" for the cases of using Pd tube and without Pd tube, respectively. A similar quadratic dependence on "mass 4" was observed in both cases. This implies that the "mass 6" component was mainly generated inside the mass spectrometer in terms of Langevin rate.
355 D + Pd, 2004-7-7 1
0.00018-
m
0.000160.00014-
>
1 "'»""(
(
"
i
1
•
i
•
t
'
I
i
I y *
Data points Quadratic fit
y = -7.10914E - 6 + 0.00377X + 0.35837X2
M
-
0.00012"5" S> 0.00010-
•
<0 •
1 0.000085 0.00006 -
, -
0.00004-
-
0.00002 -
-
0.00000 0.000
0.002
0.004
0.006
0.008
0.010 0.012 0.014 0.016 0.018 0.020
Mass 4 (Pa)
Figure 4.
Mass 6 varies with mass 4 quadratically as Langevin rate.
3.1. The Role of Pd In order to eliminate the Langevin rate of Djj" generation, we might search the low "mass 4" region where the quadratic dependence might suppress the Langevin rate. Figure 6 shows the results when the mixture of H 2 and D2 gases was fed into the Pd tube. At 33,720 s, the heater was turned on, masses 1-4 were all increasing with time due to the enhanced flux permeating through the thin wall of Pd tube, but
0.0014Data points
0.0012-
Quadratic fit Y= 7.79058E - 6 - 0 . 0 0 1 9 5 X + 0.84493X 2
0.0010co
0.0008-
0.0006 •
0.0004-
0.0002 •
0.0000-
Figure 5.
- 1 — 0.04
Mass 6 dependence on mass 4 in the case of having no Pd.
356
masses 5 and 6 were decreasing first. This "mass 6" dependence on "mass 4" is very different from the quadratic Langevin rate. This dependence appeared only when the mixture of H 2 and D 2 gases was fed into the Pd tube. We did not observe such dependence when the mixture of H 2 and D 2 gases was fed directly into the mass spectrometer, or when the D 2 was fed into the Pd tube. Although it is not easy to judge what the "mass 6" component is, we can be sure this "mass 6" was not generated inside the mass spectrometer. The Pd tube played important role here, and H2 gas played important role here as well. A plausible explanation based on the selective resonant tunneling model 1 0 - 1 5 is that p+ d
3
—> RESONANT TUNNELING
He*+ek
—>
T + ve.
(2)
K-ELECTRON CAPTURE
As a result of resonant tunneling, the He-3 excited state was formed as an intermediate state first; then, the K-electron capture would turn He-3 into tritium. 16 The tritium ion, Tj", formed a part of the "mass 6" component in mass spectroscopy.
33000
34000
35000
36000
37000
Time (s)
Figure 6. When the mixture of H2 and D2 gas was fed into the Pd tube, mass 6 decreased at low mass 4 region when mass 4 increased.
4. Detection Limit It is important to discuss the detection limit, if the triton was formed in process (2). The pumping rate of the turbo-molecular pump is 4501/s having considered the conductance of the system, the effective pumping rate is about 2501/s. The detection limit of this mass spectrometer is about 10~ 7 Pa; hence, the detection limit of the generation rate of "mass 6" is about 2.5 x 10~ 5 Pa-l/s which is about 10 11 triton/s. This is a rather high rate of triton generation in usual condensed matter nuclear
357 science experiments. (F. Will's early electrolytic experiment 1 7 generated tritons at an average rate of 2 x 10 5 t r i t o n / s / c m 2 ) . In order t o enhance the rate of triton generation, we might enhance the deuterium flux. However, the mass spectrometer was not able to work when the pressure was higher t h a n 10~ 2 Pa; hence, the maximum D 2 flux was limited to 2 . 5 P a - l / s . Consequently, we have to develop a new a p p a r a t u s which is able t o detect much lower triton generation rate under a heavy deuteron back ground, or circulate the gas in the system in order to accumulate the number of tritons.
5. F u t u r e E x p e r i m e n t A new mass spectrometer has been developed in the department of physics at Tsinghua University. It combined the time-of-flight mass spectrometer with a laser stimulated fluorescence spectrometer. Hence, not only is the sensitivity greatly enhanced, but also the light emission would provide a new criterion to distinguish the T j from D + . Hopefully, this new system would produce the evidence of the correlation between deuterium flux, excess heat, and the nuclear products.
Acknowledgments This work is supported by T h e Ministry of Science and Technology (Fundamental Division), Natural Science Foundation of China (#10145004) and Tsinghua University [Basic Research Fund (985-1)]. We are grateful to T h e Institute of P l a s m a Physics for providing enssential assistance during this experiment.
References 1. X.Z. Li, et al., Pumping effect - reproducible excess heat in a gas-loading D / P d system, in Proceedings of the ICCF-9 (Beijing, China, May 19-24, 2002); X.Z. Li (Ed.) (Tsinghua University Press, 2003), p. 197. 2. X.Z. Li, B. Liu, et al, Super-absorption - correlation between deuterium flux and excess heat, in Proceedings of the ICCF-9 (Beijing, China, May 19-24, 2002); X.Z. Li (Ed.) (Tsinghua University Press, 2003), p. 202. 3. X.Z. Li, J. Tian, et ah, Correlation between abnormal deuterium flux and heat flow in a D / P d system, J. Phys. D: Appl. Phys. 36, 3095-3097 (2003). 4. X.Z. Li, et al., Progress in gas-loading D / P d systems: the feasibility of a self-sustaining heat generator, in Proceedings of the ICCF-10 (Cambridge, USA, September 19-24, 2003). 5. X.Z. Li, B. Liu, Q.M. Wei, G.L. Schmidt, and J. Tian, Anomalies correlated with abnormal deuterium flux and heat flow in D(H)/Pd systems, in W.E. Colfis (Ed.), Proceedings of the Fifth Asti Workshop on Anomalies in Hydrogen/Deuterium Loaded Metals (Asti, Italy, March 19-21, 2004). 6. P. Langevin, Ann. Chem. Phys. 5, 245 (1905). 7. H. Eyring, J.O. Hirschfelder, and H.S. Taylor, The theoretical treatment of chemical reactions produced by ionization processes, J. Chem. Phys. 4, 479 (1936). 8. D.P. Stevenson and D.O. Schissler, Reactions of gaseous molecule ions with gaseous molecules. IV. Experimental method and results, J. Chem. Phys. 29, 282 (1958).
358 9. G. Gioumousis and D.P. Stevenson, Reactions of gaseous molecule ions with gaseous molecules. V. Theory, J. Chem. Phys. 29, 294 (1958). 10. X.Z. Li, Overcoming of the gamow tunneling insufficiencies by maximizing a dampmatching resonant tunneling, Czech. J. Phys. 49, 985 (1999). 11. X.Z. Li, J. Tian, and M.Y. Mei, Fusion energy without strong nuclear radiation, J. Fusion Energy 18, 51 (1999). 12. X.Z. Li, et al., Maximum value of the resonant tunneling current through the coulomb barrier, Fusion Technol. 36, 324 (1999). 13. X.Z. Li, J. Tian, M.Y. Mei, and C.X. Li, Sub-barrier fusion and selective resonant tunneling, Phys. Rev. C61, 024610 (2000). 14. X.Z. Li, et al., Nuclear physics for nuclear fusion. Fusion Sci. Technol. 4 1 , 63 (2002). 15. X.Z. Li, et al., Study of nuclear physics for nuclear fusion, J. Fusion Energy 19, 163 (2002). 16. S. Chen, X.Z. Li, et al., Low energy P + D fusion reaction in selective resonant tunneling model, in Proceedings of the IGCF-9 (Beijing, China, May 19-24, 2002); X.Z. Li (Ed.) (Tsinghua University Press, 2003), p. 42. 17. F.G. Will, et al., Studies of electrolytic and gas phase loading of palladium with deuterium, in Proceedings of the Second Annual Conference on Cold Fusion, The Science of Cold Fusion (Como, Italy: Societa Italiana di Fisica, Bologna, Italy, 1991).
P R E C U R S O R S A N D T H E F U S I O N R E A C T I O N S IN POLARIZED P d / D - D 2 0 SYSTEM: E F F E C T OF A N E X T E R N A L ELECTRIC FIELD
S. S Z P A K , P. A. M O S I E R - B O S S , A N D F . E. G O R D O N SPAWAR
Systems
Center
San Diego, San Diego, CA 92152-5001,
USA
The effect of an external electric field on the physical appearance of the P d / D electrode in an operating cell is discussed. It is shown that the individual globules of the "cauliflower-like" structure undergo a shape change exhibiting two distinct features, viz those that require energy expenditure that can be extracted from the applied external field (e.g., reorientation, separation of individual globules, dendrite formation) and those that require energy expenditure far in excess of one that can be supplied by the electric field alone (e.g., exhibiting features usually associated with the solidification of a molten metal under liquid or the presence of localized catastrophic events leading to the formation of craters). It is shown, by energy-dispersive X-ray method, that the needed energy is provided by nuclear events occurring in the region close to the electrode surface. The nuclear events are of the type: precursor —> unstable nucleus —• stable nucleus.
1. Introductory Remarks Apart from an excess enthalpy generation, there are other reported manifestations of unusual activities in the negatively polarized P d / D - D 2 0 system. 1 Among them (i) changes in surface morphology far greater than those associated with the lattice expansion2 and (ii) accumulation of impurities in the surface (subsurface) region that exceeds the amounts that can be transferred from the cell components during prolonged cell operation. 3 In what follows, we shall demonstrate that both these features are magnified if an operating cell is placed in an external electrostatic field. Furthermore, we shall show that the accumulation of "impurities" is, in fact, the result of nuclear activities yielding elements not originally present. To provide rational interpretation, one must (i) define the system and its initial conditions (i.e., the conditions just before the cell placement in an electric field), (ii) consider the interaction of the field with the system and, in particular, with a conductor, liquid dielectric and the relationship between the surface forces and the bulk response, and (iii) examine the effect of the field on the operation of individual components of the electrochemical cell. 1.1. System
and its
Behavior
An operating cell is viewed as a system consisting of three subsystems, viz the electrolyte, the interphase and the bulk Pd/D. The interphase itself is an 359
360
assembly of non-autonomous layers as defined by van Rysselberghe.4 The electrolyte, an ionic conductor, is treated as a dielectric with added extraneous charges (positive and negative ions). The Pd/D material is a conductor containing, in addition to free electrons, mobile positive particles, the D + complexes. Just before the application of an external field, all intensive state variables are constant in time, i.e., all irreversible processes inside the system occur continuously (there is continuous exchange between the system and surroundings). The processes involved are: reduction of D+/D20 ions/molecules and the evolution of deuterium. The mechanism of these reactions is not important except to say that all operating driving forces remain constant in time. The system's reference state is maintained by an overpotential, rj. The vanishing of all mass fluxes (at the reference state) demands that all chemical potentials be equal. The overpotential acts as an external potential, i.e., it determines the distribution of all mobile charges as well as their electrochemical potentials. The ionization D ^ —> D + , complex and precursor formation occur in an s-electron rich environment, i.e., where q+ < ^ . The IR imaging of the electrode surface shows that excess heat is generated at discrete locations, which, in turn, implies the formation of domains. The existence of hot spots indicates the presence of highly energetic fast reactions, which, in turn, produce pressure and temperature waves travelling through the electrode. Indeed, such waves were observed by the response of a pressure sensitive material onto which the Pd/D films were deposited. 5 1.2. System
Far from
Equilibrium
The characteristics of systems far from equilibrium are: (i) the formation of new structures is always the result of an instability which may be due to either internal or external fluctuations to the system, (ii) fluctuation is always followed by the response which may bring the system to its original conditions or may produce a new structure, (iii) the system's stability is determined by a complex interplay of kinetic and thermodynamic quantities (i.e., no statement can be made that is independent of kinetic considerations), (iv) chemical instabilities lead to spontaneous "self-organization" if the system is able to exchange part of the energy or matter with the outside world in order to establish a microscopic internal order (an open system must be maintained, if self-organization is to occur), and (v) as the overpotential is increased, the probability of cluster formation increases (increase in the rate of formation of hot spots). Parenthetically, in systems far from equilibrium the complexes can be viewed as "supermolecules" where the physical laws, as formulated for systems at or near equilibrium, may not apply. To quote: "... there exist new dynamic states of matter induced by a flow of free energy far from equilibrium. Such states are governed by a new physical chemistry on a supermolecular level, while all laws referring to the molecular level, remain essentially unchanged. In all cases considered, the coherent behavior on the supermolecular level corresponds in fact to an amplification of
361
specific molecular properties (such as kinetic constants) in far from thermodynamic equilibrium conditions" (Ref. 6, p. 290).
1.3. Field Interactions
with Cell
Components
1.3.1. Conductors Introduction of an uncharged conductor into the field reduces the total energy of the field. An uncharged conductor located outside the field is attracted towards the field. A conductor, charged or not, when placed in an electric field cannot remain in stable equilibrium. Consequently, if a conductor is constrained then it will suffer shape change, either reversible or permanent, depending upon conditions at the surface and the time involved.
1.3.2. Electrolyte The electrolyte phase contains mobile positive and negative ions distributed in a manner that assures charge neutrality (except at boundaries). It is known that an ion in contact with water is solvated, which means that the central ion is surrounded by an oppositely charged ionic cloud. When subjected to an electric field, each ion is acted upon with a net force representing the difference between the accelerating force arising from the applied field and the opposing forces, viz (i) the electrophoretic contribution associated with the structure of the moving entity and (ii) the force connected with the relaxation of the ionic cloud.7
1.3.3. Interphase Charging of the Pd lattice with hydrogen isotopes by electrochemical means occurs through a number of consecutive processes, i.e., charge transfer, adsorption, absorption, etc. These processes define the thermodynamic structure of the interphase (as opposed to its physical structure). The set of processes involved is as follows: D+ ( b ) -+ D+ (r) -^ D e - • D D « - D [(D+ • e") n - D+] denoting charge transfer, adsorption, absorption, placement in Pd lattice, ionization, complex formation.8
1.3.4. The Bulk Pd/D Any charge on a conductor must be located at its surface. Charged mobile species (D+ complexes) are also present in the bulk Pd/D material. In general, they will not be affected by an external field, since no field can exist there. However, in the present case, they might be affected by the field generated by the flow of the cell current, i.e., the electrodiffusion might occur.
362
1.3.5. Internal Stresses - Shape Change The relationship between the surface forces and the bulk response is given by / d iivvAA&dTr = p ,Anda,
(1)
where the div operator derives a vector from tensor. The term on the left-hand side term is the algebraic sum of all sources/sinks continuously distributed over the volume element. The right side defines the outflow, if positive and the inflow, if negative. Equation (1) indicates that forces acting on any finite volume in a body can be reduced to forces applied to the surface of that volume and vice versa. Consequently, it follows that the shape change at constant volume is associated with motion due to internal forces acting on the surface. Thus, the deformation will be determined by the distribution of surface forces, while the rate of deformation by their magnitude. Internal stresses can be present without the presence of external loads, e.g., due to inhomogeneities, imperfections, etc., a likely situation in the codeposited film and the continuous evolution of deuterium.
1000 - 3000
Vcm-1 —
•
Figure 1. An electrochemical cell. 1 - clear plastic (acrylic) wall. 2 - P t screen. 3 - Co-deposited PdD layer. 4 - Au foil. 5 - Cu foil. Cell connected to a galvanostat; electric field maintained by a regulated high voltage source (not shown).
1.3.6.
Location/Size
The presence of discrete, randomly distributed sites (hot spots, craters, boulders, etc.) implies the existence of volumes within the electrode material where conditions
363
promoting the highly energetic reactions exist. In estimating their magnitude, one must make a certain number of assumptions, e.g. (i) energy per single event is that of the reaction D + D —> He, (ii) the number of single events to produce a crater is on the order of 104 or higher, depending upon its radius, 9 and (iii) the number of single events needed to generate the "hot spot" displayed by IR imaging is on the order of 104 or higher, depending upon its size and brightness. Under these conditions and assuming the loading ratio greater than unity, one can calculate the radius of this volume to be on the order of 100 A or higher. The events take place within the bulk material in the close vicinity to the contact surface. 2. Experimental/Results An operating P d D / D 2 0 , 0.3 M LiCl/Pt cell was placed in an electrostatic field generated by a parallel plate capacitor where the field strength was maintained and controlled by setting the potential difference at a specified level. The cell geometry is shown in Fig. 1. The Pd/D electrode was prepared by the Pd deposition onto an Au foil from a solution of 0.03 M PdCl 2 + 0.3 M LiCl dissolved in D 2 0 . The electrodeposition was under galvanostatic control with the current profile as follows: 1.0 mA c m - 2 for 8 h, 3 mA c m - 2 for 8 h, and at 5.0 mA c m - 2 until all P d 2 + ions were reduced. Upon completion of the Pd deposition, the cell current was increased to a value needed to maintain a visible gas evolution (usually 30-50 mA c m - 2 ) for the next 2-3h followed by placement in an external electric field (1000-3000 V c m - 1 ) with the cell current increased to about 100mAcm~ 2 for the next 48 h or longer. The surface morphology and the bulk structure of the codeposited Pd/D film, shown in Fig. 2a, undergoes substantial changes when the operating cell is placed in an external electrostatic field. This is illustrated in a series of SEM photographs taken from various runs. In the absence of an electric field, the electrode structure consists of globules, 3-7 /zm in diameter, arranged in short columns. Each of the individual globules is an aggregate of much smaller, almost spherical units, having a diameter in a submicron range. This structure is uniform throughout the electrode. 2.1. Morphological
Changes - Minor
Deformations
The first noticeable effect, seen shortly after placing the cell in an electric field, is swelling of the codeposited material followed by displacement toward the negative capacitor plate. The reorientation without substantial change in their size is shown in Fig. 2b. We selected examples of various structures to emphasize the complexity of the system as well as to indicate the impossibility of a quantitative analysis. The selected examples include minor deformation of the original structure, definitive shape change, unusual structures to a deformation associated with, what appears to be, a localized catastrophic event. Another example of the disintegration of the Pd/D structure is shown in Fig. 2c. This figure illustrates the breaking of the bonds holding together the individual globules. The breaking of the bonding and the separation of globules may be due
364
£3X£
(a)
5
Mi IB Mi
A^
(d)
(e) %&.
B
Figure 2. An illustration of minor morphological changes, (a) Reference morphology (no field), (b) reorientation, (c) disintegration, (d) branches (fractals), and (e) dendritic growth.
to action of the electric field alone or may be due to combined action of electrical and mechanical forces arising from the bulk material response to the changing magnitude of the surface forces. A different set of processes appears to be responsible for the structural changes, viz (i) formation of branches (fractals) (Fig. 2d) and (ii) the production of dendritic growth (Fig. 2e). In what follows, we argue that these two very different forms may have a common origin, namely that they are the result of a combined action of the current flow through a porous structure, the presence of evolving deuterium, and the electric field on the separated microglobules suspended in the electrolyte and restricted by the porous structure. The observed morphological and structural changes occur during the reduction of D + / D 2 0 ions/molecules at the porous electrode. Thus, at least three factors should be considered: (i) the external field, (ii) the distribution of the cell current, and (iii) the presence of gaseous deuterium within the confines of the structure. Since the depth of current penetration (for a given electrode kinetics, current density, etc.)
365
into electrode depends on pore size and assuming that all factors are involved, a different response to the field is expected at different sites of the Pd/D material. At sites of a relatively large pore size, the microglobules are acted upon by two factors, the electric field and the convective flow due to mixing by the evolving deuterium. The electric field redistributes the surface charges while the evolving gas brings microglobules in contact with each other. Viewing Fig. 2d we identify three areas having distinct features: area A with high density of branches and unattached microglobules, area B which is sparsely populated by microglobules and area C where the unattached microglobules are absent and where branches are well denned. The latter indicates that the growth of branches by addition of microglobules leading to an apparent reversal of the action of an electric field. Entirely different situations exist in small pore sizes; the pore wall may be covered by gaseous deuterium, thus shifting the cell current deeper into the porous structure. If a microglobule is placed into the current path, and if the potential drop over the length of the microglobule in the electrolyte is greater than the sum of cathodic and anodic overpotentials needed to dissolve Pd and deposit the P d 2 + ions, then the dendritic growth is possible. 11 2.2. Morphological
Changes - Shape
Changes
The transition from the "cauliflower-like" morphology to other forms is expected due to an interaction of the electric field and the response of a solid to the action of surface forces. While the morphologies shown in Fig. 2b-e can be accounted for, those in Fig. 3b-e suggest that additional factors are involved in producing the observed shape changes. Of the great variety of forms, we selected those illustrating the reshaping of the spherical globules into (i) rods (circular and square), (ii) long wire, (iii) folded thin film, and (iv) a crater, the latter suggesting the presence of a violent event. These structural changes require substantial energy expenditure, far in excess of that can be extracted from the electric field. One such source is of nuclear origin as first suggested by Fleischmann et al.12 and supported by the emission of soft X-rays, 13 charged particles, 14 and tritium 15 and helium 16 production. The SEM photographs, Fig. 3b-e, show well defined areas that seem to represent solidification of molten metal occurring under a liquid. If, as suggested earlier (vide supra) that the energy needed to melt a metal is of nuclear origin, then the chemical analysis of these distinctly different areas should reflect it. To illustrate, we selected three morphologically different cases, viz (i) a thin layer detached from the Au substrate (Fig. 4), (ii) boulder-like region (Fig. 5), and (iii) a place where, most likely, a catastrophic event has occurred (Fig. 6). Analysis of the detached thin film (Fig. 4), showed the presence of Ca, Al, Si, Mg, Zn, Au, O, and CI. Since the latter three elements are present in the cell components, they cannot be attributed to nuclear events (further experiments are needed for verification). The presence of these new elements on the electrode surface, after a long-term polarization, was claimed to be due to the concentration of impurities. 2 ' 3 While we cannot express an opinion as to the validity of such
366
SEE
.
£*
/_v
& J M H j > h i mini » § a « l »
Figure 3. An illustration of significant morphological changes, (a) Reference morphology (no field), (b) circular and square rods, (c) boulder and long wire, (d) folded thin layer, and (e) crater.
« *
&
JSL
3.0
6.0
9.0
Energy (keV)
Figure 4. SEM of P d / D electrode, after being placed in an external electrostatic field, showing a "blister-like" deformation. XRF spectra showing the chemical composition of the blister.
367
statement, we can show unambiguously that in our experiments this is not the case. The impurities, whether originating from solution or from cell components should be uniformly distributed over the electrode surface and not concentrated in clearly recognizable spots. In addition, to minimize the notion that they are the result of contamination, initiated in either solution or cell components, we selected two cases: the boulder-like (Fig. 5), and the crater-like segments of the electrode surface (Fig. 6). Analysis of the boulder-like segment showed the presence of a single element, Al, and that resembling a crater, the presence of two elements, namely Mg and Al. Without the aid of a Maxwell demon, it would be difficult to argue that such directed motion of impurities can take place. The only sensible answer is that they were produced in the course of electrolysis of D2O in a cell placed in an external electric field by nuclear events.
0
1
2
3
4
5
Energy (keV)
0
1
2
3
4
5
Energy (keV)
Figure 5. SEM of P d / D electrode, after being placed in an external electrostatic field, showing a "boulder-like" deformation. XRF spectra showing the chemical composition of the boulder and the area adjacent to the boulder.
2.3. More About Reaction
Sites
The progression of an experimental research, experiment —> interpretation of results —> conclusions —-> new experiment —>, etc., is illustrated in Fig. 7a-c. In a separate study, 10 we showed that the excess heat is not produced continuously over the entire electrode volume but at isolated, randomly distributed in time and space, reaction
368
sites. The short-lived "hot spots" (Fig. 7a), are, in fact, "mini-explosions" arising from fast and highly energetic reactions. Such "mini-explosions" can be displayed by bringing an excess heat-generating electrode in contact with an appropriate sensor.
0
1
2
3
Energy (keV)
4
5
0
1
2
3
4
Energy (keV)
Figure 6. SEM of P d / D electrode, after being placed in an external electrostatic field, showing a "crater-like" deformation. XRF spectra showing the chemical composition of the inside and outer rim of the crater.
Indeed, by codepositing the Pd/D film onto a piezoelectric substrate, one can display the pressure and temperature waves, originating within the bulk electrode, as they arrive at the sensor's surface (Fig. 7b). In accordance with the concept that one experiment leads to another we noted the following: An analysis of experimental results suggests that events occurring at the contact surface of the interphase region influence the events in the bulk, i.e., influence the intensity and type of the nuclear events through the interactions between the D+ complexes and the Pd lattice assisted by the stress fields at the reaction sites. Consequently, by placing an operating cell in an external electric field one would expect to see effects quite different from those observed in the absence of field. This is illustrated in Fig. 7c. 3. Discussion The variety of forms/structures resulting from the exposure to an electric field can be divided in two groups viz those that arise from the co-operative and/or competitive
369
Figure 7. Sites and energetics of events, (a) Discrete hot spots, (b) mini-explosion(s), and (c) chemical composition indicating nuclear origin.
interaction between cell components, relevant processes and their driving forces and those that require substantial energy expenditure. 3.1. Search for
Precursors
In a previous communication 17 we examined the behavior of the Pd/D-D2 0 system using cyclic voltammetry. An analysis of voltammograms indicated the presence of what we have interpreted as Dj" species in analogy to the existing H j molecule-ion. The Hj molecule-ion was first considered in electrochemical systems by Horiuti 18 and was modeled by Gryzinski. 19 Basically, it involves injection of an s-electron into an orbit in a manner so that [(H + -e~) - H + ] molecule-ion is formed. Here, the s-electron effectively shields one of the H + ions. The s-electron injection can be written as follows: H+ + H + + e ~ —> [(H + • e~) — H + ] indicating that (1) the reaction is of the electron-ion recombination type and that (2) shielding of one of the originally close H+ ions removes the Coulomb barrier and creates chemical bond. 3.1.1. Formation of [(D+ • e~) n — D+] molecule-ion Using the same arguments, we have D+ + D+ + e~ -> [(D+ • e") - D+], and, by addition of another D + ion [(D+ • e~) - D+] + D+ + e" -> [(D+ • e") 2 - D+], or, in general [(D+ • e") n - D+] + D+ + e" -> [(D+ • e - ) n + 1 - D+]. Similarly, an addition of two complex molecule-ions can occur yielding [(D+ • e~) m - D+] + [(D+ • e") n - D+] + e~ - [(D+ • e - ) m + n - D+].
370
These complexes interact with the Pd lattice - this is symbolically indicated as Pd . . . [(D+ • e~) n — D + ] . Each of these reactions occurs with the rate constant that is affected by an electric field. 3.2. Complex
distribution
The multiple reaction paths result in a distribution of complexes of varying number of (D + • e~) units. Two factors would have to be considered when assessing the distribution pattern: the reaction rate constants and the stability (mechanical) of the complex [(D+ • e~) n - D+]. (a) Reaction rate. The reaction path can be viewed as an electron-ion recombination occurring in an external electric field. The effect of an electric field on the rate constant of such reactions was examined by Wojcik and Tachiya. 20 Evidently, the rate constant is affected by an external field in a way that depends on the conditions outside the molecule-ion boundary. In particular, the action of an external field may either accelerate or slow down the electron-ion recombination reaction. (b) Mechanical stability. The mechanical stability of the [(D + • e~) n — D + ] as well as the stability of a domain (of complexes) P d . . . [(D + • e~) n — D + ] N can be examined using the liquid drop analogy, i.e., via the energy considerations and, in particular, by the change in the potential energy associated with the deformation of the spherical drop. The energy of the complex molecule-ion (represented as a liquid drop) consists of two parts: (i) binding energy (energy needed to take the complex apart) and (ii) surface (capillary) energy while that of a domain includes also the electrostatic energy. To evaluate, one can employ the liquid drop model and carry out calculations in a manner similar to that used in assessing the stability of a nucleus. (c) Distribution. Two distributions are considered (i) that of a [(D + •e~) n —D+] complex and (ii) that of a P d . . . [(D + • e~) n — D + ] N domain. In both cases, the stability conditions are derived from energy considerations associated with the shape change resulting from the motion of components (charged or not) that occur within the molecule-ion or the domain. In both cases, capillary energy plays an important role. The shape changes arise from fluctuations, which, in turn, modify the magnitudes of the potential and kinetic energies of the molecule-ion, respectively, the P d . . . [(D + • e~) n — D + ] N domain. The interaction with an environment (the Pd lattice and/or s-electrons) occurs in a coherent way. 3.3. Fusion
Reactions
3.3.1. Fusion of Light Elements, T and He The production of light elements (T and He) occurs via the following set of events: (i) An s-electron is captured by the molecule-ion [(D + • e~) — D + ] , so that the precursor [(D+ • e") - D*] is formed ([(D+ • e") - D+] + e" - • [(D+ • e _ ) - D*]). The electron capture (K-capture) is favored at the "heavy end" of the periodic table where the K-orbits are small and the probability of an electron to be at nucleus is
371
large. In our case, the high probability is assured by high concentration of energetic s-electrons within the domains. The rate of transmutation of the molecule-ion to a precursor increases with an increase in the chemical potential of s-electrons. This can be demonstrated as follows: for the reaction Z M A + e~ —> z _ i X A + v at equilibrium, the chemical potentials must be equal. The chemical potential of a single molecule (here, the precursor) is just its internal energy, -e. Consequently, —£M + M e ~) = —£x- Now, since the neutrino leaves the system, its chemical potential does not appear and furthermore, an increase in the s-electron concentration or their energies, tends to increase the ej" capture. Following the s-electron capture the electrostatic energy of the complex molecule-ion is reduced causing its collapse to the precursor, (ii) The electron capture effectively changes the nature of the force acting between the shielded deuterons, i.e., change from chemical bonding to nuclear forces, to form [(D+ - e ~ ) . . . D*] or i(X) 4 , a highly excited nucleus, (iii) The excited nucleus can decay via the /3 emission to He :i (X) — e~ —* 2He and via the proton emission followed by f3 emission to T :i(X) — p + —>• o(X) 3 — e~ —> 1X3 = T (emission of charged particles was observed).
3.3.2. Fusion of Heavier Elements, Qualitative Observations Fusion of heavier elements, e.g., Al, Mg, Si, Ca, Zn, etc., occurs (in our system) when an operating cell is placed in an external electric field. Qualitatively, the newly fused elements are found to be randomly distributed over the electrode surface area indicating highly localized reaction sites. The analysis of the reaction sites show either a single element, e.g., Al, or more than one element, e.g., Al and Mg. There appears to be some correlation between the structure of the reaction site, as displayed by SEM, and the number of fused elements present. A common feature exhibited in both cases (presence or absence of field) is the presence of highly localized reaction sites (note the hot spots displayed by IR imaging in the absence of field).
3.3.3. Proposed Fusion Mechanism for Heavier Elements In formulating the fusion mechanism, we note the following: (a) Fusion must be a single event in the sense that it follows the reaction scheme: precursor + trigger —> unstable "nucleus" —• stable nucleus. One triggering mechanism might be due to e~-capture assisted by local conditions, e.g., stress field, electric field, etc. (1) Fusion must involve events within the precursor as well as to provide the balancing charge of electrons in the K, L, M, and N orbits. (2) Fusion to heavier elements (in our system) requires the presence of an external electrostatic field. The fields used in our experiments were on the order of 10 3 Vcm _ 1 , i.e., too small to affect chemical bonding within the precursor. Consequently, there are a number of questions that need to be
372
answered, viz how the field interacts with the system as a whole to produce precursors containing a large number of (D+ • e~) n elements within the [(D + -e~) n —D+] complex. Is the fusion reaction leading to multiple elements due to a single large precursor, which disintegrates when in an excited state to yield multiple elements, or is a number of precursors present within the domain? 4. Concluding Remarks (1) The most obvious effect of an external electric field is the shape change of the individual globules of the "cauliflower" structure of the codeposited material. With the shape change there is a change in the defects density as well as in the stress field intensity. Both these factors affect the interaction between the D + -complexes and the Pd lattice, i.e., they contribute to the formation of the Pd . . . [(D + • e~) n — D + ] N domains. (2) The concentration of the D + -complexes is determined by the overpotential. The effect of an external electric field is minimal. (3) Excess enthalpy is generated by highly energetic fast reactions that resemble "mini-explosions." This view is supported by IR imaging (hot spots), by the response of the pressure/temperature sensitive substrates (piezoelectric material) onto which the Pd/D films are codeposited and by SEM examination and analysis of selected isolated spots showing elements not originally present. (4) The formation of precursors as well as the fusion reactions is of the type: A + B—>C + D. As written, this statement implies conservation of matter - otherwise, both the reactants and products are not constrained. In practice, however, the initial conditions of the reactants are specified by the experimental protocol while those of products by energy considerations and the rate constants. If such reaction occurs in, e.g., the Pd lattice, additional constraints are operative. Consequently, in the reaction: A + e~ —> z - i X A + v, the particles are constrained by an interaction ZM with the Pd lattice. This, we indicate by writing Pd .. .z M A , etc. It is with this in mind that we examine the effects of placing an operating cell in an external electrostatic field. (5) The triggering activities (to initiate fusion reactions) are located within the first few atomic layers and, most likely, involve changes in the electronic structure of this region. These changes are transferred deeper into the Pd lattice where the nuclear events occur. References 1. S. Pons and M. Fleischmann, Calorimetry of the palladium - deuterium system, in Proceedings of the ICCF-1, 1990, p. 1. 2. D. R. Rolison and P. P. Trzaskoma, J. Electroanal. Chem. 287, 375 (1990).
373
3. D. R. Rolison, W. E. O'Grady, R. F. Doyle, and P. P. Trzaskoma, Anomalies in the surface analysis of deuteratedpalladium, in Proceedings of the ICCF-1, 1990, p. 272. 4. P. van Rysselberghe, Some aspects of the thermodynamic structure of electrochemistry, in J. O'M. Bockris (ed.), Modern Aspects of Electrochemistry, Vol. 4 (Plenum Press, New York, 1966). 5. S. Szpak, P. A. Mosier-Boss, J. Dea, and F. E. Gordon, PolarizedD + /Pd-D20 system: hot spots and mini-explosion, in Proceedings of the ICCF, Vol. 10, 2003, p. 113. 6. P. Glansdorff and I. Prigogine, Thermodynamic Theory of Structure, Stability and Fluctuations (Wiley-Interscience). 7. J. O'M. Bockris and A. K. N. Reddy, Modern Electrochemistry (Plenum Press, New York, 1974). 8. S. Szpak and P. A. Mosier-Boss, Nuovo Cimento, submitted. 9. George Russ, http://d2fusion.com/volcanoes.html. 10. P. A. Mosier-Boss and S. Szpak, Nouvo Cimento, 112A, 577 (1999). 11. S. Szpak, T. Katan, and P. J. Carlen, J. Electrochem. Soc. 133, 1340 (1986). 12. M. Fleischmann, S. Pons, and M. Hawkins, J. Electroanal. Chem. 201, 301 (1989). 13. S. Szpak, P. A. Mosier-Boss, and J. J. Smith, Phys. Lett. A 210, 382 (1996). 14. A. G. Lipson, A. S. Roussetski, G. M. Miley, and E. I. Saunin, Phenomenon of an energetic charged particle emission from hydrogen/deuterium loaded metals, in Proceedings of the ICCF, Vol. 10, 2003. 15. S. Szpak, P. A. Mosier-Boss, R. D. Boss, and J. J. Smith, Fusion Technol 33, 38 (1998). 16. B. F. Bush, J. J. Lagowski, M. H. Miles, and G. S. Ostrom, J. Electroanal. Chem. 304, 271 (1991). 17. S. Szpak, P. A. Mosier-Boss, and R. S. Scharber, J. Electroanal. Chem. 337, 147 (1992). 18. J. Horiuti, The mechanism of the hydrogen electrode reaction in Transactions of the symposium on electrode processes, in E. Yeager (ed.) (J. Wiley & Sons, New York, 1961). 19. M. Gryzinski, Phys. Lett. A 123, 170 (1987). 20. M. Wojcik and M. Tachiya, J. Chem. Phys. 109, 3999 (1998).
CALORIMETRIC A N D N E U T R O N DIAGNOSTICS OF LIQUIDS D U R I N G LASER I R R A D I A T I O N
Yu. N. B A Z H U T O V Institute
of Terrestrial
Magnetism, Ionosphere and Radiowave 142092, Troitsk, Moscow region, Russia E-mail: [email protected]
Propagation
(RAS)
S. Y u . B A Z H U T O V A A N D V. V. N E K R A S O V Moscow State Academy
of Device
Constructing
& Informatics
(MGAPI),
Moscow,
Russia
A. P. D Y A D ' K I N A N D V. F . S H A R K O V Troitsk Institute
for Innovation
& Thermonuclear
Researches
A series of experiments were performed with laser irradiation on different liquids in special work cells. A red semiconductor laser (A = 655 ± 25 nm) was used, with power output in the milliwatt range. In each test, before, during and after laser irradiation, calorimetric and neutron diagnostics were performed. The calorimetry was done with a thermistor (sensitivity ~0.05°) was used. For neutron diagnostic gas neutron counters (BF3 and He 3 ) were used. All experimental results are discussed.
1. Introduction In the last conference (ICCF-10, Boston) there were some reports 1,2 of excess heat observation in electrolytes during electrolysis after laser irradiation. These results can be understood in framework of Erzion model.3~5 According to this model, Enions (stable neutral baryons consisted from nucleon and Erzion) are captured by only a few of nuclei (donors), and may be kept in this state for a rather long time. After they are released, them they begin run the Erzion-nuclear catalytic chains with large frequency (in the GHz range). The energy of this bounded state depends on the donor nucleus, and the smallest bounded energy is about 1.5 eV for a proton nucleus. If we irradiate such a compound nucleus with photons with such equal or higher energy we can provide the process of Enionization, very similar to photo effect. Red laser (A = 650 nm) can provide us such irradiation. During such catalytic Erzion-nucleus chain reaction, Enions again may be captured by donor nucleus (H 1 or O 16 ), and the chain will be broken. The most dramatic fact in the framework of Erzion model is that bounded energy for O 16 donor is about 10 eV (region of vacuum ultraviolet light). This fact prevents running of CF process in water or some other materials. But for a short time we can observe this process. The Erzion model may be alone among models that attempt to explain CF in that 374
375
it predicts what kind of concrete nuclear reactions can run, and with what release energy. We cannot predict their cross sections precisely, but we do know their priorities. 6 This is why we decided to perform the experiment with laser irradiation of water solutions while recording neutron radiation and excess heat. To understand what chemical elements we must use in our experimental cell as a supplement to water solution let us look though all Erzion-nuclear reactions for light chemical elements: H 1 ( 9 - , 3 ° ) n + 1 . 6 5 M e V (100%),
(1)
H 2 ( 9 " , 9 N )n +5.6MeV (0.016%),
(2)
H 2 ( 9 N , 3 ° ) H 3 + 0 . 1 MeV (0.016%),
(3)
H 2 (9°, 9 N )H 1 + 3.9 MeV (0.016%),
(4)
Li 6 (9 N ,3°)Li 7 + l.lMeV(7.5%),
(5)
Li 6 (3°,9 N )Li 5 + 0.48MeV (7.5%),
Li5 -> He 4 + H 1 + 1.7MeV,
(6)
L i 6 ( 9 - , 9 N ) H e 5 + 3.2MeV(7.5%),
He 5 -> He 4 + n + 1.36MeV,
(7)
Be 8 -» 2 x He 4 + 4.8MeV,
(8)
L i 7 ( 9 N , 9 - ) B e 8 + 9.5MeV (92.5%)
C 1 3 (9 N ,3°)C 1 4 + 2.0MeV(l.l%),
(9)
C 1 3 (9°,9 N )C 1 2 + 1.2MeV(l.l%),
(10)
C 1 4 ( 9 N , 9 - ) N 1 5 + 2.4MeV(—),
(11)
N 1 4 ( 9 - , 9 ° ) C 1 4 +2.3MeV (99.6%),
(12)
N 1 4 ( 9 ~ , 3 N ) C 1 3 + 0.25MeV (99.6%),
(13)
N 1 4 (9 N , 9°)N 15 + 4.7MeV (99.6%),
(14)
N 1 5 ( 9 N , 9 " ) 0 1 6 + 4.3MeV (0.37%),
(15)
0 1 7 ( 9 N , 3°)018 + 1.9MeV (0.038%),
(16)
0 1 7 ( 9 ° , 3 N ) 0 1 6 + 2.0MeV (0.038%),
(17)
0 1 8 ( 9 N , 3 " ) F 1 9 + 0.2MeV (0.2%).
(18) 1
From these reactions we can see that neutrons can be created only on the H and Li 6 nuclei in reactions (l)-(3), and only due to creation of negative Erzions (9~) in reactions (8), (11), and (18). The best nucleus for such creation is Li 7 (converter nucleus), because it is the most concentrated in the natural element (92.5%). Such way for our work solution we decided to use alkaline solution of lithium (LiOH) with addition of heavy water (D 2 0) for Erzion-nuclear chains prolongation.
376
2. Experimental Installations In the first experimental series the large (015 x 200 cm 2 ) BF3 neutron counter was used. The work cell was placed near one of the end faces of this counter (Fig. 1). The efficiency of this neutron counter for this cell, measured with a Cf252 neutron source, was —r; = (2±0.5)%. The main part of the cell is narrow glass (01.5 x 15cm 2 ) with alkaline water solution (15ml, 2.2M LiOH, 20% D 2 0 , C = 6 J / g K ) , which was placed inside of plastic thermostatic glass with small laser indicator (W ~ 1 mW, A = 650 nm) on the upper portion. The thermistor was placed on the surface of the narrow glass. The sensitivity of this thermistor was 0.05 K.
Laser ( I V - 1 mW) Thermometer
Polysterene
I
Ph \
BF3
I Pb Polysterene
r
I [ I
Figure 1. View of installation 1.
In the second experimental series, a better He 3 neutron detector was used. It consisted of a paraffin cylinder (022 x 40 cm 2 ) with one center cylindrical hole (08 x 30 cm 2 ) for the cell, and two narrow cylindrical holes (03.5 x 35 cm 2 ) on both sides for He 3 parallel counters (Fig. 2). The efficiency of this neutron detector for the same work cell, measured with a Cf252 neutron source, was — rj = (9 ± 0.5)%. The cell was very similar the first cell, but a more powerful laser (W ~ 5mW, A = 650nm) was used, and the narrow glass was larger (03 x 20cm ). A new water solution (132ml, 3.5M LiOH, 15% D2O) was used. The thermistor was not used in this series. 3. Experimental Results Over a 6-month period, from March to September 2004, we performed 20 experimental runs using installations 1 and 2 (~10 runs for each). Calorimetric diagnostic was used only with installation 1. We did not observe clear positive results. We can only estimate the upper limit for energy production
377 Laser(l
He 3 neutron counters
n
cr>
Figure 2.
View of installation 2.
systems. For the first cell, (15 ml, 2.2 M LiOH, 20% D 2 0) we determined the calibration constant was equal to C = 6 J/g K. Since the sensitivity of the thermistor was 0.05 K we can estimate the upper limit for energy production was equal to Wmax = 0.5 mW, what is comparable with the laser power (W ~ l m W , A = 650 nm). Therefore, we did not detect excess heat. So in the second series we did not perform calorimetry.
Mean neutron account in "Laser-2" experiment (13-08-04) (BF3-counter; W< 1 mW; 2.2 M LiOH (20% D20) 15 ml_ solution) (1) Background - = (595.5 ± 5.9) epm, SN = (28.5 ± 6.9) epm (4.1 a)
600
m
590 580 570
JLAJJ
j.y
yj
560 550 540 530 ' 520 j 510 j 500 ' 21
26
31
36
Time (1 min intervals)
Figure 3.
Mean neutron account for best experiment from first series.
378
Mean neutron account in "B Laser-1" experiment (1) Background • = (394.1 ± 2.8) epm, A(N2) = (22.4 ± 3.6) epm - (6.2 a), (2) Laser off - (N3(11-12)> = (384.2 + 4.4) epm, A(N3> = (12.5 ± 5.0) epm - (2.5 a).
emp)
410 400
Acco unt (event perm
390 380 370
T i
'
I T
T
360
350 34 0
Time (10 min intervals)
Figure 4.
Mean neutron account for best experiment from second series.
But we did measure positive neutron results. In some runs we have observed positive results during variation of concentration of Li and D2O in water solutions, using b o t h kinds of installation. T h e best results are presented in Figs. 3 and 4. As you can see b o t h cases were statistically significant (4.1 and 6.2 are more then 3 standard deviations). But the reproducibility of these results was not good. This can be explained in framework of Erzion model (see Section 1). Now, we are working to develop this explanation.
References 1. D. Letts and D. Cravens, Laser stimulation of deuterated palladium, in Proceedings of the ICCF-10, 2003. 2. M.R. Swartz, Photoinduced excess heat from laser-irradiated electrically-polarized palladium cathodes in heavy water, in Proceedings of the ICCF-10, 2003. 3. Yu.N. Bazhutov and G.M. Vereshkov, New Stable Hadrons in Cosmic Rays, their Theoretical Interpretation & Possible Role in Catalysis of Cold Nuclear Fusion, Preprint No. 1, Central Research Institute of Machine Building, 1990. 4. Yu.N. Bazhutov, G.M. Vereshkov, and V.L Kuksa, On a possibility of existing new stable hadrons-hypothetical catalyst of cold nuclear transmutation, in Proceeding of 3-d Russian Conference On Cold Fusion & Nuclear Transmutation, Vol. 157 (Moscow, 1996). 5. Yu.N. Bazhutov and G.M. Vereshkov, in Proceedings of ICCF-4, Vol. 4 (Hawaii, 1993), pp. 8-1. 6. Yu.N. Bazhutov, Influence of spin and parity preservation lows on Erzion model predictions in cold fusion experiments, in Proceedings of the The Seventh International Conference on Cold Fusion (Vancouver, Canada: ENECO Inc., Salt Lake City, UT, 1998).
A N O M A L O U S N E U T R O N C A P T U R E A N D PLASTIC D E F O R M A T I O N OF Cu A N D Pd CATHODES D U R I N G ELECTROLYSIS IN A W E A K THERMALIZED N E U T R O N FIELD: E V I D E N C E OF NUCLEI-LATTICE E X C H A N G E
A. G. L I P S O N A N D G. H. M I L E Y Department
of Nuclear, Plasma and Radiological Engineering, University S Goodwin Avenue, Urbana, IL 61801-2384, USA
of Illinois,
103
A. G. L I P S O N Institute
of Physical
Chemistry,
Russian Academy of Sciences, Moscow 117915, Russia
31 Leninsky
prospect,
Anomalous neutron capture and plastic deformation in the hardened Cu and Pd cathodes has been established under combined action of electrolysis and a weak thermalized neutron field (WTNF) with a flux in the range of 180-400 n / s cm 2 . Experiments with these cathodes showed ~7.0% decrease in the 2224 keV n-D gamma peak accompanying thermalized neutron capture inside the P E cavity during electrolysis vs. experiments with annealed Cu and Pd as well as with the background runs (i.e., no electrolysis). The anomalous neutron capture and plastic deformation of Cu and Pd cathodes under combined action of electrolysis and W T N F may be explained energetically by assuming a selective radiationless thermalized neutron capture at high-internal strain concentration sites in the hardened cathodes. The results of these experiments provide straightforward (avoids the Coulomb barrier penetration issue) evidence that nuclei—lattice energy exchange can result in an increase in neutron capture probability and radiationless de-excitation of the resulting compound nuclei.
1. Introduction Earlier it was shown that DD-reaction rate at low-deuteron energies are strongly affected by crystalline lattice of metals with high-hydrogen solubility, including Pd. 1 However, the study of low-energy deuteron interaction with Pd-metal is limited by the presence of nuclear Coulomb barrier, resulting in dramatic decrease in the DD-reaction yield at lower projectile energy.2 Meanwhile, if the phenomenon nuclear-lattice exchange (or, in fact, LENR) in metal deuetrides/hydrides had really existed then the effects of nuclear interaction (doesn't matter what kind of nuclear particle interact with solid) in crystalline lattice of such deuterides would be sharply distinctive of that in vacuum/plasma environment. The effects of nuclear interaction with crystalline lattice of deuterides could be displayed as kind of cross-sections variation, compared to vacuum environment. In that sense, in order to confirm the reality of LENR in metal deuterides, we considered feasibility of 379
380
neutral nuclear particles (neutrons) irradiation of metal deuterides, allowing to rule out the Coulomb barrier effect on the yields of nuclear reaction. As we showed in our previous works, the thermalized neutron capture cross-section in metals during electrolysis can be enhanced drastically due to specific of low-energy neutron interaction with non-equilibrium lattice. 3 ^ 5 The phenomenon of increase in thermal neutron cross-sections is accompanied by synergetic effect of a strong plastic deformation of irradiated non-equilibrium solids which cannot be explained without concept of "radiationless" decay of compound nuclei resulted in that neutron capture. In present paper, we studied the process of thermalized neutron absorption in Pd and Cu cathodes during their loading by deuterium and hydrogen, respectively. We found anomalous enhancement of weak thermalized neutron field (WTNF) capture (suggesting about 7.5 times increase in cross-section) and of plastic deformation in both cathodes during electrolysis. This anomalous processes in Cu and Pd cathodes under combined action of electrolysis and WTNF could be explained energetically suggesting a selective radiationless thermalized neutron capture beneath the surface at the high-internal strain concentration sites. The results present a simplest (avoid Coulomb barrier penetration issue) evidence for nuclei-lattice exchange,6 resulting an increase in neutron capture probability and radiationless de-excitation of the compound nuclei formed in the lattice. 2. Experimental In the present work, we are strictly concerned with WTNF, defined by a highly rarefied neutron gas (a low-neutron density n < 10~ 3 cm ~ 3 or a low flux <]>n < 4 x 10 2 n/s/cm 2 ) with under-Maxwellian velocities (with mean energy (En) ~ 1 — — lOkT) and isotropic angular distribution. In order to create the neutrons field with flux
381
count rate over the 2225-keV peak, An is the neutron mean free path length inside the cavity, K = 1.5 x 10 4 cm 3 is a cavity volume; aK, /i H and n H are the effective cross section of n(p,d)7 reaction for neutrons with En = 80meV, moderator thickness and hydrogen concentration in the moderator, respectively.
I
;
!
|
Figure 1.
The cold-worked Pd-foils (purity 99.99%) of 100 yum thick were used as the cathodes. The samples of 5.0 x 2.0 cm 2 area were cut from a single foil sheet and then served as a cathode during electrolysis in 1 N N a O D / D 2 0 solution (in the cell with separated cathode and anodic spaces5 at electrolysis current density j = 30 mA/cm 2 during 1-3 days at room temperature. After electrolysis deuterium loading ratio in Pd samples was determined by thermal-desorption technique and constituted within the range of x = D / P d ~ 0.80. Dislocation density in the initial (cold-worked, not annealed) Pd-foils was N& = 10 7 cm~ 2 . After finishing of electrolysis, the macroscopic longitudinal bending (I) (induced by the difference in molar volume of PdDx phase across the electrode, developed during D-diffusion5) and the residual plastic deformation of the sample (e p ) were measured. It was established that after the electrolytic deuterium loading at natural neutron background condition those mechanical characteristics reach, in average, (I) = 1.5 cm and (ep) = 3 x 10~ 3 and dislocation density N^ = 1.5 x 1 0 n c m ~ 2 . Under combined electrolysis and UTNF due to a stronger deformation at the same electrolysis current these parameters became much larger, so that (ln) = 5.0 cm and (ep}n = 3.3 x 1 0 - 2 and A"d = 3.8 x 1 0 n c m - 2 . Two types of cold-worked Cu foils (0.3 mm thick, area 5" = 5.0 x 2.0 cm 2 were used as cathodes in the electrolytic cell. The first type of cathode (designated Cu-1)
382
was cut from cold-worked hardened copper foil, containing 0.14% Si (Cu:Si) with an edge dislocation density of N^ ~ 108 c m - 2 (estimated from a coherent X-ray scattering measurement). A similar shaped cathode of the second type (termed Cu-2) was produced from a nominally pure (99.99% purity) copper foil annealed in vacuum resulting in a minimum edge dislocation density of N^ < 5 x 104 c m - 2 . A I M solution of KOH/H2O was used as the electrolyte (V = 250ml). The electrolysis was carried out at room temperature with a DC current density j = 20-30 mA/cm 2 and a voltage range 5.0-6.0 V. The electrolyte temperature rise during electrolysis was limited to about 5.0°C as recorded from thermocouple reading. At this temperature the evaporation rate in the electrolytic cell was <4ml/h. Typically, the evaporation volume of electrolyte for a 3h. electrolysis run was <5%. Since the set up was not hermetic, the gases formed by electrolysis were continuously removed. Thus, with this low-evaporation rate, combined with the continuous removal, gas dissolved in electrolyte at any given moment was too low to significantly effect neutron flux inside the cell. 3. Experimental Results In the case of the strained Pd samples electrolysis (a) a statistic decrease of 2225 keV gamma line intensity in foreground runs (with electrolysis) compared to the background runs (j = 0) has been established (Fig. 2). From 20 similar strained samples used in a row, the negative difference between foreground and background was obtained in 18 cases, including 11 samples completely out of three sigma corridor, while positive difference with low-significant level has been shown only in two samples. In the case of net ROI, difference between foreground and background (after subtracting of continuum produced by inelastic scattering of fast neutrons from Cf252-source) the mean value AN is strongly negative: (AiVnet) = -(5.95 ± 0.75) x 10- 3 cps. For annealed Pd samples (b) the situation with thermal neutron capture during electrolysis is completely different. The effect of thermal neutron capture for samples (b) was not observed, despite of the same broadening of 2225 keV line that is in (a) case. The number of positive and negative differences between foreground and background is approximately the same for this case. Moreover, all these values are inside of three Sigma corridor. The mean value of difference between foreground and background count for annealed samples was: (iVnet) = +(0.90 ± 1.15) x 1 0 - 3 cps, that are demonstrated a total absence of any significant difference between foreground and background count rate. It should be noted that statistically significant change in 7-line intensity is observed only for 2225 keV line in the case (a). For other intensive lines (for instance, 40 K, E1 = 1458keV) no any change in ROI upon the foreground runs has been detected, neither in (a) nor in (b) cases. Thus, during the electrolysis (deuterium loading) of the strained Pd samples the effect of enhancement of thermal neutron absorption is appeared due to capture of thermal neutrons by Pd cathode. In the case under consideration of about 5.5% of
383
Anomalous neutron absorption y-2225 keV (net) ROI 20 runs in succession Distribution of A N net vs. run number A ( A N n e t i o n e t ) . 1 0 " cps +8 +6 +4f O. T +2 51617181920 8 < 10HT12U141 1 2I 4 5 6 0 \r—o ~xr -2 -4 <> $ J---J-o
j _
(M-
( )
<)
+3c -*• Run,
-3o
oj
O
Figure 2.
thermal neutrons from total flux inside the cavity containing detector and cell with Pd cathode were captured by sample during electrolysis. The data obtained allow to estimate the average effective coefficient of thermal neutron absorption increase (Ka) in the strained Pd samples as follows: Ka~ ( /crpd= ( l / n s x L s x cr P d ln[l/(l - n c )],
(2)
where n s , Ls are the concentration of Pd atoms and sample thickness (Ls = 0.01 cm), while under In sign there is a ratio between the fractions of falling thermal neutrons and transmitted through the sample (with subtracting of absorbed part nc of total falling flux). In the case of strained Pd samples (a) we obtain the increase in thermal neutron absorption probability K& = 7.5 taking into consideration an average thermal neutron cross section for Pd isotope mixture cpd » 10.0 b. Therefore, the probability of thermal neutron capture in a strained Pd under combined electrolysis and UTNF is 7.5 times larger compared to that for normal (unloaded) state as well as for Pd samples with no internal strain. The effect of WTNF absorption was studied more carefully in experiments with Cu-cathodes in light water electrolyte. In order to correctly identify the gamma intensity in the energy intervals corresponding to neutron capture in hydrogen and in the Cu cathode (7-decay of Cu 64 and Cu 66 isotope generation), a channel-bychannel computer analysis of the gamma spectra observed during electrolysis [with the background spectra (for j = 0) subtracted) is presented in Table 1. In the case of Cu-1 samples statistically significant differences occur only in two energy
384
intervals: (1) 1029-1049 keV (ch 815-827) and (2) 2219-2229 keV (ch 1755-1761). In the case of Cu-2 samples (pure annealed Cu) no statistically significant differences are detected, either in these two intervals or in the rest of 0.1-7.0 MeV energy range. The latter result indicates that no significant anomalous neutron capture (compared to background) occurred during electrolysis of the pure annealed copper samples. In every run both integral and net count rates were determined for the energy intervals of interest. The Bremsstrahlung correction to obtain the "net" peak area was derived automatically using the Maestro-II software by subtracting the continuous part of gamma spectrum corresponding to the base- line of the integral peak area. Table 1. Gamma-count rate for combined UTNF and electrolysis of the copper cathodes Cu-1 and Cu-2 (foreground runs) after subtracting background count rate (electrolysis off, i.e., j = 0): Energy range (keV)
Sample
( A i V t ) x l O - 3 (cps)
(AJV n e t }xlO- 3 (cps)
1039.4 1039.4 2224.5 2224.5
Cu-1 Cu-2 Cu-1 Cu-2
+(1.32 -(0.16 -(1.42 ±(0.07
±(1.08 ±(0.12 -(1.44 ±(0.10
±10.0 ±10.0 ± 5.0 ±5.0
±0.30) ±0.50) ±0.35) ±0.81)
±0.34) ±0.62) ±0.38) ±0.85)
Resulting intensity 0.34 ±0.09*
11.8±2.8**
-
Here: (ANt) is a mean value of the integral count rate in the foreground runs after subtracting the background run rate (foreground run time t < 5000 s); (A7Vnet) is a net count rate (after subtracting gamma Bremsstrahlung in the same runs as for (A7Vt));* - (Q), (at. Cu 6 6 /s x cm 2 ) is a mean rate corrected for Cu 66 isotope decay (1039.4 keV line) and branching ratio (9.5%), taking into account the detection efficiency £i;** - A3>n, (n/s x cm 2 ) is a mean rate of neutron capture by the samples, calculated from the change in intensity of 2225 keV line with efficiency £2-
Electrolysis experiments with Cu-1 cathodes exhibited an activity (count rate) in the energy range corresponding to interval (1) (ch. 815-827) that depended on electrolysis duration. A count rate significantly above the background was detected only if electrolysis time was <5000s. In contrast, the count rate over the interval (2) during electrolysis runs was found to be independent on electrolysis duration showing significant decrease compared to background. The similar experiments performed with Cu-1 cathodes that had been previously used in electrolysis runs also showed no excessive count rate in the interval (1) compared to the background. In this connection, to obtain statistically significant data on gamma-activity in the vicinity of 1039 keV we used the 22 cathode-samples in a row prepared from the same batch of Cu-1 using an electrolysis duration of 2000< t <5000s each. For comparison the other 12 Cu-1 cathodes (from the same batch) were used separately to carry out long-time electrolysis runs with duration t> 12,000 s.
385
The experiments also show anomalously high-plastic deformation of the Cu-1 cathodes under combined electrolysis and WTNF. Measurement of a residual plastic deformation (e p ) of cathode samples and their bending (I) due to electrolysis (associated with a non-uniform hydrogen loading of the sample's faces in the cell with the separate cathode and anode spaces2) showed that combined electrolysis and WTNF resulted in average values of e p n = 10~ 3 and ln = 1.5 mm in the hardened Cu:Si (Cu-l)samples. For the same Cu samples, when electrolysis was done in absence of WTNF e p = 1(T 4 and I <0.2 mm were found (i.e., an order of magnitude smaller than with WTNF). The deformation and bending for Cu-2 samples was so small, that these parameters could not be measured, either with or without WTNF irradiation. Statistical analysis of the gamma energy interval (1) from Cu-1 samples shows that the maximum emission intensity (after subtracting the background) is in good agreement with a mean gamma energy of E7 = 1039.0 ± 1.0 keV. This energy closely corresponds to 7-line emission from Cu 66 (half life Ti/ 2 = 5.1 min), which is generated by thermal neutron capture in Cu 65 . This suggests that anomalous thermal neutron capture in the Cu 65 of the copper cathode causes the decreased neutron flux observed when electrolysis is turned on. To verify this assumption, a gammameasurement was done in the range of 1029-1049 keV (channels 812-830) for two different run times (t): (a) t < 5000 s and (b) t > 12,000 s. These data were summed three channels at a time, and the total standard deviation corresponding to each sum is shown in the count rate diagrams (Fig. 3a,b). As seen for t < 5000 s (Fig. 3a) the mean differences (AN) = (N{) - (Nh) (where Nf and N\, are the count rates in foreground and background, respectively) having a significance level (exceeding three standard deviations) are only located in the narrow ch. 819-824 interval. This result is in good agreement with the 1039.4 keV Cu 66 line position. In contrast, the similar, but long-foreground runs (12,000 < t < 24,000 s), presented in Fig. 3b do not exhibit any statistically significant (AN) values in the vicinity of 1039.4 keV line. A possible reason for this electrolysis duration effect on the 1039.4 keV band count rate will be discussed following the proposed model of anomalous WTNF capture in Cu-1 samples. Here we only note that this effect might be attributed to a transient equilibrium between parent and progeny Cu-nuclei at the surface of Cu-1 cathode. Equilibrium is probably affected by the atomic state of the surface in terms of impurity and vacancy motion, which could displace Cu 65 atoms located in the high-internal strain sites near the surface, reducing neutron capture in these sites. Taking into account both the gamma-detection efficiency with respect to the cathode (ei = 8.0 x 10~3) and the branching ratio for the Cu 66 gamma line (9.5%), the average generation rate of Cu 66 isotope in the "short" runs ((£) «4000s) is estimated as (7) = 1.73 ± 0.43 at/s. Taking into consideration the generation and decay of the Cu 66 nucleus for the detection time (t) a "corrected rate" of Cu 66 isotope generation of (Q) = 3.46 ± 0.87 at. Cu 6 6 /s (sample area) is obtained (Table 1).
386
1039.4 keV
A-
(a)
2"
** 1C3C
820 1040
a--* m T05tr
„ E(keV)
-2-
Figure 3.
The change in neutron flux was also monitored. In the 2219-2229 keV energy range corresponding to thermal neutron capture in the hydrogen-containing moderator, a statistically significant decrease (negative A<J> value) is observed for Cu-1 runs with combined electrolysis and UTNF (Table 1). In contrast, the corresponding A $ difference for Cu-2 samples is not significant [as also for (1) interval]. As shown earlier,3 this decrease in WTNF flux provides evidence of an anomalous thermal neutron capture during combined electrolysis and WTNF (compared to normal neutron capture without electrolysis, i.e., with j = 0). The fraction of thermalized neutron flux absorbed by the Cu-1 cathode under electrolysis was Anc = {ANt)/{Nb) = 6.5%. Here (ANt) = —1.42 x 10~ 3 cps is the difference between foreground and background count rates, averaged over the total number of measurements, taking into account the statistical weight of each measurement. 14 Also (iVb) = N 7 m formula (1) is the mean background count rate within interval (2), taken for all measurements with Cu-1 samples. Thus, the absolute value of the thermalized neutron flux captured in the sample was found to be A $ n = 11.8 ± 2.8n/scm 2 . The calculated fractional absorption Anc value of 6.5% makes it possible to directly estimate the change in the effective thermalized neutron capture coefficient (Kg.) for the hardened Cu-1 samples during combined electrolysis and UTNF irradiation. Accordingly to Eq. (2) for the Cu sample with thickness of hcu = 0.03 cm
387
used here, aeg = 26.5 barn, and K& = 7.4. In other words, the probability of thermal neutron capture in the bulk Cu-1 sample during combined electrolysis and UTNF action is 7.4 times higher than that for the "normal" state, i.e., either in the absence of electrolysis or when annealed pure copper (Cu-2) is used. Now it is possible to estimate an isotopic abundance (x) for the base Cu 65 leading to the production rate (Q) of Cu 66 nuclei observed in the Cu-1 cathodes. This permits a verification that the average value (x) actually corresponded to Cu 65 isotope concentration in Cu sample if the effective cross section aes = 26.5 barn is employed for a UTNF flux of $ n = 180n/scm 2 . The neutron activation equation can be solved for (x) to give: _ {X)
X(Q)(t) S4>n
[ )
where A = 2.3 x 1 0 ~ 3 s _ 1 is the decay constant for Cu 66 ; (t) = 4000s is a mean foreground run time; S = 10 cm 2 is the Cu sample's area, hcu = 0.03 cm and "•Cu = 8-4 x 1 0 2 2 c m - 3 the same as in formula (2). In accordance with Eq. (3), ifCTthis taken as cres, the fraction of Cu nuclei absorbing neutrons in the Cu-1 sample is (x) = 0.26 ±0.11. This value is in a reasonable agreement with natural isotopic abunadance of Cu 65 (~31%) in the copper isotopic mixture. Thus, the Cu 66 isotope generation observed, is generally consistent with the assumed anomalous neutron capture by Cu 65 nucleus in the Cu-1 cathode under combined electrolysis and UTNF. Therefore, the simultaneous change in neutron absorption and Cu 66 isotope generation in the Cu-1 electrode during combined electrolysis and UTNF irradiation provides a strong confirmation on the anomalous thermalized neutron absorption effect under these unique conditions. The macro and micro-deformations (bending and fracture of subsurface layer) observed in the same runs would allow to be related to the anomalous absorption in some fashion. 4. Discussions We consider possible physical reasons of anomalous neutron capture and plastic deformations of Pd and Cu cathodes during combined WTNF and electrolysis using as an example Cu-cathode experimental data. Based on the results of previous studies 3 - 5 and the present experiments, the following conditions appear to be required to create these effects: (a) generation of high-energy excitations in the crystal, caused the non-equilibrium optic phonon mode formation and/or population of high-energy level phonon states with energy E > hui£,, where h is the Plank constant, WD is the Debye frequency for the solid; (b) presence of an WTNF with a broad energy spectra that overlaps the characteristic optic mode frequency of the solid being irradiated; (c) presence of an essentially isotropic field (not a beam) of thermalized neutrons that are able to interact with all different phonon wave vector k directions when the crystal has no particular orientation with refernce to neutron flux.
388
Conditions (b) and (c) are already fulfilled by use of neutron cavity (Fig. 1). The thermalized neutron flux is isotropically distributed inside the moderator cavity and possesses a Maxwellian-like spectrum with an estimated mean energy (En) 80meV. Condition (a) is achieved through the electrolysis process, which loads the copper subsurface layer with hydrogen to a concentration x = H/Cu ~ 0.1 4 to a depth of h ~ 1 0 ~ 7 - 1 0 - 6 cm, producing a non-uniform deformation of the Cu sample. 3 This condition can lead to increased neutron inelastic scattering by optic phonons causing an "anomalous" absorption by effectively reducing the average neutron energy. To show this, consider the generalized equation for energy and momentum conservation for inelastic scattering of thermalized neutrons by lattice phonons in the single phonon scattering case:
{K2/^n=K/^n±^[K-^h\ 2
(4)
where [En = P^/2m n and E'n = (Pn /2m n ] and ( P n , P' n are, respectively, the energies and momentums of a neutron (m n is a neutron mass) before and after interaction with phonons with frequency w s (k) = u)s[{P'n—Pn)h], where the subscript s represents the phonon branch. The sign (+) in Eq. (4) indicates phonon absorption, while the sign (—) corresponds to phonon emission and are assumed to occur with equal probability. 18 In the case of the equilibrium cathode state (current off), neutrons will interact only with the equilibrium spectrum of phonons in the sample (fceT1). Under these conditions the probability of occupation of the states that correspond to the maximal frequency WD (or to Debye wave vector ISD ) is very small. Hence, the values of the wave vector k in the u>B(k) expression are quite small also, i.e., |k| D. Then, the change in neutron energy during inelastic scattering (i.e., optic phonon emission or absorption) is negligibly small. In contrast, during electrolysis with UTNF, the hydrogen loading creates conditions for strong non-equilibrium optic phonon mode generation. Then the population of phonon states with high k values (|k| ~ ko) significantly increases. For the copper-hydrogen system, and the similar f.c.c. metal hydrides the optic phonon vibration mode located in the range of 50-100 meV4 is near to the mean energy of the thermalized neutrons (50-110meV), i.e., En ~ huis(k). Then two limiting options for a change in neutron energy E'n follow for Eq. (4), namely: (1) E'n ~2/iu; s (k), corresponding to phonon absorption (+ sign) and (2) E'n —>0, with phonon emission ( - sign). Phonon absorption (case #1) results in only a small decrease (~ y 2 in the thermalized neutron cross section value (
389
reduces to | P j , - P n | = hkD. Then, the mean interatomic distance ( r d ) at the sites of internal strain concentration (i.e., where the strong neutron-lattice optic phonon coupling occurs) approaches ra = (97r/2) 1 / 3 kQ 1 . In the case of f.c.c. Cu, the lattice spacing rd = 1.28 A, or about one-third of the equilibrium lattice parameter of a0 = 3.6 A. A reduced spacing like this is characteristic of a region with strongly disordered defect sites such as caused by a large density of edge dislocation cores (D). This reasoning is in accordance with the experimental observation of anomalous U T N F capture only in the pretreated ("hardened") Cu:Si cathodes with a highinternal strain concentration. T h e strain results in an increased concentration of edge dislocations. Regardless of the actual mechanism of anomalous U T N F capture during combined electrolysis and U T N F , the energy associated with the strong plastic deformation in the Cu cathode must be supplied by anomalous source t h a t can not be explained by neutron absorption alone. It seems logical to consider energy transfer to the crystalline lattice from the compound nucleus formed during thermal neutron capture in the Cu. Otherwise, it is impossible to explain appearance of excessive plastic flow, since the total energy of t h e U T N F flux entering the sample is negligibly low (En ^ 1 0 e V / s c m 2 ) compared t o t h a t needed for deformation ( ~ 1 0 7 e V / s c m 2 ) . However, in the case of "normal" radiation decay [(n/y) - reaction], taking into account the g a m m a attenuation coefficient for the 0.03 cm thick Cu foil (in ~ 8.0 x 1 0 ~ 3 c m ^ 1 ) and assuming (E-y) ~ 8 . 0 M e V , the autointegral gamma-decay energy absorbed in the sample would be at least two orders of magnitude less then t h a t required to provide the observed plastic deformation. Thus, the explanation appears to require a hypothesis of direct transfer of the neutron induced excitation energy of the Cu nucleus to the lattice, i.e., "radiationless" nuclear decay. T h e mechanism describing radiationless nuclear decay in a highly loaded metal hydride/deuteride has been considered in Refs. 6 and 7. It is suggested t h a t significant electromagnetic excitation of crystalline lattice of f.c.c. hydrides can be produced by coherent oscillations of metal electrons near the Fermi level. T h e resulting high-intensity electric field interacts with the compound (excited) nucleon suppressing the gamma-decay process and leads to situation where lattice atoms behave collectively to absorb recoil energy. 7 Such collective coherent recoil by the lattice as whole is a t t r i b u t e d to p h o n o n / p l a s m o n emission generated within local zones surrounding the nucleus. 6 , 7 This view suggests t h a t the anomalous capture must occur within the zones of internal strain localization ("selective capture" 4 ) , e.g., within t h e edge dislocation cores localized in t h e defect subsurface layer of cathode. In scope of the above considerations energy conservation for the radiationless process of "selective capture" can be represented as: nth+D -
huD+no+A*
- • (Ax+1*
— Ax+1+Wc(MeV)
(5)
where n t h is a thermalized neutron, D is a lattice defect, no is a neutron having roughly "zero" energy; Ax and Ax+1 are the acceptor nucleus before and after neutron capture, respectively (for example, Ax = Cu 6 5 , Ax+1 = C u 6 6 ) ; Wc is the
390
binding energy of a neutron in the Ax+1 nucleus, which can be coherently transferred to the lattice following de-excitation of the (Ax+1)* compound nucleus. This proposed model for anomalous capture under combined electrolysis and WTNF also provides some insight into the electrolysis "duration effect" on the gamma-activity of 1039.4 keV band observed for the Cu-1 cathodes. An important point, underlying the non-equilibrium situation with respect to the Cu 65 isotope concentration in the subsurface layer of the Cu-1 cathode, is based on the known change in atomic and isotope content at the cathode surface during electrolysis in water solutions. The reasons for this change are self-diffusion of the host-metal by a vacancy mechanism5 and impurity migration induced by mechanical stress stimulated by hydrogen impingement into the metal. Deformation in the lattice produced by hydrogen loading and enhanced with WTNF, 4 ' 5 will induce motion of dislocations with their impurity/vacancies (point defects) atmospheres toward the surface. As stressed earlier, we assume that anomalous neutron capture takes place only within the strained near-the-surface layer corresponding to the hydrogen penetration depth in Cu (h ~ 10~ 6 -10 - 5 cm). Initially, when electrolysis first starts, this layer consists mainly of the pristine copper atoms. Under the mechanical strain induced by the hydrogen implantation into the surface, defects (including impurities and vacancies) diffuse toward the Cu surface causing impurity aggregation near dislocation cores. Adsorption of electrolyte atoms at the Cu surface and the hydrogen also represent an additional source of impurities in this layer. As a result of both processes, the cathode subsurface layer will be enriched with impurity atoms reducing the density of pristine Cu-atoms. At the same time Cu atoms will migrate away from the surface, moving toward the bulk where the mechanical stress is lower. The resulting decrease in Cu 65 atom concentration in the subsurface layer would decrease the Cu 66 generation rate per unit volume. Only a 10% decrease in Cu-65 concentration in the subsurface layer of 10-100 nm thick (which could possibly be reached during 2 h of electrolysis) would cause the 1039 keV count rate drop to approach the background level. Neutron capture by impurity nuclei might produce other isotopes emitting gamma radiation (if any) outside the range of expected Cu 66 isotope (1039 ± lOkeV). This range was not covered by present study. In summary, we propose that the excessive plastic flow observed is a consequence of dislocation and point defect (impurities) transport activation due to radiationless energy transfer (Wc) to Cu lattice from the compound nuclei, which are formed at the UTNF capture sites. In this case the synergetic action of "low-radiation dose" (UTNF) effect on the non-equilibrium solid structure is cleared up because the energy for defect transport activation is the result of the process of "selective" neutron capture energy transformation. 5. Conclusions In present paper, we studied the process of thermalized neutron absorption in Pd and Cu cathodes during their loading by deuterium and hydrogen, respectively. We
391 found anomalous enhancement of W T N F absorption (suggesting about 7.5 times increase in effective capture cross-section) as well as of plastic deformation/flow in b o t h cathodes under combined electrolysis and W T N F . This anomalous processes in Cu and P d cathodes could be explained energetically suggesting a selective radiationless thermalized neutron capture b e n e a t h the surface at the high-internal strain concentration sites. T h e results present a simplest (avoid Coulomb barrier penetration issue) evidence for nuclei-lattice exchange, resulting an increase in neutron capture probability and radiationless de-excitation of the compound nuclei formed in the lattice.
References 1. H. Yuki, J. Kasagi, A. G. Lipson et al, JETP Lett. 68 785 (1998). 2. H. S. Bosch, and G. M. Halle, Nucl. Fusion 32 611 (1994). 3. A. G. Lipson, G. H. Miley, V. Kuznetsov, and E. I. Saunin, in Nuclear Science Symposium Record, 2001 IEEE, Vol. 1, pp. 104-108 (2001). 4. A. G. Lipson, G. H. Miley, and V. A. Kuznetsov, Radiat. Phys. Chem. 69 7 (2004). 5. A. Lipson et al, Phys. Solid State 45 1409 (2003). 6. P. L. Hagelstein, Anomalies in metal deuterides, in Proceedings of the ICCF-9, Beijing, May 2002. 7. V. Violante, A. Torre, G. Selvaggi, and G. H. Miley, Fusion Technol. 39 266 (2001).
A N OVERVIEW OF E X P E R I M E N T A L STUDIES O N H / P d OVER-LOADING W I T H T H I N Pd WIRES A N D D I F F E R E N T ELECTROLYTIC SOLUTIONS
A. S P A L L O N E A N D F . C E L A N I INFN-LNF,
Via Enrico
Fermi,
00044 Frascati
(Roma),
Italy
P. M A R I N I A N D V. DI S T E F A N O EURESYS,
Via Lero 30, 00129 Roma,
Italy
Hundreds of electrolytic loading tests of thin Pd wires in different experimental conditions have been performed in order to find out the best procedures for stable, high hydrogen overloading into the palladium lattice. In a very dilute acid solution thin Pd cathodes (50 or 100 /»m in diameter) and thick Pt anodes (0.5 mm in diameter) were used in a parallel or coaxial geometry. Normalised resistance (R/Ro) of the Pd cathode was on-line and continuously measured in order to determine the actual H / P d values. Different electrolytic solutions have been tested by adding to the acid solution very low amounts of Ca, Sr, Li, and Hg ions; high loading H / P d ratios have been achieved with a satisfactory grade of reproducibility. Several loading procedures have been performed in a wide range of electrolysis current (from a few mA up to 100 mA) and at different Hg ion concentrations. The obtained results allowed for the definition of a loading protocol that ensures very high H / P d over-loading. Stable R/Ro < 1.2 values (corresponding to H / P d ratios > 1) can be currently achieved with an extremely low power electrolytic supply (10 V, 5 mA).
1. Introduction During the last 6 years a lot of effort was spent in finding the best hydrogen loading procedures for thin Pd cathodes. Most researchers agree that in cold fusion experiments, in order to obtain stable and reproducible excess heat, it is necessary to achieve and maintain very high D/Pd (>0.85) loading ratios. 1 The poor results generally achieved by the conventional electrolytic techniques, based on the use of LiOH solutions, especially from the point of view of their reproducibility, induced us to develop a completely different approach. In fact, in our previous papers, we have reported a reproducible procedure to achieve very high loading ratios using palladium thin wires (H/Pd « l ) . 2 , 3 This procedure is based on the increasing of the cathodic over-voltage (which is known to be the main controlling parameter of the H(D)-Pd loading) by modifying the nature of the cathode surface (i.e., by inducing the formation of a very thin layer of an alkaline-earth carbonate on its surface). 392
393
2. Evaluation of the H / P d Ratio In order to estimate the actual H/Pd atomic ratio of the Pd cathode during the electrolytic loading process, we measure the normalised resistance (R/Ro) of the Pd wire; i.e., the ratio between the actual resistance (R, during the loading) and the resistance of the electrode at the beginning of the electrolysis (i?o), when the value H/Pd = 0. The loading ratio was inferred and continuously monitored by means of the wellknown relationship 4-6 between the resistance and the H(D) content in the Pd matrix (Fig. 1). The actual known values of this relationship terminate at H/Pd = 0.9, corresponding to R/Ro = 1.40. Beyond this value the correspondence is estimated by a linear extrapolation. Accordingly, we estimate that the ratio H/Pd = 1.00 is achieved when R/RQ = 1.20. 2
1.8
1.6
of 1.4
1.2
1 0.00
0.20
0.40
0.60
0.80
1.00
H(D)/Pd Figure 1.
Normalized Resistance R/RQ vs. H ( D ) / P d .
3. Experimental Apparatus A schematic diagram of the experimental set-up is shown in Fig. 2. The vessels are typically cylindrical glass beakers of different sizes (from 0.5 to 51). The power supply can operate either at constant DC current or at constant DC voltage. The cathode is grounded. The voltage is applied to the anode through an impedance adapter circuit (impedance booster), in order to avoid current feedback from the AC measuring circuit. The latter is composed of a pulse generator (allowing for sinusoidal, square and triangular wave forms; we always used the sinusoidal ones) and a coupling circuit (ground return, for both for the DC and AC generators).
394 Electrolysis
AfS^
a.c. out. Pt anode
Pd cathode
Ground return (a.c. + D.C.) [DC+ac->DVM]
a.c. in • D.C
B
(Electrolytic cell)
a.c. pulser
Figure 2.
Electrolytic cell: a schematic view.
Temperature sensors (based on silicon integrated circuits) are located inside the cell (in the solution at three different levels) and outside the cell (two sensors for the thermal bath and one for room temperature) and are monitored on-line. The Pd cathode, because of its favorable surface/volume ratio, allows for very fast hydrogen absorption and its high resistance (about 8 0 ) improves both the accuracy and the precision of the measurements. Furthermore, the \jr dependence of the electric field around the wire creates a sharp increase of the pH value in its proximity, promoting the carbonate precipitation in that region. (For more details, see Refs. 2 and 3.) The geometry of the electrolytic cell strongly affects the loading process: the relative position of the electrodes is crucial for a proper set up of the primary electric fields during the electrolysis.7 Moreover, we have to take into account that during the loading the Pd wire's length remarkably increases (5-15%); the wire is consequently forced to bend and the original separation of the electrodes could be significantly changed. We tested two different P d - P t electrodes separation values (variable from 1.5 to 7 cm) in two different geometries: (1) a parallel geometry with Pd and P t wires of the same length at the same separation, (2) a Pd central axial geometry with 4 Pt wires cylindrically located around the cathode at the same separation. The electrodes are about 25 cm long; The Pt wire (sector AB as drawn in Fig. 2) is 1 mm thick; Pd cathodes of two different sizes (50 or 100 /an thickness) are used. A pick-up junction divides the Pd wire into two equally long sections of electric resistance 2 or 8 0 s , respectively, for the 100 or 50/mi Pd wire diameters. This
395
allows for the measurement of the resistances of the corresponding wire segments (sectors CD and DE are named "up" and "down" in Fig. 2). H 2 0 , ethyl alcohol (C 2 H 5 OH) or methyl alcohol (CH 3 OH) was used for the preparation of the electrolyte. In order to reduce the impurities present in commercial heavy water 8 ' 9 some tests using alcohol based electrolytes were previously performed with D2O/C2H5OD solvents. In the present work the alcohol-based electrolytes were also tested for hydrogen loading. Very low concentrations (less than lmmol) of HC1 or H2SO4 were added to the electrolytes in order to maintain the pH around 4.5-5.5; the anode-cathode electrolytic resistance ranged between 1 and 5 k$7. Small amounts (tenth of fimol) of different alkaline elements such as Ca, Sr, and Li were added to the electrolyte, according to the original procedure previously developed in order to improve the H/Pd loading (motivations and details of this addition are also reported in Ref. 3). Many tests were performed by adding a very small amount of HgCl2 (ranging from 0.1 to 10/xmol) to the electrolyte. In some tests very small amounts of Hg (estimated on the order of a tenth of nmol) were actually present in the electrolyte (nominally Hg 2 + free). Because of the de-loading process of the cathode normally effected at the end of a set of experiments, the Hg amalgam previously formed on the Pd surface in the cathodic cycles is stripped away during the final anodic cycle. Some residual traces of Hg normally remains on the Pt surface even after the Hg containing electrolyte has been fully removed. Hg traces on the Pt surface go back into solution as soon as the cathodic cycle of the new set of experiments starts up. Mercury, as is shown below, plays a fundamental role in the over-loading process. 4. H / P d Loading Procedure In the achievement of very high H/Pd loadings, the role played by the electric parameters (anode-cathode voltage and current) is crucial for any given cell geometry and electrolyte. The primary and secondary electric field7 operating on the Pd cathode may produce an Hg and alkaline element deposit with a particular structure, which seems to be responsible for the Pd-bulk over-loading. We tried several procedures to produce this particular structure. We changed electrolysis current values not only when the electrolysis started up [start in low current (SL) or start in high current (SH)] but also during electrolysis. The Pd electrode was loaded, and the loading was steady, after the value of R/RQ was reached 1.8 (Fig. 1). Low current (Low: L) means just a few milliamperes (2-10 mA and 5-15 V). High current (High: H) means some tens of milliamperes (30-150 mA and 50-200 V) and middle current (M) is in the middle range. In the following a list of these loading procedures (depending on the Hg deposition onto the Pd) is reported: • Start and load: Start at constant current (low or high) until the Pd cathode reaches a consistent over-loading (R/RQ < 1.3). In general, if the Hg
396
concentration is high, when the current is switched off, a very slow de-loading occurs (although in one test no de-loading was observed for two days). 10 We call this condition H/Pd-locked. • OFFJON: The Pd electrode is loaded just over the R/RQ peak, and the current is switched off, allowing the Pd to de-load to the peak. Then the current is switched on again (either at low or at high current). This cycle can be repeated several times until the Pd reaches a high loading. This procedure can be applied when the Hg concentration is very low and the "ON" condition is corresponding to high current during the previous cycles. • L/H: Similar to OFF/ON, but the current is not totally switched off. "OFF" corresponds to a low current while "ON" corresponds to a high current. • L/H/L: Similar to L/H, but after the Pd achieves a high and steady loading at a high current condition, the current is then set to a low value. At this low current a rapid de-loading occurs, but sometimes the de-loading stops and the Pd reloads slowly up to high values (sometimes higher than the ones obtainable at high current). This procedure is effective when Hg is neither very diluted nor very concentrated. 5. Experimental Tests Table 1 shows only the most revealing tests out of the many hundreds that were performed. In this table all the parameters cited above are listed, that is: cell geometry, Pd sample thickness, electrolyte solution, electric values, and loading procedure. The column "best R/RQ" means the final H/Pd over-loading reached while applying the proper procedure (relative to the "up" and "down" Pd sectors). The 20 tests in Table 1 are in chronological order (from 1998 to 2004) and some of them have been repeated many times. The "best R/RQ" reproducibility was very poor at the beginning (about 10%) and increased with time reaching reasonably good values (>50%) at present, particularly when the Hg concentration is finely tuned and an optimal "current cycle" procedure is adopted. Figures 3 and 4 show the values of R/RQ vs. time corresponding to the parameters in the first two rows of Table 1. In these figures it can be seen that alkaline elements like Ca and Sr are quite equivalent for the achievement of high loading with a high Hg concentration. A typical Start and Load procedure is also shown. In this case, the Pd electrode very often appears to be covered with a very thin Hg film, which is very impervious. This explains the observed very slow de-loading process when the current is switched off (a load and lock condition). In Figs. 5 and 6, a typical OFF/ON operation is shown in connection with runs with Sr and "residual" Hg (data from Table 1, rows 3 and 4). This shows that it is possible to achieve a high and steady loading starting from a low loading (R/RQ = 1.8 —> 1.2). Moreover, the de-loading curve (electrolysis OFF for 1 day) shows that the resistance measurements are correct and consistent (peak at R/RQ = 1.8 returning to R/RQ = 1.0, the starting condition). The de-loading vs.
397
" ' ' ' '*'!
(Ca2+)
1.8 .. -
// ^ b s ;
1.6 -
5
up/*
down l
•/
\
up
•
down^vk
down
1.4 MR.....
1.2 ..
----- .
100
. .
10000
1000
-
i
100000
Time (s) Figure 3.
Test "Start and Load" with Ca ions and high Hg concentration (Tablet, 1).
time curve allows the observation of the typical (3 —> a + (3 Pd-H lattice phase transition (occurring at R/RQ = 1.68, H/Pd = 0.6 at room temperature and at a pressure of 1 atm. 1 1 ). Figure 7 (row 7) shows the role played by the Hg addition during the run (at the time of about 75 ks). In combination with a Low/High operation; high loading values persist even when the current is decreased. The effects of the substitution of ethyl alcohol for H2O (as a base for the electrolyte) are shown in Fig. 8 (row 11). The presence of Sr and Hg in a sulphuric environment is effective for reaching a very high loading, when applying an OFF/High/Low current procedure.
1.6
-
?-
;
^ V \-
[
^H.
SE 1.4
: 1.2 '-
/ /
(Sr2+)
'
down
1.8
! ;
-
•
-\ K ^r ss **«-_do wn
.
;
. •
up
1
1
100
!
•
1000
10000
100000
Time (s) Figure 4.
Test "Start and Load" with Sr + Hg (10 /J,M), ending with a H / P d "lock" (Table 1, 2).
398
250
200
< E
150
- 100
80000
85000
90000
95000
100000
Time (s)
Figure 5.
Test of O F F / O N procedure with Sr (+Hg very low concentration) (Table 1,3).
Even with very small Hg additions (down to 0.5/xmol), it is possible to reach very high loadings (R/Ro = 1.05) as shown in Fig. 9 (row 15). In this case, just a Start-Low/High current variation is sufficient to trigger the loading process. By exchanging Sr with Li similar high loading effects are obtained (rows 16-19) but additions of fair amounts of Hg (1 /xmol), cause the role played by the electrolytic current to become crucial, as shown in Fig. 10 (row 20). In this plot, the first run is performed at low current (5 mA) resulting in a poor loading. On the contrary, the subsequent run, which was started with a medium range current of 36 mA (after a de-loading at R/RQ = 1, with -5 mA anodic current) a steady high loading (R/Ro = 1.2) was obtained within a few hours.
<E
1 •
0
20000 40000 60000 80000 100000120000140000160000
Time (s)
Figure 6.
Test O F F / O N with Sr (+very low Hg) and de-loading run in O F F (Table 1,4).
399 200
2000
4000
6000
8000
10000
12000
Time (s) Figure 7.
Test with Sr and Hg addition during the run with a L/H operation (Table 1,7).
Several tests with methyl alcohol have also been performed showing loadings around R/Ro — 1.3. We never measured "anomalous" temperature variations inside the cell even when very high loadings were achieved.
100
< £
0
Figure 8.
OFF 5000
10000 15000 Time (s)
20000
25000
Test with Sr + Hg in an ethylic solution; S t a r t - O F F / H / L procedure (Table 1, 11).
100
03
>
0
10000
20000
30000
40000
50000
Time (s) Figure 9.
Test with Sr + Hg (0.5 fiM); S t a r t - L / H / M procedure (Table 1, 15).
OFF 0
20000 40000 60000 80000 100000120000140000
Time (s) ure 10.
Test with Li + Hg (1 fiM); Start-L and Start-H procedures comparison (Table 1, 20).
Table 1. The most relevant tests (out of many hundreds) showing high over-loadings performed with different solutions, different added elements and different loading procedures (tests performed at room temperature, 22 ± 5°C). Pd5> (fim)
Electrolysis solution (HC1 in
Alkaline element (in /iM)
HgCl 2 (in pM)
Power supply (V; mA)
LOAD procedure
"Best" (u;d)
1
50
CaCl 2 = 70
Hgg « 10
(60;20)
Start and load
(1.28;1.35)
2
50
SrCl 2 = 35
H g « 10
(40;20)
Start and load
3
50
SrCl 2 = 180
(150;90)
OFF/ON
50
(150;65)
(1.10;1.11)
50
(100;77)
OFF/ON (+ deload) OFF/ON
K - A = 6 cm geo. parallel Idem
5
(1.20;1.25)
Idem
6
50
(150;70)
OFF/ON
(1.25;1.30)
Idem
7
50
Very low («0.1) Very low («0.1) Very low («0.1) Very low («0.1) Hg = 10 cm 3
(1.15;1.18) (load + lock) (1.16;1.20)
4
(90;105) -> (40;50)
Low/high /low
(1.12;1.15)
8
50
(140;133)
OFF/ON
(1.15;1.15)
50
(6.5;4.4)
High/low
(1.28;1.28)
Idem
10
100
Very low («0.1) Very low («0.1) Hg = 5
K - A = 1.5 cm geom. axial Idem
9
(11;2)
Start and load
(1.25;1.30)
Idem
11
100
H2O=2400cm3 + HC1 = 140 H 2 0=2400 cm 3 + HC1 = 140 H2O=2400cm3 + HC1 = 210 H 2 0 = 2400 cm 3 + HC1 = 210 H2O=2400cm3 + HC1 = 500 H2O=2400cm3 + HC1 = 250 H 2 0 = 5000 cm 3 + HC1 = 250 H2O=1200cm3 + HC1 = 20 H 2 0 = 1200 cm 3 + HC1 = 20 Ethyl=395 cm 3 + H 2 0 =20 cm 3 H 2 S 0 4 = 25 + HC1 = 210 Ethyl = 395 cm 3 H „ S 0 4 = 25 + HC1 = 210
Hg = 2.5
(11;2.5)
Start OFF/H/L
(1.15;1.15)
Idem
SrCl 2 = 180 SrCl 2 = 20 SrCl 2 = 160 S r S 0 4 = 60 SrCl 2 = 30 SrCl 2 = 30 S r C 0 3 = 17 mg (powder)
S r C 0 3 = 17 mg (powder)
R/R0
Remark (set-up) K-A = 7 cm geo. parallel Idem
Table 1.
12
Continued.
P d $ (Mm)
Electrolysis solution (HCl in MM)
Alkaline element (in [iM)
HgCl 2 (in fjM)
Power supply (V; mA)
LOAD procedure
"Best" (u;d)
100
Ethyl=395 cm 3 + H20 = 20 cm 3 H 2 S 0 4 = 10 HCl = 200 H2O=400cm3 HCl = 200 H2O=400cm3 HCl = 200 H 2 0 = 4 2 0 cm 3 HCl = 70
SrCO3=30mg (powder)
Hg = 8
(12;3.7) - (12;1)
Start and load
(1.34;1.34)
Idem
S r C 0 3 = 85mg (powder) SrCl 2 (6H 2 0) = 53 mg SrC03 = 7mg (powder)
Hg = 5
(45;60)
Start in L / M / H
(1.30;1.35)
Idem
Hg = 2.5
(6;7)
Start and load
(1.33;1.36)
Idem
Hg = 0.5
(10;6) -
Start in L/H
(1.07;1.05)
Idem
Hg = 0.5
(50;45) (10;6)
H/L
(1.31;1.26)
Idem
L/H/L
(1.25;1.25) (1.21 in H) (1.33;1.31) (1.19 in H) (1.30;1.30) (1.22 in H) - • (1.5;1.5) -> (1.2;1.2)
Idem
13
100
14
100
15
50
16
50
17
50
18
50
19
50
20
50
R/Ro
Remark (set-up)
+ + + +
H2O=420cm3 + HCl = 70 H 2 0 = 420 cm 3 4- HCl = 70 H2O=420cm3 + HC1= 70 H2O=420cm3 + HCl = 70 H2O=420cm3 + HCl = 100
SrCOs = 7mg (powder) LiOH = 50
Hg = 0 -> 0.2
LiOH = 50
Hg = 0.3
LiOH = 50
Hg = 0.1
LiOH = 50
Hg = 1
(10;6) (48;34) (10;5) - • (48;34) (10;6) -> (49;53) (10;5) (42;36)
—>
L/H/L L/H/L Start in L—> Start in H-+
Idem Idem Idem
403
6.
Discussion
Taking into account also previous studies (particularly the ones performed during the last 2years), we can confirm t h a t our procedure for the P d - H overloading up to 1:1 loading ratio is effective using b o t h aqueous and alcoholic solutions. This method is based on a proper deposition of a alkaline and mercury containing thin film onto the P d cathode surface (independent of the wire section). Particular current cycles can improve the loading. T h e complexity of these tests and the large spread of the process parameters distribution, can be tracked down t o a peculiar deposition layer (ranging from 20 to 200 nm) onto the P d cathode. We conjecture the formation of a nano-structure on the surface t h a t can give rise to relevant electrochemical potentials and locally high current densities. 1 2 During the performance of a test consisting of a dozen of high current loadings (120 V; 60 mA) at high Hg concentration (about 10//mol it was observed t h a t after each loading/de-loading cycle the RQ value increased some percent. At the end of the test we measured t h e P d wire thickness and found a decrease in diameter from t h e original 50 t o 46 (jm. These values are consistent with the increase of RQ with respect t o t h e one a t t h e beginning of t h e test. It is reasonable t o assume t h a t t h e alkaline, Hg and P d layer formed during the loading (cathodic) cycle resulted in the removal of about a 200 n m P d layer during each de-loading (anodic) cycle. A further structural analysis of this deposition is required to confirm the Tightness of our conjecture. It was shown 9 t h a t the achievement of high loadings with D2O instead of H2O is much more difficult. Nevertheless, we think t h a t our method could be transferred to heavy water solutions. New tests are in progress showing encouraging preliminary results (R/RQ == 1.55 at a low current regime of 5 m A ) . T h e obstacles limiting the over-loading of P d - D systems are mainly due to impurities present in the commercial D2O.
Acknowledgements We are indebted t o Eng. Alfredo Mancini for his valuable support. We are grateful t o Dr. Daniele Garbelli and Dr Luca Gamberale for their important help and we want to t h a n k Dr Mike McKubre for his useful suggestions. Regarding the last tests, it has been crucial the expertness of Mr Vincenzo Andreassi, our skilled technician.
References 1. M.C.H. McKubre, et al, Frontiers of cold fusion, in Proceedings of the ICCF3, 1992, Vol. 5 (Nagoya, Japan, 1993). 2. F. Celani and A. Spallone et al., "High hydrogen loading into thin palladium wires through precipitate of alkaline-earth carbonate on the surface of cathode: evidence of new phases in the Pd-H system and unexpected problems due to bacteria contamination in the heavy water, in F. Scaramuzzi (ed.), Proceedings of the 8th International
404
3.
4. 5. 6. 7. 8.
9.
10.
11.
12.
Conference on Cold Fusion, SIF - Conference Proceedings, Vol. 70 (Lerici (La Spezia), Italy 21-26 May 2000); Compositori-Bologna, Italy, 2000, pp. 181-190. A. Spallone, F. Celani, P. Marini, and V. di Stefano, New electrolytic procedure for the obtainment of very high H/Pd loading ratios. Preliminary attempts for its application to the D-Pd system, in F. Scaramuzzi (ed.), Proceedings of the "8th International Conference on Cold Fusion, SIF - Conference Proceedings, Vol. 70 (Lerici (La Spezia), Italy 21-26 May 2000); Compositori-Bologna, Italy, 2000, pp. 191-198. B. Baranowski and R. Wisniewski, Phys. Stat. Sol. 35, 539 (1969). J.C. Barton, F.A. Lewis, and I. Woodward, Trans. Faraday Soc. 59, 1201 (1963). M. McKubre, et al, in Proceedings of the ICCF1 Conference (Salt Lake City, Utah, March 28-31, 1990), pp. 20-31. P. Gallone, Principi dei processi elettrochimici (Tamburini Editore Milano, 1970), pp. 197-199 (in Italian). F. Celani and A. Spallone, et al., Electrochemical D loading of palladium wires by heavy ethyl-alcohol and water electrolyte, related to ralstonia bacteria problematics, in X.Z. Li (ed.), Proceedings of the 9th International Conference on Cold Fusion, Condensed Matter Nuclear Science (Beijing, China, 19-24 May 2002), pp. 29-35. A. Spallone, F. Celani, P. Marini, and V. di Stefano, Experimental studies to achieve H / P d loading ratio close to 1 in thin wires, using different electrolytic solutions, in X.Z. Li (ed.), Proceedings of the 9th International Conference on Cold Fusion, Condensed Matter Nuclear Science (Beijing, China, 19-24 May 2002), pp. 319-322. A. Spallone, F. Celani, P. Marini, and V. di Stefano, A reproducible method to achieve very high (over 1:1) H/Pd loading ratio using thin wires in acidic solution with addition of very low concentration impurities. Presented at the UIV Workshop on Anomalies in Hydrogen/Deuterium Loaded Metals", Conf. Proc. 22-24 October 1999, Published by INFN, Asti, Italy: LNF-00/018 (P), 27 Giugno 2000. F. Celani, A. Spallone, P. Tripodi, et al, The effect of gamma-beta phase on H(D)/Pd overloading, in Proceedings of the Seventh International Conference on Cold Fusion, Vol. 1 (Vancouver BC, Canada, April 19-24, 1998), pp. 62-67. Y. Arata. "The formation of "Solid Deuterium" solidified inside crystal lattice and intense solid-state nuclear fusion ("Cold Fusion")". II Nuovo Saggiatore (Bollettino SIF) Vol. 20, Nos. 5-6, pp. 56-61 (2004).
P H O T O N A N D PARTICLE EMISSION, HEAT P R O D U C T I O N A N D SURFACE T R A N S F O R M A T I O N I N N i - H S Y S T E M
E . C A M P A R I , G. F A S A N O , S. F O C A R D I , G. L O R U S S O , V. G A B B A N I , V. M O N T A L B A N O , F . P I A N T E L L I , C. S T A N G H I N I , A N D S. V E R O N E S I Centro I.M.O
- sez.
Siena
E. C A M P A R I A N D S. F O C A R D I Physics
Department,
University
of Bologna
and Centro I.M.O
- sez. Siena,
Italy
V. M O N T A L B A N O A N D F . P I A N T E L L I Physics
Department,
University
of Siena
and Centro I.M.O
- sez. Siena,
Italy
S. V E R O N E S I I.N.F.M.
- UdR Siena
and Centro I.M.O
- sez. Siena,
Italy
The results obtained in several experiments on Ni—H system are presented here. Photon emission during the preliminary phases of activation and 1 H isotope absorption are shown; their correlation with the kind of surfaces (Ni and its alloys) and with neutron and other particle emission in the excitation progress and in large heat production is also presented. Finally, the SEM-EDAX analysis of the sample surfaces after same months of heat production is shown; new elements (not present in the initial analysis) appeared. The concentrations of these elements with atomic number between C and Zn, are compared to the unmodified parts of same samples that remained inside the cell, outside of the activated region.
1. Introduction In this paper, we report a selection of more interesting experimental results obtained in a Ni-H system in the last years. In particular, we present photon, neutron and particle emission, energy production and surface analysis on metal samples. We have studied systems composed by several kinds of metal samples, such as pure Ni, nickel alloys and nickel plated, of a cylindrical or planar shape, in a hydrogen atmosphere. In a typical experiment the samples were inserted in a cell, loaded with hydrogen at pressure in the range of 100-1000 mbar and kept at temperatures between 420 and 720 K. 1-3 Experiments were performed using three different kind of cells built to hold one cylindrical sample, four cylindrical samples, or three planar samples. The samples can be made of pure nickel, nickel alloys or they can be nickel-plated. They are chemically and physically cleaned by annealing cycles in vacuum and in hydrogen 405
406 (1) (2) (3)
W (5) (6) Th P. Tce
T5
Cell vessel External SS tube CF35 flanges Heater Ceramic cylinder Sample holder R 1 0 0 temperature se Type K thermocouple
T1
Figure 1. Two types of experimental cells, cylindrical sample.
Figure 2.
(a) Cell for three planar samples,
(b) Cell for a
A ceramic holder with a heater and a planar sample.
atmosphere. A typical experimental setup in these experiments is shown in Fig. 3.
Figure 3.
A schematic layout of experimental setup.
Usually, some temperature sensors are placed inside the cell in contact with the metal samples and heaters. Other thermocouples are places on the external wall of the cell in order to obtain a calorimetric measure of emitted power. All cell parameters, such as temperatures, pressure, power supply, are monitored by means of a computer data acquisition card (Labview).
407
2. Hydrogen Loading In the cell, thermal cycles are performed in vacuum and in a hydrogen atmosphere. The gas pressure is maintained in the range 100-1000 mbar. During hydrogen loading it is possible to recognize two distinct types of behavior. 5 ' 9 Some samples shows a fast loading with characteristic time of a few hours. In Fig. 4, a typical fast loading, well fitted by an exponential function, is shown.
Data: CARIAC_C Mode!: Exp D e d
1050-
Chi2/Dof = 33.9364 H 2 = 0.99248
1000
Y0 41 fl
829.11603 223.34338 72.28777
±4.3053 ±5.3927 ±3.95249
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900 850800
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'
600
f
*
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<
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800 1000 1200 1400 1600
f(min)
Figure 4.
An example of fast hydrogen loading.
In other experiments, a slow loading can be observed with characteristic time of days. In this case, the quantities of loaded gas are smaller and it is not easy to
400 350 i 300 CO
.a
250-
E
200150100 200
250
300
350
400
VO Figure 5.
An annealing cycle of slow hydrogen loading.
450
408
excite the metal sample in order to obtain excess heat. Figure 5 shows an annealing cycle during a slow loading. In two experiments 3 ' 7 , a considerable amount of energy was produced: a cell with a single cylindrical sample produced 900 MJ in 278 days; a second cell with four cylindrical samples produced 600 MJ in 319 days. Moreover, it is possible to observe different slow rates of loading depending on the sample's temperature. 5 ' 6 ' 9
3. Excess Heat Production In all experiments, excess heat production is detected by means of a calibration. At the beginning of the experiment, a set of calibration curves is constructed by plotting the temperature of several reference positions as a function of the input power. An increase of measured temperatures allows us to determine the emitted power by using a simple calorimetric model. 3
AP valued using temperature on a sample • AP valued using temperature on a external wall
i
10000
20000
30000
40000
50000
60000
Time (min) Figure 6. The differences Pout — -Pin are estimated during a heat production in one case by measuring a temperature inside the cell and, in the other one, by using a temperature on the external wall.
Many other examples of heat productions have been detected, such as that shown in Fig. 6. This shows a cell with planar samples where the measure of the energy production was made by using an internal probe of temperature and an external one. Both measurements give the same result. Thus, it is proved that no local phenomena on the internal probe (i.e., vortex) affected the measurement of heat production.
409
Figure 7. Nal 7-rays spectrum showing a peak superimposed on the background. Five following acquisitions are shown.
4. Photon, Neutron, and Particles Emission A paper dedicated to evidence of photon emission from these systems is presented elsewhere.10 Here we present, just as an example, an emission by a planar cell detected with a Nal counter. 5 The spectrum detected (Fig. 7) shows, superposed to the background, a peak centered at 661.5 ± 0.8 keV. Such peak energy was determined by using a high purity germanium detector. The emission arose when the cell was isolated from external influences and a sudden and brief decrease of the power supply induced a photon emission for a period of about 12 h.
3500 3000 2500 2
2000
c
O
1500 1000 500 0 350
400
450
500
E(keV) Figure 8. Gold activation 1 9 7 Au + n - 4 1 9 8 A u + 7 —• 1 9 8 H g * + e~ + P J is revealed by detecting the 7-ray emitted by excited Hg.
410
Figure 9. A charged particle emitted from a metal sample after loading, excitation, and a long heat excess production.
Figure 10.
A scanning electron microscope picture of a sample.
6000 5000 4000§
o O
3000
Figure 11.
Elemental analysis of unaltered surface.
Moreover, in a previous experiment a neutron emission was detected 4 both by using He 3 counters, shielded with paraffin or polythene for neutron thermalization, and by means of gold activation as shown in Fig. 8. In the same experiment, 5,7 particles emission has been detected by using a cloud chamber. An example of tracks is shown in Fig. 9.
411
•'•Ka
4000 -,
1
350030002500-
..
Ni L 20001500-
I C
-•'KQ
i
\
1000 -
Ga
Ko
I ".
5 0 0 - C. ' j .
SiK *
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/J
0 +—• 0
3
4
5
6
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l A ?
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1
Ni
:
Kc
7
8
* 10
<
E (keV)
Figure 12.
Example of elemental analysis of the sample.
2000 -i
1500
1000 C Ca„.
500
bU.
AI?
£Kp
Fe •'Win—'
,—r
- I LA
Zn,Kp
-t~
10
E(keV) Figure 13.
Another example of elemental analysis.
5. Surface Analysis The surface of the samples has been analyzed by using a SEM, which allows two different type of analysis: morphology and elemental distribution of the surface. An electron gun excites atoms in the surface (until a depth of few /Ltm), secondary electrons (SE) emitted by the atoms and back-scattered electrons (BSE) allow us to obtain images of the surface.
412
Furthermore, an X-microprobe with an energy-dispersive X-ray (EDX) system for elemental analysis is used to measure the elemental distribution on the surface in a quantitative fashion. T h e surface analysis of nickel alloys are presented in Ref. 11. Here we describe an analysis performed on a pure nickel specimen. As an example of morphological analysis, Fig. 10 shows a sample with two different regions. T h e right side of this image shows an unaltered surface, and the left side shows a surface with several alterations. In this case, the sample was heated only in the region on the left, and it is likely t h a t only here the loading and the excitation occurred. T h e corresponding elemental analysis shows many new elements on the metal surface. Figure 11 shows an X-microprobe analysis of the unaltered surface, where only nickel is present. In contrast, the elemental analysis of the altered surface (Fig. 12) is very different from Fig. 11, and there is considerable variation at different points along the sample. Two examples are shown in Figs. 12 and 13. 6. R e m a r k s a n d C o n c l u s i o n This survey shows t h a t very interesting and complex phenomena can arise in N i - H system. On the other hand, these experiments seem to indicate t h a t other, poorly understood parameters must be controlled to obtain similar experimental results. In particular, surface structure and geometry of cells are critical for loading and exciting nickel samples. References 1. S. Focardi, R. Habel, and F. Piantelli, Nuovo Cimento A 107, 163 (1994). 2. S. Focardi, V. Gabbani, V. Montalbano, F. Piantelli, and S. Veronesi, Atti Accad. Fisioc, Serie XV, X V 109 (1996). 3. S. Focardi, V. Gabbani, V. Montalbano, F. Piantelli, and S. Veronesi, Nuovo Cimento A 111, 1233 (1998). 4. L.D. Battaglia, S. Focardi, V. Gabbani, V. Montalbano, F. Piantelli, P.G. Sona, and S. Veronesi, Nuovo Cimento A 112, 921 (1999). 5. S. Focardi, V. Gabbani, V. Montalbano, F. Piantelli, and S. Veronesi, Asti Workshop on Hydrogen/Deuterium loaded metals, in W.J.M.F. Collis (Ed.) Conference Proceedings 64, 35 (1999). 6. S. Focardi, V. Gabbani, V. Montalbano, F. Piantelli, and S. Veronesi, Atti Accad. Fisioc, Serie XV, X V I I I , 109 (1999). 7. E.G. Campari, S. Focardi, V. Gabbani, V. Montalbano, F. Piantelli, E. Porcu, E. Tosti, and S. Veronesi, in F. Scaramuzzi (Ed.) Proceedings of the ICCF8, 70, 69 (2000). 8. E.G. Campari, S. Focardi, V. Gabbani, V. Montalbano, F. Piantelli, and S. Veronesi, in A. Lorussoe, V. Nassisi (Eds.) Proceedings of the Workshop TESMI (Lecce, 2002), p. 35. 9. E.G. Campari, S. Focardi, V. Gabbani, V. Montalbano, F. Piantelli, and S. Veronesi, in Proceedings of the fifth Asti Workshop on Anomalies in Hydrogen\Deuterium Loaded Metals (Asti, 19-21 marzo, 2004), to appear on Condensed Matter Nuclear Physics.
413
10. E.G. in J. 11. E.G. in J.
Campari, S. Focardi, V. Gabbani, V. Montalbano, F. Piantelli, and S. Veronesi, Biberian (Ed.) Proceedings of the ICCFll (2004). Campari, S. Focardi, V. Gabbani, V. Montalbano, F. Piantelli, and S. Veronesi, Biberian (Ed.) Proceedings of the ICCFll (2004).
SURFACE ANALYSIS OF H Y D R O G E N - L O A D E D NICKEL ALLOYS
E. C A M P A R I A N D S. F O C A R D I Dipartimento
di fisica, Universita
di Bologna,
Centro IMO,
Bologna,
Italy
V. G A B B A N I , V. M O N T A L B A N O , F . P I A N T E L L I , A N D S. V E R O N E S I Dipartimento
di fisica, Universita
di Siena,
Centro IMO,
Bologna,
Italy
S. V E R O N E S I INFM,
UdR Siena,
Siena,
Italy
We present a surface analysis of nickel alloy rods loaded with hydrogen. By comparing these with a blank (unused) metal rod, morphological differences and a different composition of the surface are observed. These surface modifications follow a spatial distribution along the rod. These results are compared with a previous analysis of similar samples.
1. Introduction In order to investigate the behavior of a metal loaded with hydrogen, we performed an accurate surface analysis on a nickel alloys sample loaded with hydrogen by mean of a scanning electron microscopy (SEM). Previous experiments with these systems have produced very interesting phenomena such as excess heat production, 1 ' 3 ' 7 alterations of elements on the metal surface,2>7~9 neutron emission,4 and photon emission. 5 ~ 7 In this experiment, a nickel alloy rod was loaded with hydrogen5 and then analyzed. The same analysis was performed on a similar nickel alloy rod that had not been loaded with hydrogen. A comparison of the surface morphology and the elemental distribution shows many differences that seem to outline a spatial distribution of phenomena probably caused by the geometry of the experimental cell. 2. Hydrogen Loading The sample is a cylindrical rod made by a nickel alloy (NiCrFeMn 7.6-20.6-70.41.4) with length 9.0 cm. A chemical and a physical cleaning are performed before of sealing the sample in the experimental cell, showed in Fig. 1 and described in Ref. 3. In the cell, annealing cycles are performed in vacuum and in a hydrogen atmosphere with the temperature in the range 400-700 K. The gas pressure is maintained in the range 100-1000 mbar. The hydrogen loading is described in Ref. 5. 414
415 Cell vessel External SS tube CF35 flanges Heater Ceramic cylinder Sample holder Pt100 temperature sensor Type K thermocouple
(1) (2) (3) (4) (5) (6) Thp, Tce
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3.
3
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The experimental cell for hydrogen loading.
Surface Analysis
The surface of the sample has been analyzed by using an SEM which allows two different type of analysis: morphology and elemental distribution. An electron gun excites atoms in the surface (to a depth of few /xm), secondary electrons (SE) emitted by the atoms and back-scattered electrons (BSE) allow us to obtain images of the surface. Furthermore, an X-microprobe utilizing an energy-dispersive X-ray (EDX) system for elemental analysis, determines the elemental distribution on the surface in a quantitative fashion.
4.
Morphological Analysis
The blank rod shows uniform surface that always presents the same morphology along the cylindrical rod. In Fig. 2, a typical image of the surface is shown at different scales.
(a) Figure 2.
(b)
(c)
Blank rod BSE. (a) Scale 200 (im, (b) scale 50 (im, and (c) scale 10 (im.
416
In contrast, the surface of the used sample shows many differences along the cylindrical rod. For this reason a systematic investigation along the rod has been performed. The surface near to the gas inflow is indistinguishable from the blank rod surface. Moving along the sample, the surface gradually changes up to the other end where the most impressive differences are observed. We have indicated the beginning of the rod where no changes are detected as I = 0.
(a) Figure 3.
(b)
(c)
Sample rod at I = 2.0 cm BSE. (a) Scale 200 /im, (b) scale 50/rai, and (c) scale 10 jim.
In Figs. 3-5, the morphological alterations of the surface are shown. Initially, changes are distributed in isolated zones distributed uniformly. In particular, darker zones appear here and there; new structures similar to broken bubbles arise. The amount of altered surface increases along the rod. Completely altered surfaces are only found at the end of the rod. Only in one case, shown in Fig. 5c, it is still possible to recognize the initial surface in a region in which layers of the surface have been removed.
(b) Figure 4.
(c)
Sample rod at I = 5.0 cm BSE. (a) Scale 200 //m, (b) scale 50 /im, and (c) scale 10 /an.
In the images shown in this paragraph, the dimension of the spot and all other SEM parameters are optimized in order to obtain more details of the surface. 5. Elemental Analysis In order to quantitatively characterize the elemental distribution on the sample surface, all elemental analyses were performed under the same conditions, i.e. with the electron gun at 20 kV, spot dimension 2-6 nm, windows of 200 /zm x 200 /zm,
417
«
(a) Figure 5.
&
•
*
(b)
(c)
Sample rod at I = 8.0 cm BSE. (a) Scale 200 (an, (b) scale 50 /urn, and (c) scale 10 /im.
with an acquisition time of 100 s. In these conditions, a blank rod analysis is shown in Fig. 6. The quantities of Ni, Cr, Fe, and Mn remain the same along the rod, and surface analyses are indistinguishable from one region to another. 6000-,
Fe
Ka
50004000-
o O
Cr,Ka
30002000 O 1000
f;Mn,Ka, f p r K p ; ? FeKP NL
0 [aWif \m*f**"
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1K 'P
5 E(keV) Figure 6.
10
Elemental analysis of the blank rod.
In contrast, the elemental analysis of the sample rod (Fig. 7) are very different from the blank rod analysis, and they are very different from one region to the next along the sample. This is why a systematic investigation along the sample was performed. We obtained the elemental distribution along the rod. To correctly compare the components of the alloy, we note that the changes are essentially on the surface, i.e. at most in the first /im. This fact is confirmed by the elemental analysis performed in the central region showed in Fig. 5c, which is identical to an analysis of the blank. The X-microprobe interacts with atoms in few (im and for this reason we obtain information from atoms on the surface and in the bulk. A simple model2 allows us to separate the contribution to spectra of the element of the surface from the bulk and from other elements on the surface (e.g., O). The most interesting results are shown in Figs. 8-10.
418 4000 Fe„ 3000
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-: :-Fe, ,C feL
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7
8
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E(keV) Figure 7.
Example of elemental analysis of the sample.
In Fig. 10, a quantity of Cu is measured in a narrow zone of the sample. Moreover, in a wide region of the sample, nickel is absent from the surface.
Cr
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Spatial distribution of Cr and Fe in the sample. The measures on Fe show the bar
419
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15-
10o O
*>
040
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—!— /(mm)
Figure 9.
60
80
Spatial distribution of Ni and Mn in the sample.
6. Remarks and Conclusion The surface analysis of the nickel alloy confirm previous results 2,9 obtained using a sample of the same composition in a similar experimental cell. In particular, the observed spatial distribution of the changes in the elements that appear on the surface seems to suggest an important contribution due to the geometry of the experimental cell. This geometry causes a temperature gradient and pressure that -..- Ni -»- Cu
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-••»•
Zn
25 20-
o O
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0
Figure 10.
10
20
30
40
50 60 /(mm)
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80
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Spatial distribution of Ni and Cu on the sample surface.
420
seems to drive the processes on the metal surface. Moreover, these processes are important and produce new elements on t h e surface without massive production of excess heat.
References 1. S. Focardi, R. Habel, and F. Piantelli, Nuovo Cimento A 107, 163 (1994) 2. S. Focardi, V. Gabbani, V. Montalbano, F. Piantelli, and S. Veronesi, Atti Accad. Fisioc., Serie XV, XV 109 (1996). 3. S. Focardi, V Gabbani, V Montalbano, F. Piantelli, and S. Veronesi, Nuovo CimentoA 111, 1233 (1998). 4. Battaglia, L. Daddi, S. Focardi, V. Gabbani, V. Montalbano, F. Piantelli, P.G. Sona, and S. Veronesi, Nuovo Cimento A 112, 921 (1999). 5. S. Focardi, V. Gabbani, V. Montalbano, F. Piantelli, and S. Veronesi, W.J.M.F. Collis (ed.), Asti Workshop on Hydrogen/Deuterium loaded metals, Conference Proceedings, Vol. 64, 1999, p. 35. 6. S. Focardi, V. Gabbani, V. Montalbano, F. Piantelli, and S. Veronesi, Atti Accad. Fisioc., Serie XV, X V I I I 109 (1999). 7. E.G. Campari, S. Focardi, V. Gabbani, V. Montalbano, F. Piantelli, E. Porcu, E. Tosti, and S. Veronesi, in F. Scaramuzzi (ed.), ICCF8, Conference Proceedings, Vol. 70, 2000, p. 69. 8. E.G. Campari, S. Focardi, V. Gabbani, V. Montalbano, F. Piantelli, and S. Veronesi, in A. Lorusso and V. Nassisi (eds.), Proceedings of the Workshop TESMI (Lecce 2002), p. 35. 9. E.G. Campari, S. Focardi, V. Gabbani, V. Montalbano, F. Piantelli, and S. Veronesi, in Proceedings of the 5th Asti Workshop on Anomalies in Hydrogen\Deuterium Loaded Metals, Asti 19-21 marzo 2004, to appear on Condensed Matter Nuclear Physics.
LOW-ENERGY NUCLEAR REACTIONS A N D THE LEPTONIC MONOPOLE
GEORGES LOCHAK Fondation Louis de Broglie, 23, rue Marsoulan, 75012 Paris, France LEONID URUTSKOEV RECOM, Kurchatov Institute, Moscow, Russia
1.
Transformation
Our report surveys the experimental and theoretical studies carried out at the R E C O M since 1998 and the theoretical studies of leptonic monopoles by Georges Lochak (Fondation Louis de Broglie). We will outline briefly all the results to give the overall picture of our research. In 1998, to solve some applied problem, our research group studied the electric explosion of titanium foil in water. By pure accident, in massspectrometric analysis of the titanium powder formed after the electric explosion, we noted a pronounced distortion of the n a t u r a l isotope composition of titanium. T h e principle of the experiment was as follows. Two banks of capacitors with the total energy store W = 50 kJ and the voltage U = 5 kV are discharged simultaneously and independent of each other t o two foil loads over time t ~ 0.1 ms. Of course, during the long period of our studies, we employed different experimental block diagrams, which we cannot describe in detail here. T h e most general experimental diagram is shown in Fig. 1. Figure 1 shows a half of the setup. T h e load is located in the explosion chamber, which is a strong, leak-tight metal container, with an internal structure made of high-density polyethylene. T h e design of the explosion chamber includes facilities for the gas exhaust and bleeding-in, and for taking gas samples into cylinders. T h e electrodes were made of high-purity titanium. As the operating fluid, we used either bi-distilled water with an impurity level of 1 0 - 6 g/1, or solutions of various metal salts in bi-distilled water. T h e key result is as follows. T h e remainder of the titanium foil shows a distorted titanium isotope ratio (Fig. 2). It can be seen from the figure t h a t the situation looks as if 4 8 T i "disappeared" during the instance of the pulse. Please note t h a t the 48 T i isotope was not transformed into another isotope, but instead it disappeared, while other isotopes remained approximately in the same proportion, to within the error of measurements of course. T h e deficiency of 4 8 T i in some experiments is ~ 5 % while the measurement error is ± 0 . 4 % . Simultaneously with disappearance of 4 8 T i , a sharp (10-fold) increase in the impurity content in the samples was detected by 421
422
massspectrometry, X-ray fluorescence analysis, and other methods. The percentage of the new impurities corresponded to the percentage of the lost 4 8 Ti. The chemical composition of the resulting foreign components is shown in Fig. 3. All the components that could be present from the beginning have been subtracted.
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Figure 1. Design of the experimental setup: (1) bank of capacitors; (2) discharger; (3) wire; (4) foil; (5) electrode; (6) polyethylene cover; (7) sealing; (8) blasting chamber; (9) liquid; (10) valves; (11) gas cylinders; (12) stainless-steel shell; (13) pressure gauge.
The author is not going to analyze the experimental results, as this analysis has been published in Ref. 1. Nevertheless, the results were so unexpected that they called for an independent verification. This was done by our colleagues from Dubna (Kuznetsov's group). The verification was thorough, and the results were published in Ref. 2. An important result is that, unlike Fleischmann and Pons, we claim that no neutrons are observed in our experiments within the limitations on a neutron flux of / < 103 per pulse. This is important evidence supporting the assumption that our "magical" nuclear transformations do not involve strong interactions. Another important fact was found both in our experiments and in Kuznetsov's group experiments. Neither of us observed any significant residual 7-activity in the samples. The lack of excited nuclei is important because this allows one to reject all hypothetical accelerative mechanisms for the observed nuclear transformations,
423
because it is impossible to overcome the Coulomb barrier through an acceleration mechanism without exciting the nucleus. Similarly one cannot conquer a fortress by a forward storm without destroying the walls or gates. Nevertheless, the fortress has been conquered, as follows from the experiments. Hence, we should look for evidence that the wall was undermined. The reader may wonder how reliable these results are. Could there be a procedural mistake? The answer is as follows: the data on the isotope shift were obtained independently on three types of mass spectrometers. Hence, it is not a systematic error made on one particular type mass spectrometer. Could this isotope shift result from an error inherent in mass spectrometry, e.g., from a superimposition of lighter masses? Our colleagues from Dubna verified our results on the isotope shift of 48 Ti using gamma-activation analysis. The idea was that nuclear transitions for titanium isotopes differ appreciably from one another and, therefore, they are easily detectable. As noted earlier, they got the same result - a loss of 4 8 Ti. Thus, a procedural error also can be ruled out. We focus on the isotope shift in detail because it proves that low-energy nuclear reactions did, in fact occur. The mere detection of foreign chemical elements in a tightly sealed chamber could be attributed to admixtures of the materials that make up the device. Conversely, an isotope shift from the natural isotope ratio of a chemical element cannot be attributed to admixtures. Indeed, the admixtures must also obey the natural isotope ratio. An occasional isotope redistribution in a sample, first, contradicts the second law of thermodynamics, because it implies a spontaneous decrease in the entropy. Second, the sample is thoroughly stirred prior to mass spectrometry and a random portion is taken every time. Therefore, we would have observed not only a decrease in the 48 Ti content in some samples, but also an increase in this content in other samples. However, this is not the case. Last year, at the colloquium in Paris organized by Fondation Louis de Broglie, a French colleague made a felicitous remark on this topic. He said: it looks as if an isotope revolution was going to overwhelm physics. If this is really the case, please, do not imagine that Russians or Frenchmen are again responsible for a revolution. This is not at all the case; this revolution is obviously international. Let us turn again to the results of measurements shown in Fig. 3. I intentionally did not mark the errors in the chart, as this would complicate understanding. The problem is that the accuracy of measurement is variable for different chemical elements. In some cases, it is 5%; in other cases 10%, and for light elements the error may reach 30%. However, this is not very important at this stage. We can even consider this picture (Fig. 3) semi-quantitative. Another fact is important, namely, one isotope (the parent atom), in particular: 48 Ti is not converted into one or two daughter isotopes of another chemical element or titanium, as would be expected from the views of known nuclear physics. Instead, it decomposes into a spectrum of daughter elements. This fact by itself suggests that we are dealing with a collective process, because one atom cannot decompose into a spectrum of other atoms, if for no other reason because of the substantial difference in the nuclear-binding energy.
424
Nevertheless, some words should be said about the procedures used to determine the composition of daughter chemical elements presented in Fig. 3. Apart from mass spectrometry, X-ray fluorescence analysis and optical spectrometry methods were used for this purpose. All the results are in satisfactory quantitative agreement. I will not dwell on this point, as it has been described in detail in Refs. 1 and 2. Yet another problem, namely, the reproducibility of experiments, is critical for the whole cold nuclear synthesis, and we will consider it here. The scatter of the electrical parameters of our setup (the current and the charge) from one experiment to another is about 15% with the same load. This is a good result. The usual scatter for pulsed plasma devices is about 25%. We achieved a reproducibility of measurable physical parameters, e.g., the isotope distortion of titanium, equal to ±0.56%) and the pressure jump 5P/P, equal to ~1.1%. Thus, the reproducibility of physical parameters is better than that of electrical parameters, and we conclude that our experiments show a rather high reproducibility. However, we must admit that in some cases, the effect of, e.g., isotope distortion increases several-fold for unknown reasons. These experiments are not reproducible, which may be due to some cosmological factor. This only means that our understanding of the lowenergy nuclear transformations is still inadequate. By the way, the charts shown here (Figs. 2 and 3) do not include these "Olympic records." Despite all our reasoning, one can state that an effect actually exists if a parameter has been found whose change induces an enhancement of the effect. In this particular case, the isotope shift. We were able to find such a parameter. If glycerol is added to the bi-distilled water, the titanium 48-isotope shift increases. Figure 4 shows the average 48 Ti isotope shifts for two series of experiments, one carried out in bi-distilled water and the other, in glycerol. It can be seen from the figure that the shift is greater in glycerol. The reason for this is still unclear. A rather interesting question is whether Ti is the only element to possess this remarkable feature. The answer is no. Experiments with other types of foils (Pb, Zr, Ta, and so on) were carried out, and isotope shifts were again detected. For example, the 2 0 8 Pb isotope is the parent atom for Pb. It is noteworthy that the tendency for transformation is usually found for even-even nuclei. Note that this is only an observation rather than a statement. We did not carry out systematic studies with other foils, but we concentrated mainly on Ti. Note that to attain significant effects in these experiments, it is necessary to carefully select the current, the weight of the load, and other parameters for each type of foil. Nevertheless, the data obtained are sufficient to claim that each chemical element is transformed to give its own spectrum of chemical elements. The question of the isotope ratios of the chemical elements formed upon the transformation also cannot be passed over in silence. For the vast majority of chemical elements, we did not notice significant distortions of the isotope composition with respect to the natural distribution. This offers hope that we have not invented or imagined anything but only came across a natural phenomenon.
425
Ti isotope ratio
"A
46
Figure 2.
47
48
49
50
Distorted titanium isotope ratio.
In order to complete the story of transformation, we should consider this problem: where does the transformation take place, either throughout the whole space of the explosion chamber or only in the plasma channel? To answer this question, we carried out experiments with uranium salts (uranyl sulfate, UO2SO4).3 The idea of the experiment was as follows. The plasma channel has a small volume with respect to the volume of the whole chamber. Thus, if some salt of a metal having several isotopes is added to bi-distilled water, the number of admixture atoms from the solution that get to the plasma channel would be small compared to the number of Ti atoms. It is clear that recording of the isotope shift of admixture atoms would indicate that transformation takes place throughout the whole bulk of the chamber. As this metal, we used U. Uranium has two isotopes, 235 U and 238 U, whose ratio can be easily measured even at a low-specific concentration by means of 7, /?, and a-spectrometry. Figure 5 shows the 2 3 5 U/ 2 3 8 U ratios measured by various procedures and compared to the ratio measured in the starting solution. Thus, if no changes were detected after the experiment, this ratio would be equal to unity. It can be seen from the figure that the real ratio is far from unity. The isotope shift effect extends far beyond the possible errors. The shift occurs toward enrichment of the mixture in the 235 U isotope. This does not mean that 238 U is converted into
426 235
U. This interpretation is wrong. We added some 137 Cs isotope as the marker. Then we measured the specific activity (i.e., activity divided by the volume) of each U isotope with respect to the Cs activity before and after the experiment. It was found that the activity of both U isotopes decreased with respect to that of Cs. However, the activity of the 238 U isotope decreases to a greater extent. Thus, the ratio of 235 U to 238 U becomes bigger than unity. Prior to these experiments, we made sure that the specific activity of 137 Cs does not change noticeably. The real situation is more complicated 3 but this is a topic of a separate report. For us, it is important that the transformation can also take place outside the plasma channel. This is a rather "unpleasant surprise," because, probably, within several years, when the low-temperature transmutation will be studied in more detail, it would be rather easy to devise a facile and inexpensive process to enrich uranium. In view of the growth of terrorism all over the world, this outcome seems deplorable. Here is the final remark concerning the experimental study of the transformation with regard to gases. Gases are also chemical elements, and it is likely that they are formed in these experiments. This aspect will be considered in Ref. 4. 2. Phenomenological Model A direct clue to the phenomenological model comes from the proportionality between the 4 8 Ti isotope shift and the percentage of foreign chemical elements observed in the experiment. Thus, a material balance equation is required. We were able to compose the balance equations for the binding energy and baryon, electric, and lepton charges. 5 ' 6 The first step toward the computer simulation of the low-temperature transformations was made by our colleague Doctor Penkov from Dubna. 2 We are also working along this line. Doctor Fillippov will make a detailed report on this topic. 7 We will only briefly mention the main principles that underlie the phenomenological model. We will proceed from the fact that the transformation does take place but we do not understand how the Coulomb barrier is overcome. We consider the assembly of atoms in the initial state and in the transformed state and require that all conservation laws including the energy and the baryon, electric, and lepton charge conservation laws, are fulfilled. By the way, a similar strategy was used by Heisenberg and Born in the early construction of quantum mechanics. As mentioned above, the experiment does not show the presence of radioactivity or neutrons, hence, the transformation does not involve strong interactions. Then let only weak interactions be allowed, i.e., /3-decay and K-capture and the corresponding processes for positrons (3+. It follows from he experiment that no substantial heat evolution is observed during the transformation. This means that we must look for similar binding energies for the initial and final assemblies of atoms. Then we must decide what particular atoms are to be included in the initial assembly. It is clear that this would be atoms of the chemical elements that occur in the explosion chamber, in particular, oxygen, titanium and hydrogen. It only remains now to put a question to the Mendeleev periodic table and to authorize a computer to carry
427
on a long dialog with the table. Doctor Fillipov managed to teach a computer to do this. He will describe his experience in detail. 7 We will cite only one example: 23V + 22Ti + s 8 0 - ^ F e + ? 3 Na + ??C1 + e + o (1 keV). Now, when the answer has been found, the problem looks simple and can be verified using a reference book on the nuclear binding energies. A surprising fact is that with a nuclear binding energy of about lOmeV per nucleon, it is possible to select combinations of atoms that ensure that the total binding energies in the left and right parts of the equation coincide to within approximately A = 100 eV. An even more surprising fact is that these combinations coincide qualitatively with the experimental results. For example, the model including titanium, oxygen, and hydrogen does not give any combinations with elements higher than zinc. This is in line with the results presented in Fig. 3. Moreover, the model predicts that the addition of vanadium should yield the 57 Fe isotope. This result was actually obtained in experiments. We drew the following conclusions from the numerical experiment: (1) Contrary to the opinion of the majority of physicists, the possibility of lowenergy transformation does not contradict the conservation laws. (2) This process is collective in principle and can be simulated within the framework of processes based on weak interactions. (3) Since weak interactions are characterized by small cross-sections, a catalyst is needed. 3. Monopole As a Catalyst? Experimental searches for the monopole started immediately after the transformation phenomenon had been found. In the first experiment, the explosion chamber was insufficiently sealed and the unit did not include a prechamber. Plasma broke through the sealing, and a plasma glow appeared above the unit. 1 Figure 6 shows sample photos of this, made using electron-optical image converters with an exposure time of the order of 10~ 4 s. The time delay between the frames equals 10~ 3 s. The second image is yielded by a mirror mounted above the unit. The lifetime of such a structure was 5 x 10~ 3 s, i.e., it was 50 times longer than the electric pulse duration. This phenomenon is very interesting but it is not the subject of the present report. It should be stressed that radiation traces were registered by nuclear emulsions located at some distance (up to 2 m) from the plasma structure. Typical traces are shown in Fig. 7. The blackening density scale is shown in the figure. The traces are very unusual, and because of that the hypothetical radiation was called a "strange" one. In Fig. 8, a typical track created by an ion in a nuclear emulsion is shown for comparison. One can readily see that the traces we have found are much broader. Moreover, they are not continuous; frequently they are followed by narrower traces, and traces of ^-electrons cannot be seen at all. Such traces (hairs) are always observed when high-energy particles are absorbed. This
428
Figure 3.
The chemical composition of the resulting foreign components.
phenomenon has one more specific feature. Let ft denote a vector perpendicular to the emulsion plane and RQ a radius-vector originating at the center of the unit. The
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Figure 4. C3H8O3.
Average
48
T i isotope shifts for two series of experiments: (1) natural; (2) H2O; (3)
429 'U235~
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-
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Figure 5. The 235TJ/238TJ r a t,; o s measured by various procedures and referred to the same ratio measured in the starting solution: (1) a-spectrometry, (2) 7-spectrometry, and (3) massspectrometry.
traces are observed even in the configuration where n 0 and R0 are collinear. We have experimentally found that the larger is the distance between the detector and the unit center, the narrower is the trace pattern. At a distance equal to about half meter, the track width is about 30 /im, while at a 2-m distance it is only around 5/mi.
Figure 6. Pictures seen on the EOT screens. Exposure time 130 mcs. Time delay between the frames 1 ms.
430
Figure 7.
Typical traces.
To make sure that the traces are not related to some electromagnetic artifact, we installed detectors near the foil remnants only after the explosion. During 24 h, we were registering the traces, which were indistinguishable from those, observed at the instant of electric pulse. Thus, we have confirmed the nuclear origin of the radiation being registered. It should be noted that when the unit was subjected to a magnetic field,1 the traces in the nuclear emulsion changed. This is seen in Fig. 9. Doctor Ivoilov will present in his report some very interesting results for the traces. 8 Here are some conclusions based on the presented experimental data. (1) The particle, which left the trace in the nuclear emulsion is charged, as nuclear emulsions are insensitive to neutrons. (2) The particle cannot have electric charge, as otherwise it could not be able to pass through two meters of atmospheric air and two layers of black paper. (3) The particle does not have high energy, as no delta electrons are observed. (4) The mechanism of the interaction between the particle and the photosensitive layer is not clear. Assuming the Coulomb mechanism, the absorbed energy estimated using the darkening area equals around 1 GeV.
431
I
Figure 8.
I
t
l
i
I
Typical track created by an ion.
500 mkm
Figure 9.
Typical traces when the unit was subjected to a magnetic field.
432
(5) The radiation is of nuclear origin; it interacts with magnetic fields. This calls for a discussion of Lochak's magnetic monopole. Lochak created his theory 20 years before our experiments, 9 " 12 i.e., before those results for understanding and explaining of which we are now attempting to use it. It should be emphasized that this is a good omen for a theory. It is always suspicious when the theories are created specially to explain an experimental observation. They are like the circles drawn on a target after a shoot has been made. Dirac's magnetic monopole theory is well known in physics. 13 In his theory Dirac with a mathematic ingenuity specific to him managed to relate non-integrability of the wave function's phase to the singularity, which emerges when describing the interaction between the electron and the magnetic pole. Paradoxically, the Dirac monopole is not described by the fundamental equation of the quantum electrodynamics, which is named after him. This seems to be the reason why the Dirac monopole is not in the mainstream of the development of theoretical physics. There is one more reason for that which is related to symmetry. Writing the equation for the Lorentz force acting on a magnetic charge:
Fh = g (H - itf x E we can see easily that inasmuch as F^ is a polar vector and the right-hand side of the equation is a pseudo-vector, then g7 the magnetic charge, is to be a pseudo-scalar. This fact is very unusual for physicists. It means that the magnetic charge features a symmetry type other than the electric charge. Pierre Curie was the first to notice this fact. His reasoning was very simple and at the same time very wise. The electric charge is a scalar and it generates a field described by a polar vector E. Inasmuch as the magnetic field vector if is a pseudo-vector, the source, which generates this field (i.e., the magnetic charge) should have the same symmetry, implying that the magnetic charge is a pseudo-scalar. Based on this Lochak argues: "There is no real symmetry between electricity and magnetism but there are two slopes of the same
Ax Figure 10.
Mossbauer spectrum.
433
pinnacle: a vector slope and a pseudo-vector one." In mathematical terms, the Dirac equation is invariant to two and only two gauge transformations. Indeed, the Dirac equation for a relativistic charged particle with spin S = 1/2 in an external field can be written in the following form: (1)
( 7 M V , + ^ ) ^ = 0,
where 7M are 4 x 4 Dirac matrices, and ip is a bi-spinor. Then, if we subject the bi-spinor to the following transformation: ip —> ij)i = exp (i-r-Iip) ip, where I is the unit matrix and the operators have the following form:
then Eq. (1) transforms into the well-known equation for the electron: 7 , ( ^ - ^ ) ^ + ^
= 0.
(2)
Now, if we use Dirac equation (1) without the mass term, i.e., actually the equation describing the neutrino 7MVMtf> = 0,
(3)
and represents the gauge invariance using a pseudo-scalar matrix '01 75 = 7i 72 73 74
,
I 0
where I is the 2 x 2 unit matrix, and transform the bi-spinor as follows: ip -> V' = exp ( i ^ 7 5 x ) V>, then the operator will have the form: VM = d„ - ^ 7 s B M , and the local gauge will have the following form: B M -> B M +
id^
Note that because of the pseudo-scalar matrix 75 the field B is a pseudo-potential and x i s a pseudo-phase. However, the pseudo-scalar feature of magnetism is expressed using the charge operator G = g • 75, where g is a usual scalar. The Lochak equation for the magnetic charge has the form: 7M ( ^ - ^ T s B M ) V = 0.
(4)
The phase gauge using 75 was known before Lochak's works, but he managed to find the physical sense in Eq. (4): it is the equation describing the magnetic monopole with zero mass. Thus, in Lochak's theory the magnetic monopole is a kind of
434
the magnetically excited neutrino. Do not forget that it is described by the same equation as the neutrino. No doubt, Lochak's theory is not complete yet and needs further development. Professor Harald Stumpf has worked actively for several years to apply it to solve the exact physical problems and to integrate it into the Standard Model. 14
a
Figure 11.
b
System in stable (a) and unstable (b) position of equilibrium.
One might ask: If Lochak's theory is correct, why has it garnered so little interest for 20 years? The answer is obvious. French physicists are deeply convinced that all genuine physical theories can only be developed outside France. Other physicists usually do not read scientific publications in French. Because of that Lochak's works are not known to academics. A more profound reason is that the Standard Model does not need the leptonic magnetic monopole. Today's physics are dominated by the dictatorship of democracy. Let us explain that using a simple example. About 5 years ago a CERN paper was published which had around 600 authors. The list of authors was longer than the article itself. As to the authors of the present report, we believe that a new idea may come to one head or at most two heads, but in no way to 600 heads at the same time. Bearing in mind that theorists and experimentalists tend to consider the Standard Model impeccable (something like a holy icon), you will understand the attitude to Lochak's theory. After this brief digression we should return to the main subject and draw some conclusions, which are much needed by an experimentalist. According to Lochak, 11 the magnetic monopole is a fermion. Moreover, it features chiral symmetry; under a spatial reflection the charge seems to change its sign. In reality the charge operator G passes from one of its own meanings (e.g., corresponding to the left monopole) to another one (right monopole). 12 This is very unusual for experimentalists who are accustomed to deal with electric charges which do not allow themselves such a behavior. According to the classification adopted in the elementary particle physics, the monopole is a lepton and, hence, it participates in weak interactions. Because its rest mass is zero, not much energy is needed to create a monopole-antimonopole pair. On the other hand, for this reason it is difficult to detect. Naturally one can ask: if everything is so easy, why hasn't the monopole been detected earlier? We believe that first it is necessary to find the monopole to make sure it exists, and only after that, will it be possible to answer
435
this question. Our experimental search for the monopole started with an attempt to capture it in a ferromagnetic trap. Foil made of 5 r Fe was used in the trap. The idea was that capture of the monopole by the ferromagnetic will change the field on the 57 Fe nucleus. This in turn will affect the width of Mossbauer spectrum lines. Let (Fig. 10a) be the line width before irradiation. We would expect to see (b), and have instead observed (c). This means that the Mossbauer spectrum of 57 Fe (containing six lines) has not broadened but has only shifted by the same value equal to AH = 500 ± 70 Gs. This means that we observe some collective effect. Doctor Ivoilov will discuss this subject in detail in his report. 15 Another feature of the magnetic monopole, which follows from Lochak's theory, is that it has a leptonic origin. Because of this, one can hope that the presence of the magnetic monopole affects the /3-decay. Based on this, in the experiments with uranium salts we measured very accurately the /3-decay periods of daughter isotopes in the uranium and thorium series. In the experiment, we have found that thorium secular equilibrium and, hence, the probability of the /J-decay of the protactinium isomer is strongly changed. Prof. Rukhadze will tell about our observations in his report. 16 The Lochak magnetic 'neutrino' has zero rest mass and, hence, it cannot exert any energetic effects on an atomic system. However, if a system rich in energy is in a non-equilibrium state and a chain reaction develops in it, the situation changes. This is shown in Fig. 11. In case (a) a small perturbation will only result in small oscillations. Theorists believe this is due to zero oscillations of vacuum. It is obvious that in case (b) the result will be quite different. A nuclear reactor is a good example of such system. Henri Rukhadze will describe in detail how catastrophic will be the consequences of even insignificant changes in the /3-decay periods of nuclei.16 Ammonium nitrate is another example of a system rich in energy.17 Henri Lehn, our French colleague, will describe results of our joint experiments, held in our experimental unit, in which we observed interaction between magnetic charges and ammonium nitrate. For understandable reasons the issues related to the interaction between the magnetic radiation and biological objects are of no small importance for us, because a human body is, to large extent, an electromagnetic system. Chelyabinsk biophysicists conducted some pilot experiments, in which laboratory animals were irradiated in our experimental unit. Doctor Pryakhin will describe the results of these experiments. 18 I will only mention that we have observed that the number of stem cells in the animals' marrow changes. 4. Conclusions To summarize, we seem to have found a new type of interaction. It has magnetic nature and catalyzes nuclear processes by initiating weak interactions. In our opinion, a new type of activity has been found (g- or m-activity). It should be stressed that last statements are nothing but hypotheses though, in our opinion, they are
436
not unsubstantiated. I would like to state on b o t h Lochak's should the aforementioned hypothesis prove to be wrong, responsibility. If the result is positive, it will undoubtedly the entire French and Russian team. Even if the statements effort will be needed to check their correctness.
p a r t and my own t h a t we will bear scientific be an achievement of are not wrong, a lot of
T h e results presented in this talk were obtained by a large t e a m of specialists and technical staff. It is my pleasure to list the t e a m members: (1) "RECOM" specialists: Dr. Dmitry Filippov, Dr. Vladimir Liksonov, Dr. Valery Kuznetsov, Dp.Ing. Alexander Govorun, Dp.Ing. Anatoly Volkovich, Dp.Ing. Sergei Smirnov, Dp.Ing. Victor Korolev, Dp.Ing. Alexander Guliaev, Dp.Ing. Chermen Kaitukov, Dp.Ing. Victor Kalensky, Dp.Ing. Sergei Petrushko. (2) "RECOM" technical staff. Vladimir Shevchenko, Pavel Strashko, Dp.Ing. Tatiana Sokolova, Nikolai Zubkov, Alexander Gaverdovsky, Vladimir Bajushkin, Evgeny Sergeev, Vladimir Petrushko. (3) National Research Center "Kurchatov Institute": P r . p h . Vladlen Tsinoev, Dp.In. Sergei Zukov, Dr. Rosa Rjabova, Dr. J u r y Dontsov, Dp.Ing. Boris Novoselov, Dr. Leonid Elesin, Dp.Ing Vladimir Dorovskoi, Dr. Sviatoslav Demkin, Dp.Ing. Vladimir Stolyarov. (4) Institute of Inorganic Chemistry: Dr. Alexander Steblevsky. (5) Central Research Institute for Chemical Machine Building: Dr. Pavel Stolyarov. (6) Institute of General Physics: Professor Anri Rukhadze. (7) Kazan State University: Dr. Nikolai Ivoilov. (8) Chelyabinsk State University: Dr. Evgeny Pryakhin. (9) Institute of Chemical Physics: Dr. Vladimir Fedotov. Many observations have not been included in this report because of lack of space.
References 1. L.I. Urutskoev, V.I. Liksonov, and V.G. Tsinoev, Observation of transformation of chemical elements during an electric discharge, Ann. Fond. L. de Broglie 27, 701 (2002). 2. V.D. Kunznetsov, G.V. Mishinsky, F.M. Penkov, V.I. Arbuzov, and V.I. Zhemenik, Low energy transmutation of atomic nuclei of chemical elements, Ann Fond. L. de Broglie 28 (2), 173-213 (2003). 3. A.G. Volkovich, A.P. Govorun, A.A. Gulyaev, S.V. Zhukov, V.L. Kuznetsov, A.A. Rukhadze, A.V. Steblevskii, and L.I. Urutskoev, Experimental observation of the distortion of the uranium isotopic relationship and violation of the thorium-234 secular equilibrium upon electric explosion, Bull. Lebedev Phys. Inst. 8 (2002). 4. V.M. Dorovskoi, L.A. Elesin, D.V. Filippov, A.V. Steblevskii, V.L. Stolyarov, and L.I. Urutskoev, Electron microscopy study of the transformation products, Ann Fond L. de Broglie (to be published). 5. A.A. Rukhadze, L.I. Urutskoev, and D.V. Filippov, On the possibility of low-energy
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6.
7. 8. 9. 10. 11.
12. 13. 14. 15.
16.
17. 18.
nuclear reactions from the viewpoint of conservation laws, Bull. Lebedev Phys. Inst. 4 (2004). L.I. Urutskoev and D.V. Filippov, On the possibility of low-energy nuclear reactions in low energy plasma from the viewpoint of conservation laws (NIZ GTP Erzion, Moscow, 2003), pp. 84-97. D.V. Filippov, A.A. Rukhadze, and L.I. Urutskoev, Effects of atomic electrons on nuclear stability and radioactive decay, Report, ICCF 11, Marseille 2004. N.G. Ivoilov, Low energy generation of the "strange" radiation, Report, ICCF 11, Marseille 2004. G. Lochak, Ann Fond. L. de Broglie 8, 345 (1983); 9, 5 (1984). G. Lochak, Wave equation for a magnetic monopole, Int. J. Theor. Phys. 24, 1019 (1985). G. Lochak, The symmetry between electricity and magnetism and the problem of the existence of magnetic monopoles, in T.W. Barrett and D.M. Grimes (Eds.), Advanced Electromagnetism (World Scientific, Singapore, 1995), pp. 105-148. G. Lochak, Leptonic monopole and weak interactions, Report, ICCF 11, Marseille 2004. P.A.M. Dirac, Proc. R. Soc. A133, 60 (1931); P.A.M. Dirac, Phys. Rev. 74, 817 (1948). H. Stumpf, Simultaneous formation of electric and magnetic photon states by electroweak symmetry breaking, Z. Naturforsch. 59a, 185-195 (2004). N.G. Ivoilov and L.I. Urutskoev, The influence of "strange" radiation on Mossbauer spectrum of Fe in metallic foils, Prikladnaya Fizika (Appl. Phys.; in Russian) 5, 20 (2004). A.A. Rukhadze, L.I. Urutskoev, and D.V. Filippov, On the possible magnetic mechanism of shortening the runaway of RBMK-1000 reactor at chernobyl nuclear power plant, Bull. Lebedev Phys. Inst. 1 (2004). H. Lehn, Report, ICCF 11, Marseille 2004. E.A. Pryakhin, L.I. Urutskoyev, G.A. Tryapitsina, and A.V. Akleyev, Assesment of the biological effects of "strange" radiation, Report, ICCF 11, Marseille 2004.
RESULTS OF ANALYSIS OF Ti FOIL A F T E R GLOW D I S C H A R G E WITH DEUTERIUM
I. B . SAVVATIMOVA A N D D. V. G A V R I T E N K O V FSUI SRI SFA
"Lutch"
In this study, we report on the surface structure, distribution, and isotopic composition of elements found on Ti cathodes before and after glow discharge in plasma, during which excess heat was produced. Irradiation was carried out with deuterium ions with a discharge voltage below 1000 V, with a current of 10-20 mA. The analysis of the surface structure and of elemental composition of the Ti sample was carried out with a scanning electron microscope with Energy Dispersive X-ray Spectroscopy (EDS), which can detect impurities at concentrations as low as 0.2at.%. New metallic phase formation and newly present elements were revealed by the EDS method in several different, separate active spots on the cathode surface, with concentrations ranging from 0.3 up to 10 or 20% or more. Al, Mg, Br, and Sr were found at ~ 0 . 3 % , Rb ~o.4%, S ~1.0%, F ~10%, O >20%, Ni - 0 . 3 20%, Cr ~1.4%, Fe ~4.0%, and Sn ~0.4-5.0% were detected by this method after the experiment and were not in the as-received sample before the experiment. The basic changes are observed in places of microexplosions, micromeltings, and structural inhomogeneities. Investigation of the isotopic composition was carried out by Thermal Ionization Mass Spectroscopy (TIMS). Additional elements in a thin surface layer were found by this method when analysis was performed at 1900°C. The Ti cathode produced excess heat during glow discharge, estimated at 10-20% above input power. This suggests that the heat was caused by the formation of the observed new elements. It is necessary to note that excess heat was created by the processes in a sample having weight of 0.7 g in a device weighing 5 kg. At the same time thermal losses with the water-cooling of anode, losses through a quartz wall of the discharge chamber and the losses in metal flanges were not taken into account. In the experiments with other cathode materials (including Mo, W, and Zr) under the same experimental conditions, no excess heat was observed and thermal losses were roughly 40%.
1. Introduction Results from research with Pd cathodes irradiated by deuterium ions in glow discharge were published in the previous papers. 1 ~ 12 We observed the weak gamma radiation, 2 short-lived neutron bursts, 1 _ 3 changes in surface structure, and in the elemental and isotopic composition of Pd cathode (with purity 99.99 and 99.9%)4~8 under deuterium ion irradiation. After irradiation, autoradiographs (X-ray film placed in contact with the samples) showed blackened areas. Not only were the autoradiographs placed in contact with irradiated Pd samples blackened, but also up to 7 Pd, Ti, and Ag foils that were not directly irradiated, but which were located under an irradiated sample were blackened. In Pd samples, elements other than Pd increased by factors of 100-10,000.6~8 Energy Dispersive X-ray Spectroscopy 438
439
(EDS) detected impurity elements in amounts ranging from 0.5 to 5%, which were not detected in the starting materials. 5 ~ 8 In accordance with the radiography analysis results the presence of the radioactive isotopes with various energies of emission on the Pd the cathode after glow discharge experiments had shown both highenergy and low-energy components. 5 The observed effects can be explained by a fusion-fission reaction on the cathode. That is, by an interaction of palladium with deuterium, and by the subsequent decay into more light elements. The majority of the elements which are detected by this method after irradiation, and which were not present before irradiation, were distributed on the boundaries of the grains and subgrains 2 ' 4,5 and in local zones. The content of additional elements in such places was from about a tenth of a percent up to several percent. The content of the separate impurity elements in initial samples did not exceed 10 _ 3 -10~ 4 at.% and that amount could not be detected by the microanalysis method. Groups of elements such as Sc, Ti, V; Ag, Cd, In; P, CI, Br, Ge, As, Kr, Sr, Y, Ru, and Xe were found out in Pd after an irradiation by ions of several different types (D, H, Ar, and Ar + Xe), with varying amounts of the elements detected. 9 The integral sum of all impurity elements in Pd samples after irradiation by D, H, and Ar ions was estimated in the ratio 10:(2-3):1, accordingly. Elements with charge number Z = 26-31 (Fe, Cu, Zn, and Ga) were observed by the MPA method after preferential irradiation by deuterium ions. The EDS and radiography results both indicate that nuclear transmutations occur intensively mainly on localized sites (hot spots). 5 ' 6 ' 8 Different combinations of impurity elements found in different zones on the same samples were observed in the various characteristic spectrums for the same kind of ion. 7 ' 8 The considerable changes of the isotope ratio 1 0 B / n B , 1 2 C/ 1 3 C, 6 0 Ni/ 6 1 Ni/ 6 2 Ni, 40 Ca/ 4 4 Ca, and 9 0 Zr/ 9 1 Zr were observed and were published in Ref. 6. The change of the isotope ratio for 1 0 9 Ag/ 1 0 7 Ag from 1:1 in the initial unused Pd up to 3:1 and in some cases 9:1. This was described in Refs. 7-9. In this paper, the changes of elemental and isotopic composition in the Ti sample with excess heat during deuterium ion irradiation in a glow discharge plasma is described in greater detail. 2. E x p e r i m e n t a l M e t h o d The experimental procedure is described in detail in previous papers. 2 ' 5,6 A Ti (99.93 purity) cathode was irradiated with deuterium ions in a glow discharge, and then later examined. The density of the ion current was 10-20 mA/cm 2 . The voltage of glow discharge was 300-850 V. The measurement system recorded current, the voltage of the discharge, gas pressure, the velocity of the gas stream, and the flow rate of the cathode cooling water. The temperature at the inlet and outlet of cooling water for both the cathode and the anode was recorded. The program used the inlet and outlet temperatures, flow rate, and input power to compute instantaneous input and output power, and any excess power. The program also keeps track of net input and output energy, and excess energy when present.
440
The studies on the change of structure and elemental composition in the Ti cathode were carried out with using the scanning electronic microscope (JEOL, model JSM 6460-LV) and EDS (Oxford Instrument, INC A). The quantitative analysis of the elemental content was performed using INCA software, Version 4.02. Acquisition time per location was ~2min. The SEM accelerating voltage was 25keV. The area of spot analysis was 1 /xm2 at the site being analyzed; scanned areas were ~25/im x 25 pm. The elements O, F, S, Na, Mg, Al, Ti, Cr, and Fe were determined by EDS on their K-a lines; Mo, Br using their L-a lines; and W using its M-a line. The unused sample and a sample subjected to glow discharge in deuterium were analyzed in detail. Places with structural defects (such as flaws, tracks, and projections); zones of such new formations such as blisters, craters, and micromelted spots, needle structures, and typically "pure" sites of a surface without special changes were explored. Forty-seven sites were analyzed inside new formations and on "pure" sites of the surface of Ti foil after irradiation of deuterium ions and on ten sites on the surface of initial Ti. The most typical places of analyses and the content of additional elements in them with amounts more than 3a are given on the appropriate illustrations and are accompanied by tables. The thickness of Ti foil was 0.05 mm; the titanium purity was 99.93%. Table 1 shows the impurities in the starting material, from the manufacturer's certified data taken by X-ray diffraction. 3. Results Table 1. Impurities in the Ti foil starting material. Element ~M Fe Ca Mn V S Ti
Content (ppm) 30 20 10 8 2 70
Atomic (%) 3 x 10~ 3 2 x 10"3 1 x 10"3 8 x 10"4 2 x 10~ 4 7 x 10"3 99.93
Samples after glow discharge experiments usually have the largest changes in structure and chemical element composition on the boundary between the irradiated and screened zones. Figure 1 shows a series of three places: tracks of microexplosions on the boundary of the irradiated and unirradiated areas. A typical example of these places is shown in Figs. 2 and 3 in more detail. There appear to be pair formations of the greater and smaller sizes located ~100/im apart. All these formations, along
441
with the microcraters, were carefully analyzed for chemical element composition. The composition of groups of the impurity elements in every formation is shown in Tables 1-6. The backside of the cathode has also been analyzed, but it did not reveal any changes from the original, as-received impurities. The same can be said for sites that were screened from ion irradiation. 4
Irradiated area Boundary
CD
m
Under screen
Figure 1. Surface of Ti foil on the boundary of the irradiated and unirradiated zones (the irradiated area is darker gray).
As can be seen here, the combination of elements found in different spots that were analyzed in a ~ 1 fim3 sample may vary, but usually some elements are found in common. For example, the row of selected spots contained such impurities as O, F, Al, Fe, and Mg. The increased size of the formation from zone 3, Fig. 1, which can be characterized as a microexplosion zone or a zone of local melting, is shown in Figs. 2 and 3. The analysis results of the area 50/xm x 50 /xm (2.5 x 10~ 3 mm 2 ) are placed in column 6. The composition of chemical elements in every area that was analyzed is shown in Table 2. Columns 1-6 of Table 2 are the results of the elemental analysis that were carried out for a series of new formations on the boundary between the irradiated titanium and Mo screen, which are shown in Fig. 1 and magnified in Figs. 2 and 3.
442
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(a) Close-up of the area shown in Fig. 1. (b) Enlarged Zone one shown in Fig. 2a.
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The locally melted zone near Ti-Mo screen boundary.
443
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Figure 4. Points of analysis on the moving path of the magnet pinch of high density (pinch effect or micro arc).
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Table 2.
Results of the chemical elemental analyses by EDS method in 23 selected sites. Sites
Elements
o
Al F Fe Na S Ni Mg Rb Cr Sn Br Si Sr Hf Co Ca Mn V Ti Mo
23.41±0.92 0.43± 0.09 5.59±0.65 0.52±0.10
18.59±1.5 6.63±0.83 0.89±0.08 1.89±0.2 0.25±0.08
26.9±1.2 0.24±0.1 6.72±1.0
22.0±1.0 0.25±0.1 8.6±1.0
8.11±0.6
1.08±0.1
0.39±013 1.08±0.1
0.27±0.07
0.26±0.11
0.24±0.1
0.47±0.1
53.61±0.8 0.37±0.08 6.79±0.7 0.17±0.04
30.22 ± 2 0.16±0.07 15.8±1.1
37.4±1.0 0.32±0.1 16.9±1.3
0.41±0.2
0.47±0.15
50.91±1.0
41.67±1.0
10
11
20.87±1 0.54±0.1 5.04±1.0
17±1.0 0.6±0.1 7.7±1.0
62.25±1 9.3 ±0.5
54.8±1 19.9±1
0.36±0.1 0.28±0.09 0.39±0.08
59.49± 1 9.85± 0.5
62.3± 1.1
62.46±1.2
97.36±0.4
67.7±1.2 0.13±0.5
90.78±0.7
33.47±0.7 1.21± 0.1
Table 2.
Sites
Elements 12 O Al F Fe Na S Ni Mg Rb Cr Sn Br Si Sr Hf Co Ti Mo
Continued.
13
14
15
16
17
18
19
20
21
18.1±0.4
45.0±1.0
25.42 ± 2
63.14±0.8
68.8±1.0
60.1±1
16.0±0.3
2.99±0.68 0.19±0.05 0.61±0.12
22
23 0.4±0.2
6.46±0.43
14.23±0.6
21.43±0.9
47.17±0.5
6.46±0.43
2.1±0.3 0.67±0.14
1.3±0.3
0.37±0.05
0.67±0.2 2.42±0.34 4.9±0.2 1.53±0.1
0.4±0.2
2.95±0.14 0.3±0.2
83.3± 0.7 9.85± 0.5
4.76±0.3
1.43±0.2
±1.1
88.5±1.2
2.57±0.4 97.36±0.4
6.06±0.28 67.7±1.2 0.13±0.5
50.41±0.7 0.43±0.1
44.13±1.13
2.57±0.4 31.26±0.7 3.41±0.2
20.35±0.6 7.75±0.6
1. The elements that appeared as a result after sputtering of the previous samples were not included in the tables. 2. Mo comes from sputtering of the screen that holds the sample.
32.9±1
54.8±1 19.9±1
98.0±0.6
\
Figure 6.
Track not the boundary with structure of grains or defects in initial structure.
The combination of the main impurity elements in the examined zones is variable. Most of the analyzed areas in this series contained F: F was found in all seven areas; Al in six areas; O in four areas; Na in two, and S, Br, and Mg were found in only one area. The content and combinations of impurity elements is quantitatively reproducible when the areas analyzed are situated in the new formations, e.g., in Fig. 2, zone 1. Similar elements and combinations of elements were found in Fig. 4, areas 1-3, and in Fig. 5, areas 1-3. In Table 2, the elements under columns 10 and 11, Na, Si, and Al, were found in areas 1-4. Some tracks, which appeared after the experiment and were not bound with the grain structure of the Ti were also analyzed. Areas with small amounts of Na, Mg, Al and Si, and Cr, Fe with content >3cr were revealed in points of zone 1 in Fig. 8.
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Figure 7.
The detailed site of a track in Fig. 6
447
Figure 8.
Track with new formation on the end.
The typical element composition in the field of a track Fig. 8 is given in column 12. Most of the additional elements were found in such structural defects, as zones of microexplosions, in the places of a new phase formation, of tracks (Fig. 9) and of destroyed surface structure. The tracks usually were observed near places were new phase formations occurred (Fig. 10). As shown in Figs. 7-9, these formations were sometimes convex and sometimes concave. The tracks were not bound with the grain boundaries on Ti surface. The tracks may be caused by a unipolar arc in the glow discharge moving along structural flaws, and being a consequence of overvoltages in the areas
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of microflaws, oxide films and phase inclusions.13 Formation of pair defects of the greater and smaller sizes (Figs. 12 and 15) was typical, as noted earlier (Figs. 1-3). No impurity elements were found on the undisturbed areas of the Ti surface. For example, the impurity elements were not found in Fig. 12, areas 1 and 2. The combination of Fe, Ni, Co does not correspond to any possible penetration of these elements from the stainless steel water-cooled sample holder. The Rb and Hf are not present in any of the cell components. The Sn also could not get onto the cathode from the surrounding medium. The Na and Si in small amounts were found in the defect zone (Fig. 17).
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Impurity elements were found in 23 cases from 47 areas on the analyzed surface of Ti in regions that had been irradiated (Table 2). The amount of Al and Fe (Table 3) detected increased by factors of 100-1000. The comparison of the average amount of main impurity elements in an initial material and after experiment was made. The basic impurity elements with the concentrations exceeding an error of measuring more 3er were placed in Table 3, column 3. Column 2 shows the number of points at which each element was observed. The elements present before the experiment are shown in column 4. As shown in Table 3, Cr, Sn, and Rb were revealed in two spots on the cathode, Na in four spots, Fe, Al in six, and O in 12 spots. The results at the analysis of Ti as received measured by Thermal Ionization Mass Spectroscopy (TIMS) is tabulated in Table 4. • Sr-87 is equal in mass to Rb-87 (85, 87), and a lot of it was found in the tungsten cathode, • a decrease in Fe-56 by factors of up to 100 was observed. Fe-57 had a slight change in quantity compared to the initial sample. But: • mass 55 increased strongly (by a factor of 40), • mass 55 is Mn or Fe-55 (electron capture), • Mn was not found by the EDX method. Fe was found by the EDX method to be 4 ± 0.2%. This is a very interesting change, and it may be highly significant! It may indicate the mechanism for Fe-56 to Fe-55 transformation, • the Ca-40 isotope was found in large quantities during the analysis of the initial sample and after the experiment. This is the reason it was excluded from Table 4. We observed Al, Ca, Sr, Ba, Nd, Ga, Pb, and small amounts of additional
450 Table 3. by EDS.
Main impurity elements in Ti after experiments in deuterium glow discharge detected
Elements
Number of spots on the cathode, where this element was found"
The amount of the element after the experiment (at.'Jo'')
1 O Al F Fe Na S Ni Mg Rb Cr Sn Br Si Sr Hf Co Ca Mn V Ti
2 12 9 6 6 4 3 2 2 2 2 2 1 1 1 1 1
3 27±1.2 0.33±0.1 10±0.56 4.05±0.2 0.70±0.3 1.08±0.13 10.8±0.36 0.26±0.15 0.44±0.12 1.39±0.21 2.7±0.14 0.28±0.1 0.39±0.09 0.33±0.25 4.76±0.09 2.57±0.3
The amount of the element before the experiment (at.%)
3 x 10"3
2 x to-3
1 x 10"3 8 x 10"4 2 x 10~ 4 99.93
"Number of spots on the cathode surfaces with the element measured at 3
Elements
Na, cps, 1900° C (after experiment)
N a h, cps, 1950°C (after experiment)
JVb, cps, 1900° C (before experiment)
A = N&-Nh cps, 1900° C
1 27 84, 86, 88 42, 43, 44 130,132,134,135, 136, 137, 138 142, 143, 144, 145, 146, 148, 150 155, 156, 157, 158 206, 207, 208
2 Al Sr Ca Ba
3 100,000 2,070 51,000 50,620
4
5 10,000 150 470 790
6
Nd
435
1950
30 Gd
1,500
Pb
510 211,240
£
85
48,670
60 11,930
Abbreviations: Na: the count per second for analysis temperature 1900°C after experiment; JVj,: the count per second for analysis temperature 1950°C after experiment; N^: the count per second for analysis temperature 1900°C before experiment; A = N^-N-^: is the difference of cps after and before experiment for analysis temperature 1900°C.
451
4
3
2
Figure 13.
Track with inset.
elements in the thin surface layers of the Ti. The amount of the impurity elements in the thin surface layer (~100-150A) observed by TIMS is considerably greater than the amounts measured by EDX. The total amount in counts per second was ~2 x 105 cps. Elements such as Al and Sr were also observed by the EDX method ~ 1 /Jin below the surface. Presumably the most of the transmutation reaction takes place in the thin surface layer under low energy glow discharge. It must be noted that that we study the local spots on the cathode by EDX, and integral content on the surface of the cathode in small volumes (1.5 ±0.5 mm x 20 mm x 100 ^m) by TIMS. Moreover the TIMS method can resolve in Angstrom
Figure 14.
Local inclusion with the O, Fe, Co, and Ni.
452
Figure 15.
The local melting with Na and Si only.
units near the surface, especially for heavy elements. The biggest changes in elemental composition were always observed near the boundary of irradiated and unirradiated areas. This was one reason why various methods of spectroscopy yield different levels of some elements. The cathode of the TIMS mass spectrometer itself was made from Re (masses 85 and 87), so we did not try to measure Sr-87. 4. Heat Effect Diagrams illustrating the excess heat effect in a Ti sample in a quartz cell with cooling cathode and anode are shown in Fig. 18. The heat efficiency (COPE) presented in Fig. 18 ranged from 10 up to 30%
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Figure 16.
Porous formation.
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Figure 17.
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1000 1500 2000 2500 3000 3500 4000 4500 5000 5500 6000 6500 7000 7500 8000 8500 9000
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Figure 18. (a) T i n , T o u t is the temperature of input cooling water in cathode and of output cooling water from cathode (°C). (b) P i n , P o u t is the input energy and output energy from the watercooling system (in watts), (c) C O P E = (P o u t-Pin)/Pin (an approximate measure of efficiency). For (a) and (b) out is upper curve (red) and in is under curve (black).
454
within 2.5 h, and excess energy output in these conditions was ~ 1 W , with 5W of input power. It should be noted that the excess heat effect was observed in the Ti sample with 0.7 g weight and that the weight of the working chamber was 5 kg. The excess heat was determined without taking into account the losses in anode cooling by flowing water, and without taking into account heat losses due to the heat transfer through the 785 cm 2 area quartz tube wall of the working chamber, or the heat losses through metal flanges of the working chamber. . The excess heat effects were observed repeatedly even after the equipment was turned on and off several times. Typical process in the same glow discharge parameters with other cathode materials showed the negative amount Px= (P0ut~-Pin) ~ 1 W and COPE = (Pout-Pm)/P\n (0.2-0.5). This indicates that the losses for Zr and Mo were ~20-50%.
5. Discussion Many areas on the irradiated surface of the Ti sample that were analyzed contained only titanium. Outside of the unusual new structures found on the surface, impurity elements were not detected at the limits of sensitivity of the equipment. Excess content of the impurity elements on the irradiated titanium surface were found in 20 cases from 47 analyzed places. The amount of the impurity elements in the comparison with an initial material was more from 10 up to 1000 times, and from a few tenths of a percent up to several percent. The total content of the impurity elements in an initial sample did not exceed 7 x 10~ 3 at.%. The redistribution of the elements is insignificant. Some chemical elements found on the sample surface might be the result of cathode sputtering and of sprayed metal precipitation from the cell components, cathode holder, and cathode screen, such as, e.g., Mo from the screen. However, it should be noted that: • the Mo screen was carefully cleaned before each experiment by chemical etching and washing, • most elements given in the table were absent from all of the cell components, • tracks of Al and Fe in 2 x 10~ 3 to 3 x 10~ 3 at.% certificated in Ti were not found by EDS in the unused samples of Ti, • there were no sites with a similar chemical composition and concentration of the impurity elements on the back of the sample, or under the area screened from glow discharge. Let us assume there was a redistribution or migration of these chemical elements (Al and Fe) in samples under ion bombardment in glow discharge plasma, and also that the element segregation by diffusion is possible. We might also assume that Fe, Cr, Ni in areas where microexplosions occurred could be a result of transmission of these chemical elements from the stainless steel substrate of the heat sink through
455
the foil during the formation of microarcs. However, the EDS analysis did not reveal such segregations on the back of the Ti sample. T h e existence of Hf, Rb, and Sn in new formations is difficult to explain. Some chemical elements could be a result of fusion reactions and second-order decay under excitation of microplasma discharges on the surface of defects (including unevenness, oxide films or inclusions). T h e presence of local sites in the blackening on X-ray films (hot points) took place in contact to samples of the titanium, silver and palladium after deuterium irradiation early. It is shown in Refs. 5 and 7. On the basis of the law of conservation of energy and the exothermic reaction it is was possible t o assume the following reactions: 48 + 4 !D 2 ^ 2 0 C a 4 4 + 6 C 1 2 + 3 5 . 5 M e V , 22TI 48 + 2 XD 2 ^ 1 6 S 3 2 + 8 0 1 8 + 4 M e V , 22TI 48 + 6 C 1 2 ^ 2 7 C o 5 9 + p + 6.45 MeV, 22Ti 48 + 6].D 2 - ^ 2 7 C o 5 9 + p + 85 MeV, 22Ti 46 222Ti ^16S32+28Ni60+2.239MeV, 47 2 2 2 T i ^ i 6 S 3 2 + 2 8 N i 6 2 + 2.798 MeV, 222Ti48 ^ i 6 S 3 2 + 2 8 N i 6 4 +3.863MeV, 2 2 2 T i 4 6 ^ 2 6 F e 5 6 + 1 6 S 3 4 +2.289 MeV, 2 2 2 T i 4 8 + 6 C 1 2 ^ 2 6 F e 5 6 + 2 4 C r 5 2 +19.043 MeV, 2 2 2 T i 5 0 + 6 C 12 ^ 5 0 S n 1 1 2 +46.498 MeV. In the EDS analysis, carbon was not taken into account, because carbon was always present in the electronic microscope. T h e likelihood of a transformation of a major collection of nuclei was considered in a series of papers as transitions from one state to a n o t h e r . 1 5 " 1 6 It is not clear what the mechanism of the transition might be. T h e formation of microdischarges (unipolar arcs) was observed during the impulsive discharges and was studied by Ivanov et al, 1 3 T h e craters and local sites of a remelted material were shaped on a surface of the cathode during these processes. T h e formation of craters from microexplosions and local sites of the fused metal was noted for the similar processes in glow discharge plasma. Formation of pairs of craters separated by 100 /im suggests t h a t these formations were created simultaneously. T h e result with appearing of similar additional chemical elements on P d cathode was observed after electrolysis with plasma discharge in the paper 14 also. T h e similarity of the resulting effects in the various processes (glow discharge, electrolysis with plasma discharge and other methods of excitation) could all be the same phenomenon. T h e opportunity of reactions with six deuterium atoms (ions) of the simultaneously participation was shown in the paper of Iwamura: 1 7 138 137 -62Sm150; - 62Sm149. 56Ba 56Ba But it could be fusion with one carbon a t o m (ion). Detection of the increased occurrence of anomalous elements in phase inclusions, micromeltings locations, craters from microexplosions, and tracks of the unusual
456
shape presumably could be the transmutations of elements under low-energy actions in deuterium glow discharge plasma. 2 ' 4-11 These anomalous elements were found in concentrations up to several percent, and they were not detected before the experiment. The opportunity for nuclear changes initialized by low-energy reactions was shown for uranium in an earlier paper. 12 It was shown that the uranium after irradiation by deuterium ions in a glow discharge plasma with a current of ~5 mA increased alpha, beta and gamma activity on both sides of the sample. This emission was shown to occur in subsequent analyses performed within a year of the experiment, and the change of amount of uranium and thorium in the cathode sample was also shown. 6. Conclusions (1) The following elements were found in Ti foil after deuterium glow discharge producing excess heat effect: O, F, S, Al, Na, Mg, Fe, and Ni, typically in amounts of 0.3-0.5% but sometimes up to 10%. (2) The appearance of new elements within structural defects on the surface (in the microexplosion locations, microcraters, local melting zones, phases inclusions on the tracks and others formations) could be the result of nonequilibrium processes such as a microarc with an overvoltage with some accelerated effect leading to fusion and fission reactions in the excited crystal lattice of cathode surface. (3) The appearance of most elements obeys the law of energy conservation. (4) Excess heat effect in Ti foil could be explained as a result of elements transmutation in the cathode under excitation of crystal lattice in the deuterium low energy glow discharge. (5) The similarity of resulting effects in the various processes (glow discharge, electrolysis with plasma discharge and other methods of excitation) could be due to the nature of the phenomena. (6) It is necessary to have more statistical results with sequential analysis for explanation and understanding of mechanism.
Table 5.
Isotopic shift in Ti after glow discharge.
Mass
Elements
Abundance (%)
CPS 1900°C experiment
CPS 1900° C initial
Isotopes ratio (abundance and experiment)
Abundance of I isotopes ratio/experiment of isotopes ratio
The increasing of mass after experiment (times)
A (cps)
1 40
2 Ca
3 96.9
4 1,250,000
6 > 10, 000
8 1. 5f
9
10
42
Ca
0.65
10.000
150
1. 3
66.7
9750±50
43
Ca
0.135
1,000
120
0.37
9.8
880±50
44
Ca
2.0
40,000
200
7 40/44=48.4 abun. 40/44=31exper. 40/42=161 abun. 40/42=125 exper. 44/43 14.8 abun. 44/43=40 exp. 44/42=3. 3 abun. 44/42 = 4 exper.
0.82
200
38800 ±50
55
Mn
100
1,500
450
33.3
A > 1440
458
References 1. A.B. Karabut, Ya.R. Kucherov, and LB. Savvatimova, Nuclear reaction on the cathode of glow discharge. Pisma v zhurnal technicheskoi fisiki, Lett. Tech. Phys. J. 16(12), p. 53 (1990). 2. A.B. Karabut, Ya.R. Kucherov, and LB. Savvatimova, Nuclear product ratio for glow discharge in deuterium, Phys. Lett. A 170, 265-272 (1992). 3. A.B. Karabut, Ya.R. Kucherov, and LB. Savvatimova, The investigation of deuterium nuclei fusion at glow discharge cathode, Fusion Technol 20, 924-928 (1991). 4. LB. Savvatimova, A.B. Karabut, and Ya.R. Kucherov, in Proceedings of the first Russian Conference on Cold Fusion (Novorossiysk, 1993. Moscow, VENT, 1994), p. 131. 5. LB. Savvatimova, A.B. Karabut, Ya. Kucherov, in Proceedings of the Fourth International Conference on Cold Fusion (Hawaii, USA, December, 1993), EPRI. VI. N 3.7. 6. LB. Savvatimova, Ya. Kucherov, and A.B. Karabut, Cathode material change after deuterium glow discharge experiments, Trans. Fusion Technol. 26, 4T 389-394 (1994). 7. LB. Savvatimova and A.B. Karabut, Nuclear reaction products registration on the cathode after deuterium glow discharge. Surface, Vol. 1 (RAN, Moscow, 1996), pp. 63-75. 8. LB. Savvatimova and A.B. Karabut, The chemical and isotope structure of Pd changes after ion irradiation in glow discharge, in Proceedings of the Third Russian Conference on Cold Fusion and Nuclear Transmutation (Sochy, October, 1995, , 1996), pp. 20-49. 9. LB. Savvatimova, A.D. Senchukov, and LP., Chernov transmutation phenomena in the palladium cathode after ions irradiation at the glow discharge, in Proceeding of the 6th International Conference on Cold Fusion (Japan, 1996), pp. 575-579. 10. I. Savvatimova, Transmutation in cathode materials exposed at glow discharge by low energy ions. Nuclear phenomena or ion irradiation result? in Proceeding of the ICCF-7, 1998, pp. 342-350. 11. LB Savvatimova, Reproducibility of experimental in glow discharge and process accompanying deuterium ions bombardment, in Proceedings or the ICCF8 (Italian Physical Society, Bologna, Italy, 2000) p. 277. 12. J. Dash, I. Savvatimova, S. Frantz, E. Weis, and H. Kozima, Effects of glow discharge with hydrogen isotope plasmas on radioactivity, in Proceedings of the ICCF9, (ICENES 2002) p. 122. 13. V.A. Ivanov, Excitation and effect of microplasma discharges on metals and alloys in a microwave plasma torch 2001, Appl. Phys. 2, 5-39. 14. S. Szpak, P.A. Mosier-Boss, and F.E. Gordon, Precursors and the fusion reactions in polarized Pd/D-D20 system: effect of an external electric field, in Proceedings of the ICCF11, 2004. 15. L.U. Urutzkoev, D.V. Filippov, Influence of atomic electrons on the nuclear stability and the processes of the radioactive decay, in Proceedings of the 10th Russian Conference on the Cold Transmutation of the Nuclear of Chemical Elements (Moscow, 2004). 16. B.U. Rodionov, Nuclear transmutation in polyatomic quantum ensemble, in Proceedings of the 10th Russian Conference on the Cold Transmutation of the Nuclear Of Chemical Elements (oscow, 2004). 17. Y. Iwamura, T. Itoh, J. Kasagi, et. al., Nuclear transmutation induced by deuterium permeation through the Pd complexes detected by surface and bulk analysis methods, in Proceedings of the ICCF-11 (Marseilles, France, 2004).
E N H A N C E M E N T M E C H A N I S M S OF LOW-ENERGY N U C L E A R REACTIONS
F. A. GAREEV, I. E. ZHIDKOVA, AND YU. L. RATIS Joint Institute for Nuclear Research, 141980, Dubna, Russia E-mail: [email protected]; [email protected]
1. Introduction One of the fundamental assumptions of nuclear physics since the very early days of its study has been that the radioactive process (the half-life or decay constant) is independent of external conditions. Rutherford et al.1 came to the conclusion that: The value of A (the decay constant) for any substance is a characteristic constantly independent of all physical and chemical conditions. This very important conclusion, which plays a negative role in cold fusion phenomenon, is based on the common expectation P. Curie suggested - that the decay constant is the etalon of time) - and the observation that the radioactivity is a nuclear phenomenon, and all our actions affect only states of the atom but do not change the state of the nucleus. We cannot hope to mention even a small part of the work done to establish the constancy of nuclear decay rates. For example, Emery stated 2 : Early workers tried to change the decay constants of various members of the natural radioactive series by varying the temperature between 24 and 1280 K; by applying pressure of up to 200 atm; by taking sources down into mines and up to the Jungfraujoch; by applying magnetic fields of up to 83,000 G; by whirling sources in centrifuges; and by many other ingenious techniques. Occasional positive results were usually understood, in time, as the result of changes in the counting geometry, or of the loss of volatile members of the natural decay chains. This work was reviewed by Meyer and Schweider,3 Kohlrausch, 4 and Bothe. 5 Especially, interesting for its precision is the experiment of Curie and Kamerlingh Onnes, 6 who reported that lowering the temperature of radium preparation to the boiling point of liquid hydrogen changed its activity, and thus its decay constant, by less than about 0.05%. Rutherford and Petavel, 7 who put a sample of radium emanation inside a steel-encased cordite bomb, are especially notable. Even though temperatures of 2500°C and pressures of 1000 atm were estimated to have occurred during the explosion, no discontinuity in the activity of the sample was observed. 459
460
It seemed at the time that this conclusion was supported by the following very clean and strong arguments (and common sense): (1) Nuclear processes have characteristic energies « 1 MeV, whereas chemistry has a few eV per atom, molecules have a part of eV. The inner atomic shells are bound with many keV in the medium and heavy elements. (2) The localization of electrons in atoms is « 10~ 8 cm, whereas the localization of nucleons in nuclei is fa 10~ 13 cm. Therefore, the nucleus should be unaffected by superficial atomic changes: nuclear processes should not be influenced by the surroundings. The constancy of nuclear decay rates was firmly established, confirming evidence from experimental studies of a- and /3-decays and theoretical estimations. The constancy of nuclear decay rates acquired the strength of a classical law. Any papers contradicting this law were ignored by all the scientific journals as erroneous. The history of science has own laws. The ground of the /3-decay of nuclei was given by Fermi in 1934. It was very easy to prove that certain processes of radioactive decay should be intimately connected with the presence of atomic electrons and may be affected by the changes in the electronic structure produced by chemical compounds. It took 13 years to understand this very simple phenomenon. The possibility of altering the decay rate of Be 7 was suggested in 1947 by Segre8 and by Dodel. 9 ' 10 In the case of electron-capture decays the decay rate is directly related to the density of atomic electrons in the nucleus and that the effects of different chemical environments should be measurable. The theoretical foundation was the following.8 The radioactive decay constant of a substance decaying by orbital electron capture is proportional to I^WI of the electrons. In the case of a light element like 7 Be it may be possible to alter this quantity by an appreciable amount by putting the Be in different chemical compounds. We would then have a slight change of the radioactive half-life of the Be in different compounds. The magnitude of the effect may be in the neighborhood of one percent, but it is practically impossible to give a quantitative estimate because the total change of ?/>(0) is affected by certain factors such as the density of the crystal, the nature of the chemical bond, etc. These factors are both positive and negative, and have comparable magnitudes. To obtain a reliable estimate of the effect we require more detailed knowledge of the wave functions for various compounds than is at present available. Experiments are in progress to detect the effect by comparing the half-life of 7 Be in Be metal with that in BeO or BeF 2 . The confirmed altered decay rate for Be 7 in different chemical compounds were of the order 0.1%. 2 The 6-h isomer 99m Tcdecays by internal conversion of a 2.2-keV E3 transition. The observed effects in different chemical forms were of the order 0.3%. 2 The greatest chemically induced half-life changes of the order 3.5% were established in Ref. 11.
461
The half-life of Be 7 electron capture was measured 12 in endohedral fulleren Be@C(60) and Be 7 metal: T 1 / 2 = 52.68 ± 0.05 and T 1 / 2 = 53.12 ± 0.05 days, respectively. This 0.83% difference between the electron capture in C6o and in Be 7 metal represents a strong environmental effect on the Be 7 EC capture rate, caused by the different electronic wave functions near the Be 7 nucleus inside a Ceo cage and inside Be metal. A weak interaction which is responsible for electron capture and other forms of /3-decay are of very short range. So the rate of electron capture and emission (internal conversion) is proportional to the density of electrons at the nucleus. This means that we can manage the electron-capture (emission) rate by the change of the total density in the nucleus. It can be carried out with different macroscopic ways using available environmental effects. These questions were highlighted in different reviews and books 2 > 1 3 - 1 9 at the end of the 1970s. The reader should compare the common accepted conclusions about the decay rates in the 1930s and the 1970s. Data on pleochroic halos led to the conclusion20 that those data do not provide convincing proof that the laws of radioactive decay are constant in time. Shnol et al.21 came to the conclusion that the decay rates of radioactive nuclei change in time with the period of 24 h, 27, and 365 days. Periodic variations in /3-decay rates of 60 Co, 90 Sr, and 137 Cs were discovered. 22-25 The 27-day and 24-h period in these changes were found. The aim of this talk is to discuss the possibility of inducing and controlling the nuclear reactions at low temperatures and pressures by using different low-energy external fields and various physical and chemical processes. The main question is: Is it possible to enhance LENR rates by using the low and extremely low-energy external fields? 7
2. Cold Fusion and Transmutation In 1989, Fleishmann and Pons reported their observation of nuclear products and excess heat on a palladium electrode during the electrolysis of solutions in heavy water. The electrochemical experiments were interpreted by the authors as a result of nuclear fusion reaction (named cold fusion), but the scientific community rejected this interpretation. More than 3000 papers in the field of cold fusion and transmutation (later called low-energy nuclear reactions, or LENR) were published. Various anomalous results were observed at low temperatures and pressures, which are beyond the framework of the modern theoretical paradigm. The theoretical models are not able to describe these anomalies even qualitatively. The reader can find the history and problems of cold fusion in the Proceedings of the International Conferences on Condensed Matter Nuclear Science, the Russian Conferences on Cold Nuclear Transmutation of Chemical Elements and Ball Lighting, and also in a recent review of the Department of Energy of the USA 26 and books. 27 ' 28 The Russian experimental data on the low-energy nuclear reactions are published in Refs. 29-32 and their new theoretical interpretation were given in Refs.33~36
462
T h e general important conclusion can be drawn from the studies performed during 15 years: T h e poor reproducibility of experimental results and extreme difficulties of their interpretation in the framework of modern standard theoretical physics are the main reasons of the persistent non-recognition of cold fusion and t r a n s m u t a t i o n phenomenon. Recent progress in b o t h directions is remarkable (see Abstracts ICCF-11, Marseille: France, 2004, 31 O c t o b e r - 5 November). Nevertheless understanding of rejection of this phenomenon by mainstream physicists is a key point for further success from fundamental research.
2 . 1 . Reproducibility
of Low-Energy
Nuclear
Reaction
Experiments
Reproducibility of experiments within and between laboratories is a fundamental requirement and cornerstone for any scientific investigations. There are many fundamental factors t h a t are relevant t o the issue of reproducibility (see details in Ref. 37). A person with perfect hearing might judge t h a t a viola can never be reproduced: it depends on too many factors (resonance conditions) t h a t are impossible to repeat. T h e semiconductor effect in a transistor is extremely sensitive to damage and impurities of crystal which were impossible to control in the initial experiments. T h e degree of reproducibility was gradually increased over several years when the properties of the materials were improved and standardized, and the process was optimized and controlled with high accuracy. T h e same should happen for reproducibility of L E N R . 2 7 However, we will show t h a t this expectation for L E N R is only partly correct. a T h e t a r g e t s in s t a n d a r d nuclear physics using accelerators are substances in the ground states: gases, amorphous solids or crystalline solids. T h e projectile particle interaction with target nuclei takes place in a vacuum. Therefore, the influence of the surrounding m a t t e r (say, atomic electrons) on the velocity of such nuclear processes (especially at high energies) should be negligible. It seems these expectations supported by estimations of energy and size differences (10~ 5 - 1 0 " 6 ) atoms and nuclei and experiments show almost full reproducibility. We come to the following conclusion: A greater p a r t of processes in nuclear physics take place in closed systems. Reproducibility of such experiments should be independent of the place and time of measurements - a cornerstone of t h e modern scientific method. LENRs occur in the surroundings (gases, condensed mater, water, solutions, etc.), a
References to original and review cold fusion literature are not given in our talk. available in ICCF Proceedings.
They are
463
which are induced by low-energy external fields such as ultrasound, electromagnetic fields, and lasers. So atoms, molecules in the surroundings and atoms of interacting nuclei are in excited states or ionized. Nuclei, atoms, the surrounding medium and external fields representing interacting subsystems together form a dynamic open system. Frequencies and phases of subsystem motions may be coordinated according to the universal resonance synchronization principle (see Appendix A) and the result may be a creation collective (coherent) state for the whole system. We will call such a system an auto-oscillation system in which the frequency of an external field and frequencies of the all subsystem are commensurate. The demand for frequency commensurability means that all motions in a system are in co-ordination (in resonance), which is difficult to fulfil. This is the cause of poor reproducibility of LENR. We formulate as a working hypothesis the following assumption: LENRs take places in open systems in which all frequencies and phases coordinated according to the universal resonance synchronization principle - main reason of poor reproducibility. Poor reproducibility and unexplained results do not mean that the experiment is wrong. 2.2. The Bound State
j3-Decay
Bound state f3~ decay (/3b), in which the decay electron remains in an electron bound state of the daughter atom and the monochromatic antineutrino carries the total decay energy Q, was first predicted by Daudel et al.3S in 1947 and discussed in Refs. 39-43. This new decay mode, the bound state /3~-decay, was for the first time experimentally observed for bare 163 Dy (Ref. 44) (bare means that the atom 163 Dy is ionized fully. We will use designation for this case as 1 6 3 Dy 6 6 + ) and 1 8 7 Re. 4 5 Nuclei 163 Dy are stable as a neutral atom {Qp = —2.565 keV) and become radioactive when fully ionized atoms (bare nuclei !63Dy66+) d e c a y t o i63Ho66+ ( Q K = +59.3keV) via the bound state /3b decay with a half-life of 47 days. Nucleus 163 Ho is unstable and it is transferred to 163 Dy by electron capture with a half-life of 4.6 x 103 years. The difference of masses m( 163 Ho) — m( 163 Dy) = 2.6 keV, therefore, the electron capture, is only possible from M- or higher orbits. Unstable nuclei 163 Ho became practically stable due to ionization of atoms 163 Ho up to these orbits because the electron capture in such cases is only possible from continuum states, which have an extremely small probability. The ionization of atoms changes the /3-decay direction of nuclei: in neutral atoms 163 Ho ( 163 Dy) the electron capture lead to the transition i63 H o ^163 D y (i63 D y a r e s t a b l e ) ; i n f u l l y i o n i z e d bare nuclei 1 6 3 Ho 6 7 + ( 1 6 3 Dy 6 6 + ) are stable (unstable). General conclusion: in neutral atoms the some ground state nuclei decay via orbital electron capture, for bare nuclei (fully ionized atoms) the electron capture branches are blocked. In such cases (if in addition the positron decays are lacking) bare nuclei became stable. This conclusion is a very strong and well known to nuclear researchers.
464
For neutral 187 Re only a unique, first forbidden transition to the 1 8 7 0 s ground state is energetically possible. The small matrix element and the small Qp value of Qp = 2.663 (19) keV lead to the long half-life of 42Gyr. The measured half-life45 for bare 1 8 7 Re 7 5 + (Q% = +72.97 keV) of T 1 / 2 = (32.9 ± 2.0) year is billion times shorter than that for neutral 187 Re. The ground state /3-decay (orbital electron capture) properties of nuclei cardinally change when all electrons of the atomic shells are removed: stable (unstable) nuclei become unstable (stable) and a half-life may decrease up to billion times - nine orders of magnitude. The interpretation is very simple: magnitude of Qp (Tj/ 2 ~ AQ^ ) and phase volume increase for the ionized atoms rather than for neutral ones and it is evident that the Pauli principle plays a different role in neutral and fully ionized atoms. 2.3. The Nuclear Decay of Coulomb Excited for Fully Ionized Atoms
and Isomeric
States
The half-lives of isomeric states of fully ionized i44mTt)65+; i 4 9m Dy 66+ a n d 151m Er 6 8 + have been measured. 46 The increase was observed of the half-lives of bare isomers by factors of up to 30 to their neutral counterparts. The authors 46 give the correct and evident interpretation of experimental results: This is due to the exclusion of the strong internal conversion and electroncapture channels in the radioactive decay of these bare nuclei. Experiments with highly ionized 57Fe
of
7
Be
Norman et al.49 measured 7 Be decay rates in gold (Au), graphite, boron nitride and tantalum (Ta). Among these materials, they found that the 7 Be half-life was the longest in Au and the shortest in graphite. According to their experiments, the decay rate of 7 Be in Au is lower than that in graphite by (0.38 ± 0.09)%. Ray 51 measured the difference 7 Be decay rates in Au and AI2O3 and found that the decay rate in Au was lower than that in A1 2 0 3 by (0.72 ± 0.07)%. Ray et al.50 pointed out that the apparent disagreement between the two sets of experimental results was most likely due to the choice of different reference samples with which the comparisons were carried out. Indeed, Norman et al.49 used a 7 Li beam for their implantation studies, whereas Ray 51 used proton beam. The radiation damage by 7 Li on gold lattice sites, where 7 Be nuclei stop, would be much larger 52 (3 x 10~ 4 vacancies/Angstrom/ion) than the corresponding damage
465
(10~ 5 vacancies/angstrom/ion) for a proton beam. Therefore, the radiation damage effects on lattice due to heavy ion irradiation might also be partly responsible for the apparent discrepancies. This means that to speak about reproducibility in this case we should take into account at least atomic physics effects that are usually ignored. The ratio of L to K-shell electron capture in 7 Be bare nucleus shows 53 that the measured ratio is less than half of the existing data for free 7 Be. These discrepancies are most likely due to the distortions of L and K-shell orbitals by the host medium. 2.5. Controlled
-y-Decay of Excited
Nuclei
According to modern theory, the spontaneous 7-decay of excited nuclei in free space without any material bodies is a noncontrolled process. Probability Aeg of this decay: 2 1
A eg
r
47T 2 W e g d e g
3h
is fully determined by the matrix element
p(weg)
4w,eg deg She2
of the nucleus dipole moment and
energy of the nuclear transition hu)eg = Ee — Eg. The total lifetime r t o t = T/(1 + a) and radiative lifetime r of this excited nucleus in free space are the constants. Here a is the coefficient of internal electron conversion for the nuclear transition^ — Es. Problems become very complicated in the important case when material bodies are present in the surrounding space. Vysotskii 54 considered the general system which included the excited atom nucleus, the system of atom electrons, the system of zero-energy (in vacuum state) electromagnetic modes and the screen - the system of N resonant or nonresonant atoms situated at the distance d 3> Aeg = 2nc/u)eg. The authors of55 concluded that: It is usually stated that in all cases with the presence of any material bodies at a macroscopic distance d S> Aeg = 27rc/weg from the excited nucleus the expression for the lifetime r and Ttot remains the same or changes by an immeasurably small value. This supposition is erroneous. It was shown54 that a spontaneous 7-decay is a process of an excited nucleus relaxation, the phase promise of which is caused by interaction with a fluctuating state of the thermostat at the distance d 3> Aeg from the nucleus. The phenomenon of a controlled nucleus 7-decay is a result of interaction of the nucleus with zero-energy modes, interaction of these modes with the atoms of controlled (and controlling) screen, and interaction of the nucleus with the system of atom electron. The increase in radiative lifetime r of an excited nucleus by 10-40% and total lifetime Ttot by 1% was observed in the experiments 55 ^ 57 with 7-source 57 Co (57*Fe)
466
and with 7-absorber made of stable 57 Fe isotope. So these results prove the possibility of controlled essential influence of a thin resonant screen on the amplitude, space and temporal characteristics of a spontaneous decay and excited nuclei radiation. 2.6. Okorokov
Effect
Let us consider the interaction of an incoming particle (atom or nucleus having the ground state Eg and the excited state Ee) with the crystal target. It is possible to choose the conditions 58 ' 59 when the frequency of a collision particle with the atoms of crystal vco\ = VQ/CIO (the velocity VQ of a particle motion ao is the distance between the atoms in the crystal) will be commensurate with the transition frequency vtl of the particle Ee - Eg
v
u
—
where rii is the integer numbers. It is between the particle and atoms of the If the particle interacts with the n exciting the particle is equal to W(n)
7
m — —^coi,
n n clear that in such conditions the interaction crystal should have a resonance character. atoms of the crystal, then the probability of =
W(l)n2,
where W(l) is the probability of excitation of the particle by one atom of the crystal. This is a collective (coherent) amplification mechanism of the excitation for the projectiles in the periodic field of the crystal predicted first by Okorokov 58 ' 57 and also first observed experimentally by Okorokov 60-62 . The resonance and coherent amplification of atoms and nuclei excitations by the periodic fields of crystals is now well established and recognized by the physicists and is used in different applications, but is not known to cold fusion researchers. From a modern point of view, water has a very complicated geometrical structure as a collection of quasicrystal clusters (see Ref. 63 and references therein). The hydrogen atom, atoms and molecules, water and solutions, solid states and condensed matter have the same homology in the geometric structure where the de Broglie wavelength of electron in the ground state of hydrogen atom plays the role of the standard one. 64 The puzzle of poor reproducibility of experimental data of LENR is now evident: Electrolysis in solutions, discharge in gases and any external influence on atoms means. (1) The atoms are ionized, thus changing radioactive rates by bound state /?b-decay of nuclei. (2) The ions can be accelerated in such a way that they come to resonance conditions to intensify of excitation of nuclei, atoms. (3) Even small external fields can induce large responses as an avalanche in the mountains stimulated, say, by a noise.
467
A mechanical analogue of the observed phenomenon is the synchronization of oscillations of the pendulum clock suspended from the moving girder - the Huygens synchronization principle. 65 The universal resonance synchronization principle for a microsystem (for nuclei, atoms, molecules for living and nonliving cells) was established in Ref. 66. The decrease and increase of radioactivity of tritium with increasing temperature in small titanium particles was observed, 67 although current experiment and theory overlook this effect.
2.7. Nuclei and Atoms
as
Resonators
68
Schwartz in 1953 proposed to consider the nuclear and the corresponding atomic transitions as a unified process. This process contains the /3-decay which represents the transition of nucleon from one state to another with emission of electron and antineutrino and simultaneously the transition atomic shell from the initial state to the final one. A complete and strict solution of this problem is still wanting (see, e.g., review paper in Ref. 69). The division of decay energy into nuclear and atomic energies has only a conditional sense, especially, in the resonance case. The process has a resonance charter and its probability is large when energy differences of nuclear and atomic transitions become close to zero. The drastic acceleration of decay time in H-like ions of 2 2 9 m Th may be up to 10 5 . 69 The electron shell serves as a trigger, reducing the lifetime of the isomer by up to five orders of magnitude. The probability of the resonance transfer of energy by electrons from the nuclei can be increased by application of laser, which compensates for defects in resonance. The corresponding enhancement factor in some cases may be 103. It is important to note that the knowledge of isomer energy is not necessary; the laser should be synchronized on the atomic frequency. This is a real phenomenon of resonance synchronization (see Appendix A) of nuclear, atomic, and laser frequencies to control the decay processes. It is also predicted 70 that the lifetime of the hindered photo-fission can be reduced up to 10 3 -10 4 by application of laser. The laser in this case changes the angular momentum of decaying state by unity practically without altering its energy. Low-energy external fields in LENR can play the role of a trigger changing the quantum numbers of the hindered or forbidden processes so that the first should be enhanced and the second should be allowed. This mechanism inducing LENR may be the main reason for poor reproducibility of LENR experiments and main mechanism of geotransmutations and biotransmutations.
468
2.8. Geo-, Bio- and Alchemical
Transmutations
All the above-described mechanisms of LENR are grounded in the universal resonance synchronization principle (see Appendix A). The main requirement of this principle is that the frequencies ^(ext) of external fields should be commensurate with the frequencies fj(in) of subsystems making a whole system: z^(ext) = Vj(in)n(j')/n(i).We strongly emphasize that the frequency of an external field can be infinitely small in comparison with the corresponding frequencies of subsystems. The frequencies i^(ext) function as triggers, starting the emission of internal energy. The enhancement (resonance) effect on LENR induced by external fields can be extremely large (or small) when maximal values of density distributions for external fields and the corresponding distributions of a subsystem coincide (or do not coincide). This means: Even extremely low-energy external fields may induce nuclear transmutations with emission of internal high-energies according to the universal resonance synchronization principle. Natural geo-transmutations in the atmosphere and earth occur at the points of strong change in geo-magnetic and electromagnetic fields. 71-73 Vysotsky and Kornilova published an excellent book: Nuclear Fusion and Transmutation of Isotopes in Biological Systems,74 we refer the reader to this book. According to Gareev some alchemists may 75 "change base metals into noble ones, silver or gold." This would not contradict the mechanisms of LENR described above.
2.9. Ball Lightning
as Macroscopic
Low-energy
Nuclear
Reactor
All internal contradictions of the previous theories of a ball lightning were based, by default, on an assumption that the ball lightning is a plasmoid. In order to maintain the macroscopic volume of air (the mixture of nitrogen, oxygen, water vapour, etc.) in an ionized condition it is necessary to provide a great amount of energy from some kind of a source. Many experimenters, among them such well-known experts as Kapitsa, made repeated attempts to create a long-living spherical plasmoid in laboratory conditions. However, no efficient way to supply the isolated plasma clots with energy or maintain them in a stationary condition for a few minutes (i.e., for the lifetime of natural ball lightning) could be found. The purpose of this paper is to substantiate a hypothesis that the natural ball lightning is an area of space where the chain nuclear reaction of the bound-state /3-decay of radioactive phosphorus nuclei takes place. It is shown that the analyzed phenomenon is related to the physics of electrical discharge in gases indirectly. Therefore the term globular lightning is not sufficiently correct. The main hypothesis, which is asserted hereinafter was formulated for the first time in Ref. 76. The logic of this hypothesis is as follows:
469
(1) Ball lightning always leaves a smell of sulfur, ozone and nitrogen oxide after vanishing. 77 (2) Sulfur can be generated only as a result of phosphorus /3-decay.78 (3) The rate constant of /3-decay largely depends on the degree of ionization of the decaying radionuclide. 33 The half-life of ionized radiophosphorus is approximately 1-2 min and is comparable with the lifetime of ball lightning in natural conditions. (4) Radiophosphorus is abundant in nature. It is found in rainwater in macroscopic amounts. 79 This model was proved in Ref. 76 and we believe it is now confirmed. Thus, ball lightning is a type of naturally occurring low-energy nuclear reactor.
3. Conclusions We have concluded that LENR is possible in the framework of the modern physical theory - the universal resonance synchronization principle based on its different enhancement mechanisms of reaction rates are responsible for it. b Investigation of this phenomenon requires the knowledge of different branches of science: nuclear and atomic physics, chemistry and electrochemistry, condensed matter and solidstate physics. The results of this research field can provide a new source of energy, new materials and technology. The puzzle of poor reproducibility of experimental data is due to the fact that LENR occurs in open systems and is extremely sensitive to parameters of external fields and systems. Poor reproducibility and unexplained results do not mean that the experiment is wrong.0
Appendix A A.l.
The Universal
Resonance
Principle
of
Synchronization
Many objects in Nature - elementary particles, nuclei, atoms, molecules, DNA, proteins, etc. - are built as self-consistent hierarchical systems and have the same homological constructions in the sense that they are found to obey the same fundamental physical laws: energy-momentum conservation law and sectorial conservation law (Kepler's second law). Schrodinger81 wrote that an interaction between microscopic physical objects is controlled by specific resonance laws. According to these laws, any interaction in a microscopic hierarchic wave system exhibits the b
Intensification of LENR using superwave excitation 8 0 is based on this principle. Solutions of salts, electrolytes and living systems contain a large amount of ions. In these cases the bound state /?i,-decay and other described above enhancement mechanisms of LENR can play an essential role. Unfortunately we do not know the works devoted to this problem. c
470
resonance character. The difference between eigen energies (eigen frequences) in one system should be equal to each other ' ' ' ' hv\ — hvx = hv2 — hv2, v\ ~ vx = v2 — V2h. (A.l) Therefore, eigen frequencies are additive. In other words, the resonance condition is formulated in the following way: oscillations participating in an interaction process should be constituents of the same frequencies. Thus, we come to the important conclusion: in a whole interacting self-consistent wave system the hierarchy of frequencies is established. So the sum of all partial frequencies is the integral of motion. Due to the aforementioned, the corresponding partial motions are determinate. This determinism arises as a consequence of the energy conservation law. As the resonance condition arises from the fundamental energy conservation law, the rhythms and synchronization of the majority of phenomena to be observed are the reflection of the universal property of self-organization of the Universe. The resonance synchronization principle is substantiated at the microscopic level (for details see Ref. 82) as the consequence of energy conservation law and resonance character of any interaction between wave systems. In this paper, we have demonstrated the universality of the resonance synchronization principle independent of substance, fields and interactions for microsystems. Thereby, we bring some arguments in favor of the mechanism - ORDER from ORDER, declared by Schrodinger, 83 a fundamental problem of contemporary science. We come to a conclusion84 that a stable proton and a neutron play the role of a standard for other elementary particles and nuclei. They contain all necessary information about the structure of other particles and nuclei. This information is used and reproduced by simple rational relations, according to the fundamental conservation law of energy-momentum. We originated the principles of commensurability and self-similarity.85 The commensurability and self-similarity result in the very unity of the world. The principle of commensurability is displayed in phenomena in different branches of science.85 All material objects (microsystems and macrosystems), which are described by standing waves, know all about each other. Each object is a scaled version of the other, and it is not possible to say which is more "fundamental." In this work, we have demonstrated that the structure of DNA and cell molecules can be calculated with some structure of a hydrogen atom. The interatomic distances in cell molecules are quantized according to the quantization rule of the fractional Hall effect. Therefore, we can conclude that the structure of DNA and cell molecules can be established from the analysis of hydrogen spectra using the quantization rule of the Hall effect and vice versa. 86 The bridge between the structure of a hydrogen atom, cell molecules and the Hall effect exists! It is very surprising that there are phenomena in Nature that are really described by simple rational relations. Only the fundamental conservation law of energy-momentum is responsible for this harmonic movement. The resonance principle of synchronization became a fruitful interdisciplinary science of general laws of self-organized processes in different branches of physics. It is intriguing to speculate that many questions can now be formulated as a result
471
of universality of the resonance synchronization principle independent of substance, fields, matter and interactions for microsystems and macrosystems. 86 Information concerning important details of an ecosystem's evolution is contained in frequency spectra. Therefore, matter turns out to be a form of organized information. The Universe was arranged according to number, harmony, and perfect forms. A new concept in evolution is robustness. One suggests simulating evolution of complex organisms constrained by the sole requirement of robustness in their expression patterns. Robustness in biophysics is defined as the ability to function in face of substantial changes in components. Robustness is implemented by constraining subsequent patterns to have similar expression patterns. Key properties of biochemical networks are robust, i.e., they are insensitive to precise values of the biochemical parameters. 87 Robustness is an important ingredient in simple molecular networks and, probably, also an important feature of gene regulation. Bornhold and Sneppen 88 suggest considering robustness as an evolutionary principle. We came to the conclusion that the robustness principle can be understood in the framework of the universal resonance synchronization principle. We have concluded that the homology of atom and molecule structures exists. This means that the de Broglie wavelength Ae of electron in the ground state of a hydrogen atom plays the standard role - all interatomic distances in molecules could be commensurable with Ae. There are huge examples of commensurable ratios between the interatomic distances and Ae in superconducting, nanomaterials, DNA, protein, and living molecules.86 A molecule is an aggregate of atoms in a distinct three-dimensional arrangement. Distances between atoms fix the structure of the molecules, as has been so forcefully emphasized by Pauling. These interatomic distances depend on the resonance interactions between atoms and also on the sizes of atoms. Again, we conclude that each object is a scaled version of the other. We assume now, as a working hypothesis, that the De Broglie electron wavelength in a hydrogen atom in the ground state can be considered as a standard of dimensions for atoms and interatomic distances in molecules. So, interatomic distances and radii of atoms can be written in the following way: T) 1
R=—
Ae,
(A.2)
where Ae = 0.3324918 nm is the de Broglie electron wavelength in a hydrogen atom in the ground state and ni(ri2) = 1, 2, 3 , . . .
Note that the quantization conditions for the fractional Hall effect86 are the same as (A.2). The fractional Hall effect demonstrates only the commensurable velocities of electrons in hydrogen atoms and GaAs-type heterostructures (two-dimensional electron gas). So there is no room for interpretation of the fractional Hall effect in terms of the fractional charge. Nobody observed the fractional charge in Nature.
472
It is well known in optics (in quantum mechanics too) that the transition coefficient of light through the layer is equal to one if the following relations between the thickness R of the layer and wavelength Ae is exist 71
R=-Xe,
n = 1,2,3,...
(A.3)
It is interesting to note that: (1) The Bohr quantization conditions AN = A^Ae for a hydrogen atom and the quantization conditions AN = A ^ H e for superfluid 4 He coincide with (A.3) if N = n/4. (2) The Tomasch quantization conditions for tunneling are the same as (A.3). (3) We carry out a systematic analysis of interatomic distances for a huge number of systems, using (A.3) in which A = Ae is the electron wavelength in the ground state of a hydrogen atom. We come to the conclusion that the superconductivity can be explained by the assumption: channel motions in systems like that and electron motion in the ground state of a hydrogen atom are exactly synchronous. Therefore, superconductivity systems represent a coherent synchronized state - a complex of coupled resonators with commensurable frequencies. This means that we have in principle found a possible way to achieve super-conductivity at room temperature. 86 The parameter-free formula for interatomic distances in biomoleculas, superconducters, and size of nanostructures has been obtained. This establishes a bridge between the structures of different phenomena (conductivity, superconductivity, insulator-metal transmission, quantum Hall effect, superfluidity, quantization of nanostructure cluster size, and size of biomolecules). This connection can be considered an indication of the existence of some physical phenomena in the structures of the superconducting and living systems. We have shown86 only a small part of our calculations by formula (A.3) and the corresponding comparison with experimental data for interatomic distances in some molecules. These formulas produce a surprisingly high accuracy description of the existing experimental data. Understanding of the origin and evolution of the genetic code must be the basis for a detailed knowledge of the relationship between the basic building blocks of DNA and environment. As is widely accepted today, essentially all DNA is in a eukaryotic nucleus formed from histones and different chromatin structures folded hierarchically. At least five orders of DNA and chromatin organization and folding (nucleotide, helix, nucleosome, solenoid, and chromatin fiber loop) have been described in literature. A DNA chain is a long unbranched polimer composed of only four types of subunits. These are nucleotides containing the basis adenin (A), cytozine (C), guanin (G), and thymine (T). These nucleotides form complementary flat pairs and the distances between these plains are equal toAe.
473
This means that the structures, formed in DNA molecules by nucleotides, produce the two- and three-dimensional waveguide. All proteins look like dimers in which the two copies of the recognition helix are separated by exactly one turn of the DNA helix: 3.4 nm <=> 10Ae = 3.325 nm. The DNA is packaged with histones into regularly repeating nucleosomes that are packed into 30 nm (it's diameter) fibers;30 — 90Ae = 29.92 nm, it is also elaborated, folded, and organized by other proteins into a series of subdomains of distinct character. This higher-order packing is the most fascinating and also most poorly understood aspect of chromatin. Molecules of DNA, amino acids, proteins, . . . contain tetrahedral blocks H3C-C with the angles < HCH = < HCH = 109.47° with the bond length 3d(H - C) = Ae = 0.3325 nm and 3rf(H - C) + d(C - C) = 3/2Ae = 0.4987 nm. Note that these molecules of amino acids and DNA have planar blocks H2N-C, whose bond length is equal to 2d(H — N) + d(N — C) = Ae = 0.332 nm. Pentagonal rings in adenine and guanin have the bond length equal to 0.668 andO.666 nm, respectively, which is close toAe = 0.665 nm. Many distances in living molecules are commensurable with the de Broglie wavelength Ae of an electron in the ground state of a hydrogen atom. This means that Ae play the role of the standard distance in molecules, especially in living molecules. Hence, the electron motions in a hydrogen atom and in living molecules are synchronized and self-consistent. A hydrogen atom represents radiating and accepting antennas swapping the information with the surrounding substance. Gryzinski 90-92 has proved that atoms are the quasi-crystal structure with definite angles: 90, 109, and 120°, which are the well-known angles in crystallography. We have proved the homology of atom, molecule and crystal structures. So the resonance synchronization principle is substantiated at the microscopic level as the consequence of the energy conservation law and resonance character of any interaction between wave systems. The commensurability and self-similarity result in the very unity of the world. This means our method can be used in different fields of fundamental research and also in applications such as: the construction of new materials such as hightemperature superconductors, new kinds of drugs, new methods in diagnostics of diseases, and new devices by analogy with biomolecules. References 1. E. Rutherford, J. Chadwick, and CD. Ellis, Radiations from Radioactive Substances (Cambridge University Press, Cambridge, 1930). 2. C.T. Emery, Annu. Rev. Nucl. Sci. 22, 165 (1972). 3. S. Meyer, and E. Schweidler, Radioactivitat, 2nd ed. (B.G. Teubner, Leipzig, 1927). 4. K.W.F. Kohlrausch, Radioactivitat, Handbuch der Experimentalphysik, Vol. 15 (Akademische verlagsgesellschaft mbH, Leipzig, 1928).
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5. W. Bothe, in H. Geiger and K. Scheel (Eds.), Handbuch der Physik, Vol. 22-1, 2nd ed. (Springer, Berlin, 1933), p. 201. 6. M. Curie, and M. Kamerlingh Onnes, Le Radium 10, 181 (1913). 7. E. Rutherford, and J.E. Petavel, Br. Assoc. Adv. Sci. Rep. A 456 (1907); E. Rutherford, Collected Papers, Vol. 2 (Interscience, New York, 1963), p. 36. 8. E. Segre, Phys. Rev. 7 1 , 274 (1947). 9. R. Daudel, Rev. Sci. Paris 85, 162 (1947). 10. R. Bouchez, R. Daudel, P. Daudel, and R. Muxart, J. Phys. Radium 8, 336 (1947). 11. J.A. Cooper, J.M. Hollander, and J.O. Rassmusen, Phys. Rev. Lett. 15, 680 (1965). 12. T. Ohtsuki, H. Yuki, M. Muto, J. Kasagi, and K. Ohno, Phys. Rev. Lett. 9 3 , 112501-1 (2004). 13. S. DeBenedetti, Des. Barros, and G.R. Hoy, Ann. Rev. Nucl. Sci. 16, 31 (1966). 14. C.B. Starodubchev, Transmutations of Nuclei and Atomic Shells. Book 1 (Tashkent, 1969), in Russian. 15. E.J. Konopinski, The Theory of Beta Radioactivity (Oxford University Press, London, 1966). 16. H.F. Schopper, Weak Interactions and Nuclear Beta Decay (North-Holland, Amsterdam, 1966). 17. C.S. Wu, and S.A. Moszkowski, Beta Decay (Interscience-Wiley, New York, 1966). 18. R. Bouchez, and P. Depommier, Rep. Prog. Phys. 23, 395 (1960). 19. D. Berenyi, Rev. Mod. Phys. 40, 390 (1968). 20. R.M. Spector, Phys. Rev. A 5 , 1323 (1972). 21. S.E. Shnol, et al., UFN, 168, 1129 (1998) (in Russian). 22. A. Baurov Yu, and V.L. Shutov, Prikladnaja Fizika, 1, 40 (1995) (in Russian) 23. A. Baurov Yu, A. A. Kondratov, V.F. Kushniruk, and G. Sobolev Yu, Scientific Report 1995-1996, "Heavy Ion Physics," Preprint JINR E7-97-206 (Dubna, 1997), p. 354. 24. A. Baurov Yu, A.A. Konradov, and G. Sobolev Yu, E-print hep-ex/9809014, 16 September 1998. 25. A. Baurov Yu, et al., Mod. Phys. Lett. A16, 2089 (2001). 26. P.I. Hagelstein, M.C.H. McKubre, D.J. Nagel, T.A. Chubb, and R.J. Hekman, New Physical Effects in Metal Deuterides (2004). 27. S.V. Krivit, and N. Winocur, The Rebirth of Cold Fusion (Los Angeles, 2004). 28. A. Kirkinski v., and A. Novikov Yu, Theoretical Modeling of Cold Fusion (Novosibirsk, 2002). 29. L.I. Urutskoev, and V.I. Liksonov, V.G. Tsinoev, Prikladnaja Fizika 4, 83 (2000) (in Russian) 30. L.I. Urutskoev, V.I. Liksonov, and V.G. Tsinoev, Annales de la Foundation de Broglie 27, 701 (2002). 31. V.F. Balakirev, et al., Transmutations of Chemical Elements (UrO RAN, Ekaterinberg, 2003). 32. V.D. Kuznetzov, et al., Annates de la foundation de Broglie 28, 173 (2003). 33. F.A. Gareev, I.E. Zhidkova, and L. Ratis Yu, Preprint JINR P4-2004-68 (in Russian) (Dubna, 2004). 34. F.A. Gareev, I.E. Zhidkova, and L. Ratis Yu, in Proceedings of the 11th Russian Conference on Cold Nuclear Transmutation of Chemical Elements and Ball Lighting, Dagomys, City of Sochi, September 28-October 5, 2003, Moscow 2004, p. 169. 35. F.A. Gareev, G.F. Gareeva, and I.E. Zhidkova, Geoinformatika (in Russian), 1, 51 (2003). 36. F.A. Gareev, and L. Ratis Yu, Science, Economy and Management, Vol. 3 (Samara, 2002), p. 103. 37. D.J. Nagel, and J. Godick, in Proceedings of the ICCF-10 (2003).
475 38. 39. 40. 41. 42. 43. 44. 45. 46. 47. 48. 49. 50. 51. 52. 53. 54. 55. 56. 57.
58. 59. 60. 61. 62. 63. 64. 65. 66. 67. 68. 69. 70. 71. 72. 73. 74. 75.
R. Daudel, M. Jean, and M. Lecoin, J. Phys. Radium, 8, 238 (1947). J.N. Bahcall, Phys. Rev. 124, 495 (1962). I.S. Batkin, Izv. AN SSSR, ser. fiz. (in Russian), 49, 1279 (1976). I.V. Kopytin, Doktorskaja Dissertachija (in Russian) (Voronezh, 1986). K. Takahashi, and K. Yokoi, Nucl. Phys. A404, 578 (1983). K. Takahashi, R.N. Boyd, G.J. Mathews, and K. Yokoi, Phys. Rev. C36, 1522 (1987). M. Jung, et al, Phys. Rev. Lett. 69, 2164 (1992). F. Bosch, et al, Phys. Rev. Lett. 77, 5190 (1996). A. Litvinov Yu, et al, Phys. Lett. B 5 7 3 , 80 (2003). W.R. Phillips, et al, Phys. Rev. A47, 3682 (1993). F. Attallah, et al, Phys. Rev. C55, 1665 (1997). E.B. Norman, et al, Phys. Rev. Lett. B519, 15 (2001). A. Ray, R Das, S.K. Saha, and S.K. Das, Phys. Lett. B 5 3 1 , 187 (2002). A. Ray, et al, Phys. Lett. B455, 69 (1999). I.F. Ziegler, J.P. Bierserk, and U. Littmark, The Stopping Range in Solids (Pergamon, New York, 1985). Voytas, et al, Phys. Rev. Lett. 88, 012501 (2002). V.I. Vysotskii, Phys. Rev. C58, 337 (1998). V.I. Vysotskii, A.A. Kornilova, A.A. Sorokin, V.A. Komisarova, S.I. Reiman, and G.K. Riasnii, Laser Phys. 11, 1 (2001). V.I. Vysotskii, V.P. Bugrov, A.A. Kuzmin, et al, Hyperfine Interactions 107, 277 (1997). V.I. Vysotskii, V.P. Bugrov, A.A. Kornilova, and S.I. Reiman, in Proceedings of the International Conference on the Physics of Nuclear Science and Technology, Vol. 2 (1739), 1998, p. 1739. V.V. Okorokov, Sov. J. Nucl. Phys. 2, 719 (1965); Jadernaja Fizika (in Russian), 2, 1009 (1965). V.V. Okorokov, JETP Lett, (in Russian) 2, 111 (1965). V.V. Okorokov, et al, JETP Lett, (in Russian) 16, 588 (1972); JETP Lett. 16, 415 (1972); A43, 485 (1973). V.V. Okorokov, et al, Preprint ITEP No. 19, 1973. V.V. Okorokov, in Proceedings of FPV-2002, Novosibirsk, 2002, p. 48. S.V. Senin, The Water (Moscow, 2004). F.A. Gareev and G.F. Gareeva, FPB 2000 (Novosibirsk, 2000), p. 161. I.I. Blechman, Synchronization in Nature and Technology (in Russian) (Moscow, Nauka, 1981). F.A. Gareev and G.F. Gareeva, in Proceedings of the First International Workshop, Saint-Petersburg, 18-21 June 2000, Sarov, 2001, p. 179. O. Reifenschweiler, Phys. Lett. A184, 149 (1994). H.M. Schwartz, J. Chem. Phys. 21, 45 (1953). F.F. Karpeshin, Hyperfine Interaction 143, 79 (2002). P. Gangrski Yu and B.N. Markov, Nuclei on Ray of Laser (in Russian) (Moscow, 1984). V.A. Krivizski, Transmutations of Chemical Elements in Evalutions of Earth (in Russian) (Moscow, 2003). S.E. Jones and J.E. Ellsworth, in Proceedings of the 10th International Conference on Cold Fusion (LENR-CANR.org, Cambridge, MA, 2003). B.A. Mamyrin I.N. Tolstixin, Isotops of He in Nature (in Russian) (Moscow, 1981). V.I. Vysotskii and A.A. Kornila, Nuclear Fusion and Transmutation of Isotopes in Biological Systems (Moscow, 2003). J. Perez-Pariente, J. Sci. Exploration A, 593 (2002).
476 76. L. Ratis Yu, Natural Science. Economy. Management. Special Issue. (Samara, SSAU, 2003), p. 4; L. Ratis Yu, Ball Lightening as Macroscopical Quantum Phenomena, Monography (Samara, SSC RAS, 2004), 132 p, Preprint JINR P4-2004-67, Dubna, 2004, 16 p. 77. B.M. Smirnov, UFN 160 (4), 1 (1990). 78. LP. Selinov, Isotopes 1, M: Science, 1970. 79. D. Lai, N. Narasappaya, and P.K. Zutshi, Nucl. Phys. 3, 69 (1957). 80. I. Dardik, et al., in Proceedings of the 10th International Conference on Cold Fusion (LENR-CANR.org, Cambridge, MA, 2003). 81. E. Schrodinger, Brit. J. Philos. Sci. 3, 233 (1952). 82. F.A. Gareev, Preprint No. 13-98 (in Russian), Institute of Nuclear Physics, Alma-Ata, 1998, p. 115. 83. E. Schrodinger, What is Life? The Physical Aspects of the Living Cell, 1955. 84. F.A. Gareev, in ISINN- VII (Dubna, May 25-28, 1999), p. 71. 85. F.A. Gareev, JINR Communications E4-97-25, Dubna, 1997; JINR Communications E4-96-456, Dubna, 1996. 86. F.A. Gareev, in FPB-98, Novosibirsk, June 1998, p. 92; F.A. Gareev and G.F. Gareeva, in FPB-00, Novosibirsk, July 2000, p. 161; F.A. Gareev and I.E. Zhidkova, in FPB-02, Novosibirsk, July 2002. 87. U. Alon, M.G. Surette, N. Barkai, and S. Leibler, Nature 397, 168 (1999). 88. S. Bornhold, K. Sneppen, NORDITA preprint - 99/83 CM, Copenhagen, 1999. 89. L. Pauling, The Nature of the Chemical Bond (Cornell University Press, 1960). 90. M. Gryzinski, in FPB-2000, Novosibirsk, July 2000, p. 89, 2001; Sprawa Atomu, Hamo-Sapiens, Warszawa, 2002. 91. M. Gryzinski, Preciesly About Atom (in Russian), Novosibirsk, 2004. 92. M. Gryzinski, J. Chem. Phys.62, 2629 (1975); Phys. Lett. A 4 1 , 69 (1972).
CO-DEPOSITION OF PALLADIUM W I T H H Y D R O G E N ISOTOPES
J. D A S H A N D A. A M B A D K A R Low Energy
Nuclear
Laboratory
Portland
State
University
Portland,
OR 97207,
USA
Palladium was co-deposited with hydrogen isotopes on a Pd cathode. This resulted in enhanced production of excess thermal power. After electrolysis the Pd L/3/La ratio was found to be increased in characteristic X-ray spectra from localized, microscopic areas on the surface of the Pd cathode. This suggests the possibility that appreciable amounts of silver are present in these areas.
1. Introduction In an experiment using a cell with one Pd and one Pt electrode in H2SO4-D2O electrolyte, the polarity was switched by mistake, so that the Pd became the anode and the Pt became the cathode. 1 During the next 4h and many subsequent experiments, this cell produced excess thermal power compared with a control cell. Pd dissolves from the Pd anode and co-deposits with hydrogen isotopes on the Pt cathode. Co-deposition of Pd with hydrogen isotopes has been studied extensively by Szpak and Mosier-Boss.2 In this report, we describe the results of co-deposition of Pd with hydrogen isotopes on a Pd cathode. 2. Experimental Methods and Results Closed cells were constructed using 200 ml Berzelius beakers (Pyrex, without pouring spouts), Teflon lids fitted to each beaker, perforated Teflon baskets filled with recombination catalyst and suspended above the electrolyte, and thin foil electrodes connected to platinum wires which were threaded through the Teflon tops (Fig. 1). A control cell and an experimental cell were identical except that the control cell contained two Pt foil electrodes and H2O-H2SO4 electrolyte, whereas the experimental cell contained a Pt anode and a Pd cathode, and D2O-H2SO4 electrolyte. The recombination catalyst was 0.5% Pd on coconut charcoal. The experimental cell electrolyte consisted of H2SO4 and D 2 0 in the ratio 1:6.7. The average temperature of each cell was determined with the aid of a data acquisition system which monitored three thin foil, type K thermocouples attached to the outside of each cell. One thermocouple was attached to the bottom of each cell, and one was attached opposite each electrode. The output of the thermocouples was monitored with an automated data acquisition system. The power supply was operated in the constant 477
478
Electrode lead wires
Adhesive tape
O-ring, inert * f to electrolyte
Catalyst chamber (Teflon) with perforations on bottom and on periphery Support pole (Teflon;
Control cell solution Sulphuric acid and deionized H 2 0 in the ratio 1:12.3
Pt electrodes
Figure 1.
•#
^
Control cell used for electrolysis in series with an experimental cell.
current mode, and the cells were connected in series. The cells were held in recesses cut into a Styrofoam base. Cell voltages were monitored with a strip chart recorder. The ambient temperature was monitored with a thermocouple in the space between the cells. Each cell was weighed before and after each experiment to determine the extent of energy losses due to incomplete recombination. Figure 2 shows the results of an experiment in which the control cell had greater power input throughout the 5.5 h experiment, but the experimental cell temperature was about 3°C higher at the end of the experiment. During the first 2700 s of the experiment, both cells had the same temperature, starting at 21°C and rising to 50°C. During this period the input power to the control cell was about 0.3 W greater than the input power to the experimental cell. Then the current to both cells was reversed, so that the anode of the experimental cell was now Pd and the cathode was Pt. Both electrodes of the control cell were Pt, but the cathode with a dark surface layer formed during prolonged electrolysis was now the anode.
479
Current normal
Current reversed
a
Pc Control cell power input (W)
o
Pe Experimental cell power input (W)
-•'-*••- Tc Control celi temperature (°C) m • Te Experimental cell temperature (CC) " ! -* m Ta Ambient temperature (°C)
Times (s)
Figure 2. Temperature and power results for electrolysis of heavy water with a Pd cathode compared with a control. Pd dimensions: 2.5 cm X 1.25 cm X 0.035 cm. Constant current was 3 A and current density was ~ 0 . 5 A / c m 2 . Error bars are embedded in the data points. Error for power values was ±0.03 W and ±0.1°C for temperature.
After the current was reversed, the power input to both cells dropped due to enhanced conductivity. The drop was much greater for the experimental cell than for the control cell, probably because Pd was dissolving from the anode and depositing on the cathode, thus increasing the surface area, which lowered the cell voltage. The control cell received 0.9 W more power than the experimental cell after electrolysis for 6500s, but both cells had the same temperature (55°C). After electrolysis for 8700 s, the control cell was receiving 1.2 W more power than the experimental cell. Now the control cell temperature was almost 2°C higher than the experimental cell. After 12,000 s, there was no change in power input to the two cells, but the control cell temperature was about 3°C higher. Now the current was again reversed, so that the Pd electrode in the experimental cell was again the cathode. The control cell voltage and temperature began to decrease and the experimental cell voltage and temperature began to increase. After a total of 16,200 s of electrolysis, the control cell was receiving 0.15 W more power, but its temperature was now about 1°C lower than the experimental cell. Now the cell voltages remained constant for the remainder of the experiment, but the temperatures continued to
480
SEM Mag: 0.017k x
0.6 mm
Figure 3. SEM photograph of a portion of the Pd cathode from the experimental cell. The area within the rectangle was enlarged (Fig. 4).
diverge. After 20,700 s, the control cell was receiving about 0.2 W more power, but its temperature was now almost 3°C lower than that of the experimental cell. The power output of the experimental cells compared with the control cell was determined at steady state temperature, where the power input was equal to the power output. For the control cell at steady state: power in,
VJ = k(Tc - Ta) + dffc dt '
(1)
where Vc is the cell voltage, / the constant current, k the heat transfer coefficient, Tc the cell temperature, Ta the ambient temperature, and dHc/dt is the rate of enthalpy loss due to incomplete recombination. The latter term is determined from the change in weight of the cell and the duration of the experiment. This equation is solved for k which is then used in a similar equation for the experimental cell. In the equation for the experimental cell, a term for excess thermal power output is added on the left side to give: VJ
dHxs = HTe ~ Ta) dt
d#e di
(2)
where dHx s/dt is excess thermal power, and the subscript e refers to the experimental cell. If the right-hand side of Eq. (2) exceeds VJ, the input power to the experimental cell, then excess heat is being produced by the experimental cell.
481
SEMMag: 1.12kx
10 nm
Figure 4. Enlargement of area within the white rectangle in Fig. 3. The arrows 1-3 point to spots from which characteristic X-ray spectra were obtained.
The temperature and voltage for the control cell data at 27,000 s, the constant current (3 A), ambient temperature (24°C), and the rate of enthalpy loss caused by incomplete recombination are substituted into Eq. (1), and the heat transfer coefficient k is calculated. This k is substituted into Eq. (2), along with the temperature, voltage, and enthalpy loss data for the experimental cell. The excess thermal power is found to be 0.93 W. To estimate the accuracy of this result, the errors involved in power input and power output measurements must be estimated. The power input is the product of the constant, 3 A cell current and the voltage. Because the cells are connected in series, the measurement error for the current has no significant net effect on the power input. The measurement error for cell voltage was ±0.01 V. Therefore, the error in input power measurements was ±0.03 W, which means that the error bars for input power are embedded within the data points for input power in Fig. 2. The power output is calculated from temperature and mass measurements. At the beginning of the experiment the control cell temperature was 20.9°C±0.02, the experimental cell average temperature was 21.0°C ± 0.1, and ambient temperature was 21.0°C. The balance used for measurement of mass has a precision of ±0.1 g. Using this data, the uncertainty in the power output is estimated to be about ±0.1 W, and the calculated 0.93 W excess thermal power output is statistically significant. Subsequent runs gave similar results.
482
Figure 5. Characteristic X-ray spectrum from a point on a white particle on the surface of the Pd cathode from the experimental cell. Arrow 1 indicates the location of this point. The most prominent peaks in the spectrum are from Pd, Pt, and C. P t slowly dissolves from the anode and deposits on the cathode, and C most likely comes from the charcoal catalyst. The Pd L a peak occurs at 2.84keV, and the Pd L/3 peak occurs at 2.99 keV. The intensity ratio, Pd L/3/La, is expected to be 0.42 3 . In this spectrum this ratio is 0.45.
After a total of 229 h of electrolysis, the Pd cathode from the experimental cell was examined with a scanning electron microscope (SEM) equipped with an energy dispersive spectrometer (EDS) in order to characterize surface topography and microchemical composition. Figure 3 is a low magnification photograph of a portion of the Pd cathode. The topography is varied. The relatively smooth area enclosed in the white rectangle was examined at higher magnification (Fig. 4). The topography in Fig. 4 is quite varied. The bright, dendritic particles may have resulted from electrodeposition of Pd and Pt after the current reversal, as indicated in Fig. 2. The EDS characteristic X-ray spectrum shown in Fig. 5 was obtained from the bright particle indicated by arrow 1. By fixing the electron beam in the SEM on a spot, it is possible to obtain chemical analyses from about 1/xm3 on the surface of a specimen. The spectrum in Fig. 5 indicates that the chosen spot contains about 63 weight percent (wt.%) Pd, 24wt.% Pt, and 13wt.% C. Arrows 2 and 3 indicate two spots on the smooth, dark area shown in Fig. 4. The spectrum in Fig. 6 was obtained from the spot indicated by arrow 2. Quantitative analysis of the spectrum in Fig. 6 gave 4 wt.% C, compared with 13 wt.% C from a bright spot (Fig. 5). The other elements in the spectrum, Pd and
483
Figure 6. Characteristic X-ray spectrum from the dark spot indicated by arrow 2 in Fig. 4. The ratio Pd L/3/Pd La is 0.61. This is an increase of 36% compared with the spectrum in Fig. 5. This increase may be due t o overlap with Ag L a , which occurs at 2.98 keV. If so, then quantitative analysis indicates that this spot contains about 7wt.% Ag.
Pt, are in approximately the same ratio as in Fig. 5. Another difference in Fig. 6 compared with Fig. 5 is that the Pd L/3/Pd La ratio is 0.45 in the latter compared with 0.61 in the former. This difference is possibly due to the presence of Ag , for which the La peak occurs at 2.98 keV compared with 2.99 keV for Pd L/3. If this interpretation is correct, then spot 2 in Fig. 4 contains about 7% Ag. The spectrum in Fig. 7, obtained from the black spot indicated by arrow 3 in Fig. 4, is similar to the Fig. 6 spectrum. In Fig. 7 the Pd L/3/Pd La ratio is 0.71, compared with the expected 0.42 for pure Pd. 3 If this increase is caused by the presence of Ag, then the amount of Ag is about 10wt.%.
3. Discussion of Results The experiment described here shows that co-deposition of Pd with hydrogen isotopes enhances the production of excess enthalpy. Szpak and Mosier-Boss2 also reported excess enthalpy from their co-deposition experiments. In addition, localized changes in the ratio of Pd characteristic X-ray peak intensities suggests the presence of Ag in these microscopic areas. Confirmation of the presence of silver by some other method such as mass spectroscopy is necessary.
484
Figure 7. Characteristic X-ray spectrum from black spot indicated by arrow 3 in Fig. 4. Here the Pd L/3/Pd La ratio is 0.71. This is a 58% increase compared with this ratio in Fig. 5. If this increase is caused by overlap of Ag La with Pd L/3 , then quantitative analysis indicates that this spot contains about 10% Ag.
Acknowledgment This research was supported by a gift from the New York Community Trust. References 1. C. Cano, M.S. Thesis, Portland State University, 2002. 2. S. Szpak and P. Mosier-Boss, Thermal and Nuclear Aspects of the P d / D 2 0 System, Technical Report 1862, SSC San Diego, Vol. 1, 2002, p. 7. 3. G.G. Johnson Jr. and E. W. White, ASTM Data Series DS 46, American Society for Testing and Materials, 1970, p. 4.
VARIATION OF T H E C O N C E N T R A T I O N OF ISOTOPES C O P P E R A N D ZINC IN H U M A N P L A S M A S OF PATIENTS A F F E C T E D B Y CANCER
ANTONIO TRIASSI DASIT
S.P.A,
Via Merendi N 22, 20010 Cornaredo www.dasit.it
(MI),
Italy
In this paper, we demonstrate that the increase of copper and the reduction of zinc in the human plasma of patient with cancer, and in particular the Lymphoid Leukaemia, is a consequence of the isotopic constant of the enzymatic components copper/zinc dependent (DNA/RNA polymerase). Our hypothesis is that the reaction happens at the nuclear level in the human cell, and it is due to the action of a neutron (probably of deuterium of water) (J.F. Thomson, Biological Effects of Deuterium, Pergamon Press, Oxford, 1963) with the isotopic component of 6 4 Zn transmutation into 6 B Cu stable following reaction: 64
Zn + N(HDO) ->
65
Zn - • /3+ -> EC -> 7 - •
65
Cu
this produces energy of 0.325 MeV for the /3+ and equal energy of 1.118 MeV for the photon 7 with a half-life of 250 days.
1. Introduction Several studies indicate the possibility of using trace concentrations of metals in biological materials for an early diagnosis of cancer.1 Patients with cancer have evidenced altered concentrations of copper and zinc in particular, and in a generalized way of other metals in traces. 2 There exists a correlation between the concentration of copper and zinc and the development of Hodgkin's and non-Hodgkin's tumors, sarcomas and carcinomas that produce modifications in the concentration of the two metals. 3 These studies, evidencing in the cancer an increase of the content of copper in the human plasma and a probable reduction of zinc, do not, however, explain the cause of this modification in a convincing way. 4 ' 5 This study aims to change the vision of the type of reaction that takes place during the processes of synthesis of blood components, and to verify the values of the isotopic content of copper-65 and zinc-64 probably undergoes a nuclear reaction with the participation of a neutron (the deuterium in the water), in which zinc-64 transmutes into copper-65, with liberation of gamma radiation of 1.118 MeV and positive beta emission of 0.325 MeV. 485
486
2. M e t h o d s To demonstrate the presence of a nuclear reaction in biology we have used: (1) nuclear magnetic resonance for the content of deuterium in the human plasmas, (2) gamma counter to verify the presence of radiation in human plasmas, in comparison to the natural noise radiation, (3) neutronic activation for the isotopic constant, (4) mass spectrometry for the isotopic constant. In order to demonstrate this reaction we analyzed two groups of human plasmas: 11 normal samples, nine males and two females, with mean age of 60 years; and 11 pathological samples with cancer, nine males and two females, with a mean age of 60 years. These last subjects had no pharmacological or radiotherapy treatment. The preparation of human plasma to measure the deuterium content was done by adding 3 ± 1 ml of each plasma for single pathological sample in a single plastic vial, for a final volume of 30 ml, after aliquoting in three parts with 10 ml each. The same procedure was used for normal plasma. The instrumentations used for the measurements are as follows. Spectrometer NMR Bruker ARX 400 operating in FT, using a dedicated 10 mm probe, proton decoupling (CPD), 19 locks using an international standard (TMU) for deuterium quantification, with an S/N ratio for water signal >150. These tests have been executed on tests-tube mothers of normal and pathological plasmas a comparison of spectrums of range emission energy using one instrumentation with detector of range to germanium of type High Purity Germanium (HPGe). The detector has relative efficiency of 20% and was in a position to find range beams in the range of energy from 200 keV to 6 MeV approximately. We have repeated the measures of emission spectrum using a new one pool of normal and pathological plasmas. The instrumentation used for these measures has the following characteristics. Crystal HPGe Ortec EG&G with a window of Be-coupled integrated electronics Ortec EG&G "DSPEC"1.83keV a 1132 keV of 60 Co, rate peak Compton 54, efficiency related to 1.33 MeV of the 60 Co 21.2% Shaping 6 ms, used line sensitivity Zn/Cu 1/10Be/Kg, 65 Zn 1115.4 10h 20,000, 6 6 Cu- 6 4 Cu 1039.0-1345.5 1-5 min to 1 h. After we verified the exact isotopic content of 64 Zn and 68 Zn using neutron activation analysis in the same pool of normal and pathological plasmas, we proceeded to measure the same value in the human serum. The instrument used was a nuclear reactor for research of 250 kW Tigra Mark II total flux 1 x 10 13 Crystal HPGe Ortec EG&G with a window of Be-coupled integrated electronics Ortec EG&G "DSPEC"1.73keV a 1173 keV of 60 Co rate peak Compton 54, efficiency relative to 1.33 MeV of 60 Co 21.2%, shaping 6 ms used line sensitivity 65 Zn 1115.4 10 h 20,000, 66 Cu- 6 4 Cu 1039.0-1345.5 1-5 min-1 h 300-1000 sensitivity 102-103 pg Cu-Zn.
487
o O
Figure 1. The difference between the spectrum of the normal and pathological human plasmas: x-axis is expressed in channel. To express it as energy, take into consideration that zero (0) is 70keV ca. and one channel is about 0.7 keV.
At the end we verified the isotopic constant of the 66 Zn and 64 Zn in five samples of pathological human plasma in comparison with a pool of plasmas made with five normal samples with the natural value. Instrumentation used is high-resolution inductively coupled plasma mass spectrometer (HR-ICP MS) (AXIOM plus model, Vg Element, UK). The sensitivity in low resolution is at level below ppt (alsolOppq, therefore around to 10-14g/g), Cu and Zn have a very low interference and if they are present they can be resolved working at resolution of 1500. This decreases the power of transmission of the instrument and sensibility of the instrument approximately of 20% in our case we have not found meaningful interferences, after heating the samples in a bomb, which destroyed all organic material, the results agreed in both low and high resolution. 3. Results We have analyzed three pools of normal plasmas against three pools of pathological plasmas (patients with Hodgkin's disease) repeating the measure for three times, comparing the content of deuterium of plasmas and the content of deuterium of the water of sea, the results are listed in Table 1. These results demonstrated that there are differences of the 3.6% in water ref, and about 5 ppm in defect of deuterium in pathological plasmas. We have verified the difference in the gamma emission spectrum of the normal and pathological human plasmas (Fig. 1). These results demonstrated that there are differences in emission spectrum in the energetic zone of 512, 1115, and 438 keV.
120
50.00
352.00
715.00 Energy (keV)
1077.00
1500.00
120
o O
50.00
352.00
715.00 Energy (keV)
1077.00
1500.00
50.00
352.00
715.00 Energy (keV)
1077.00
1500.00
489 120
o O
50.00
352.00
715.00 Energy (keV)
1077.00
1500.00
Figure 2. (a) Spectrum of normal plasmas human pool normal plasma (50 patients), (b) Spectrum of pathological plasmas human pool pathological plasmas (50 patients), (c) Spectrum of plasmas differences normal pool/pathological pool, (d) Spectrum of noise in University Pavia laboratory.
Table 1.
Measures of the human plasmas repeated three times.
Integral of deuterium of water ref. Water ref. Mean = 4.858 S.D. = 0.0194 S.E. = 0.0158
ppm =155
Integral of deuterium of normal plasmas Plasma 1 Mean = 4.910 S.D. = 0.1085 S.E. = 0.886
Integral of deuterium of pathological plasmas Plasma 1 Mean = 4.606 S.D. = 0.159 S.E. = 0.130
Plasma 2 Mean = 4.852 S.D. = 0.128 S.E. = 0.1051
Plasma 2 Mean = 4.750 S.D. = 0.150 S.E. = 0.122
Plasma 3 Mean = 4.630 S.D. = 0.175 S.E. = 0.143
Plasma 3 Mean = 4.575 S.D. = 0.132 S.E. = 4.575
Pools plasmas normal (pi + p2 + p3) Mean = 4.800 S.D. = 0.143 S.E. = 0.116
Pools plasmas pathological (pi + p2 + p3) Mean = 4.640 S.D. = 0.094 S.E. = 00.076
ppm = 143
ppm = 138
Note: S.D., standard deviation; S.E., standard error; ppm, parts for million. Instrumental error from 0.5 to 1 ppm.
490
We have repeated the measures on other plasmas, comparing a pool of normal plasmas compared with a pool of pathological plasmas, but we have not find a significant difference of emission in comparison to the noise. The results do not show differences in energy spectrum of the 65 Zn 69 Zn (Fig. 2a-d). Subsequently, we have tried to determine by neutron activation the isotopic constant between 69 Zn and 65 Zn; the result that we have obtained demonstrates that the isotopic composition of the samples matches the natural composition within an error of 5%. The results do not reveal differences in the isotopic composition of the samples //g/kg 65 Zn and 64 Zn. Table 2. serum. Sample 69 Zn L PN PC SN SP
Measure of the isotopic component in plasma and human
Mean 6 9 Zn (^g/kg) 7.02 7.12 11.9 8.26 10.7
69
Zn
(%) 7.68 5.11 5.23 4.96 4.45
Sample 65 Zn L PN PC SN
sc
Mean 6 5 Zn (/ig/kg) 7.11 7.23 12.2 8.23 10.4
65
Zn
(%) 8.20 6.76 4.53 5.12 4.99
Note: L, reference control; PN, normal plasma; PC, pathological plasma; SN, serum normal; SP, serum pathological.
With mass spectrometry we have verified the relationship 66 Zn and 64 Zn and the data are showed in the Table 3. In Table 3, the differences between the two zinc isotopes are not pronounced; error is less than 1%. Table 3. Sample Natural Reference Plasma Plasma 1 Plasma2 Plasma 3 Plasma4 Plasma5
Measure of the isotopic component in human plasma.
Ratio 6 6 Z n / 6 4 Z n 0.57372 0.57422 0.57341 0.58580 0.58843 0.58730 0.57321 0.57759 0.57795
SD
SD (%)
Mean; SD; SD (%)
0.003 0.003 0.005 0.004
0.5 0.5 0.9 0.7 0.7 0.7 0.7 0.7
0.573815; 0.00057; 0.1%
0.004 0.004 0.004
0.58787; 0.00080; 0.1%
Note: N, internal control; R, human pool reference normal plasmas; Plasmas 1-5 Lymphoid Leukaemia control plasmas.
4. Conclusions Results from this study provide evidence that the proposed nuclear reaction in biological tissue is not totally refuted. Our idea is that the isotopes in the biological
491
reaction can be taken in serious consideration in one possibly more accurate and precise verification. Our goal is t h a t this research will stimulate and to involve more researchers in all the scientific disciplines, without contradicting the knowledge of the classic biology. At the same, we hope this will be the beginning of a future new scientific field.
Acknowledgments I would like t o t h a n k all my colleagues of DASIT S.p.A., who have collaborated on this paper, and also all external consultants. A particular t h a n k to Dr. Ghelli expert on Magnetic Nuclear Resonant device used for measurements and Prof. Adalberto Piazzoli of Pavia University, Department of Theoretic Nuclear Physics. A special t h a n k to Dr. Francesco Celani of INFN of Frascati for his useful criticisms.
References 1. S. Inutsuka and S. Araki, Plasma copper and zinc levels in patients with malignant tumours clinical evalutation of Cu/Zn ratio, Cancer 42, 626 (1978). 2. M. Hrgovic, C.T. Tessmer, T.H. Micnkler, B. Mosier, and G.M. Taylor, Serum copper levels in lymphoma and leukaemia special reference to Hodgkin's disease, Cancer 2 1 , 743 (1968). 3. S.N. Sinha and E.R. Gabrieli, Serum copper and zinc levels in various pathologic conditions, AJCP 45, 2156 (1980). 4. M. Kucharzewski, J. Braziewicz, U. Majewska, and S. Gozdz, Biol. Trace Element Res. 92(1), (2003). 5. H. Cunzhi, J. Jiexian, Z. Xianwen, G. Jingang, and H. Suling, Biol Trace Element Res. 91(2), 191-192 (2003). 6. J.F. Thomson, Biological Effects of Deuterium (Pergamon Press, Oxford, 1963).
T R A N S M U T A T I O N OF METAL AT LOW E N E R G Y IN A CONFINED PLASMA IN WATER
D . C I R I L L O A N D V. I O R I O Laboratorio M. Ruta - 81100 - Caserta, Italy E-mails: [email protected]; [email protected]
Energetic emissions have been observed from an electrolytic cell when tungsten electrodes are used to generate a confined plasma close to the cathode immersed an alkaline solution. In addition, energy generation has been observed, always close to the cathode, along with the appearance of new chemical elements in the experimental apparatus. These elements were not present in the cell before the experiment. This observation is proof of nuclear transmutations occurring within the cell. The results of this research and a theoretical model of the phenomenon were shown for the first time on April 18, 2004 during the second Grottammare (Ap) ONNE meeting in Italy.
1. Introduction The new cells described here produce many simultaneous interactions of a chemical and physical nature. Analysis of these events requires a multidisciplinary approach, and opens a complex and not yet completely understood nuclear mechanism. Due to this complexity, the mathematical model needs more study. 2. Cell Configuration The cell shown in Fig. 1 is made from a 350 ml Pyrex container surrounded by a jacket and having an open top. The jacket is evacuated using a vacuum pump in order to reduce thermal loss. On the top side of the cell is located a cylindrical shield made of polypropylene with a diameter of 13 cm. and a height of about 16 cm. A lid made of Plexiglass closes the cell top. The electrodes, a thermocouple and a mercury thermometer pass through holes in the lid. The electrodes are cylindrical rods with a diameter of 2.45 mm, and a length of 17.5 cm. Both are made of pure tungsten, with a combined volume of 3.8 cm 3 . The cathode is partially covered with a ceramic sleeve, which allows us to control the dimensions of the exposed cathode surface submerged in the reacting solution. Transducers are placed close to the cell and connected to various measuring instruments, consisting of a pyrometer and light-meter to measure the light variations occurring inside the cell, and a Geiger counter, to measure the radiant emission caused by nuclear events. We find that RF interference can cause incorrect readings. This will be discussed later. The cell is powered by a direct current power supply 492
493
Polypropylene parryspray Cathode
Anode
16 cm
Electrodes keeper
Pirex cell vessel
Figure 1.
14 cm
Configuration of the cell and position of the electrodes.
able to output a variable voltage from 0 to 340 V and a maximum current of 8 A. The electrolytic solution is potassium carbonate (K2CO3), 0.2M concentrated in 200 ml of ultra-pure water (double-distilled), which has a pH greater than 10. This solution is standardized with a volume of 200 ± 0.5 ml at 20°C. The solution is heated to 70°C so that an electrical conductivity of 12,000(is is obtained. This condition favors formation of a plasma and facilitates the nuclear events, as we will explain below. From a thermodynamic point of view, the cell is a non-adiabatic calorimeter, because it loses heat from the top, and constant pressure, because it is always in contact with the ambient atmosphere. Even a strong vapor emission is quickly dispersed without over-pressure generation. 3. Electrochemical Plasma Cell Working Conditions Application of the voltage causes H + to migrate to the cathode (the electrode that is at negative potential) and OH to migrate to the anode (the electrode at a positive potential). This ionic flux allows current to pass through the cell and produces
494
PC interface
T°C
i
i
VIP System 3
^f
Variac
A
TJ
Rectifier \ y ^hm
> o CM CM
0
^j™*
V
1'
£L_n
Cell
V
Figure 2.
General layout of the cell system.
hydrogen at the cathode and oxygen at the anode. The oxygen is produced through the ionic O H - discharge at the anode, and the hydrogen mainly through the direct discharge of the water molecule at the cathode, following the reactions: Cathode : Anode:
2H 2 0 + 2e" = H 2 + 20fT
2H 3 0+ + 2e~ -> H 2 + 2H 2 0.
40H~ = 2H 2 0 + 4e" + 0 2 .
The overall cathode reaction is strongly enhanced by the electrolytic. For example, the potassium ions (K + ) that are dissolved in the solution have a greater oxidation potential than hydrogen. The cathode reaction will last until all the hydrogen disappears from the solution. Simultaneously, the potassium ions will condense around the cathode, without depositing on it, thereby generating a screen with a positive potential that holds itself a few nm from the electrode. This peculiar configuration is similar to a cathode condenser in which the positive electrode is created by the potassium ions and the negative electrode is the cathode itself. In this situation, the dielectric is the double layer consisting of H^O^ and H 2 located between the two electrodes. In spite of this screen of potassium ions, ions of the hydrogen, being much smaller, will continue to discharge on the cathode without difficulty and generate gaseous hydrogen. (Hydrogen ions are so small, they are practically protons, in some ways.) Normal electrolysis occurs as long as applied voltage is around 50-80 V. As the voltage is increased on the order of 100 V, the amount of hydrogen generation
495
14
\
Figure 3.
Electrochemical plasma cell.
increases significantly. Eventually, so much hydrogen is being formed that it blocks the electrode. This causes the resistance of the cell to increase according to the equation i? ( T ) = R*^ [l+a(T-T0)j in which i? ( T ) is the actual electrical resistance, -R(To) is its value at 20°C, "a" is coefficient typical for tungsten (0.0045), and T is the temperature at which resistance is measured.
Typical current displacement in the cell Plasma ignition
Time (s)
IBlillillilii Figure 4.
Current displacement in our cell.
496
II
m
Double layer Figure 5.
Electronic representation of the double layer.
Tungsten (cathode)
Electrons
Photons
Discharge
Figure 6.
Describing the double layer during the ignition phase.
497
Figure 7.
Flux of the ions in the solution.
Once the region near the cathode acquires a sufficiently high resistance, the voltage drop between the potassium ion shield and the cathode can cause a plasma
Worm gas erosion
A
EHT = 20.00 kV WD = 20 mm
Figure 8.
Signal A = SE2 Photo No. = 301
Areas etched by hydrogen gas.
Date : 13 Jan 2004 Time : 17:01:43
498
Mag = 200 X
IUU
(im
Figure 9.
EHT = 20.00 kV WD = 19 mm
Signal A = In Lens Date : 13 Jan 2004 Photo No. = 299 Time : 16:51:48
Tungsten fusion area (after 4000 s).
to form, thereby forming a gaseous dielectric. The new condition can be represented with the equivalent circuit as shown in Fig. 5, where Z{ is the Faraday impedance. This plasma is unstable and will tend to be strongest where the voltage is greatest (see Fig. 6). The high local voltage is able to excite hydrogen and potassium ions to energies that result in optical emissions. In addition, the tungsten rod is heated to a temperature that produces electron and light emission. As a result, strong RF emissions are produced that can interferer with measurements if adequate shielding is not used.
Thermoelectronic emission Richardson & Dushman
_2> LU
1400 1200 1000 800 600 400 200 0 2800
3000
Figure 10.
3200
3400
3600
Tungsten thermoionic emission.
3800
4000
499
3226°C 100°C
100°C
Vaporization
area (cooling)
^—^ ,^_
Figure 11.
-Mh
HMh
•+•-*-•
0, 24 cm
View of the plasma heat transfer mechanism.
All together this phenomenon rises the cathode temperature close to 500°C, giving birth to an important consequence: the water in the solution, finding itself very close to the cathode, will evaporate instantaneously, generating a sort of vapor-sleeve. As a result, the electrical conduction mechanism in the cell changes. The region covered by plasma is much less involved in electrical conduction through the cell causing conduction to shift to the upper cooler part of the cathode, called "reaction band," where gaseous hydrogen continues to be produced, but hydrogen formation
w
1
Test W2 January - micro2
{ Re
Re
W
I Be s I
ww i Re | Re I
.' ! MO
N
W fe W f
Re
keV
/
0 1 2 3 4 5 6 7 Full scale 11869 cts Cursor: 7.253 keV (175 cts)
8
9
10
11
12
13
14
15
Figure 12. Analysis executed with an SEM on an area of the cathode surface after 4000 s of plasma—January 2004.
500
Os
V
Test W2 January 2004 - micro 10
Os
w
0 1 2 3 4 5 6 7 Full scale 3604 cts Cursor: 4.740 keV (189 cts) Figure 13. Analysis executed with an SEM on an area of the cathode surface after 4000 s of plasma—January 2004.
Figure 14. Analysis executed with an SEM on an area of the cathode surface after 4000 s of plasma—January 2004.
501
Un
I
,I
vM'w Wi
fc*
'lOO.OOM
200.00M
Figure 15.
k».ODM
4OQ.0OM
500.COM
600.00M
;i#'Wn.L J i I M - r 700.00M
MHz 800.00M
900.00M
Electromagnetic spectrum during plasma ignition.
is reduced. This causes the current to stabilize at about 1-1.5 A, as observed during the ignition phase (see Fig. 4). The limiting current value depends only on the ion concentration. This demonstrates that when the cathode surface is covered with the plasma, electrical conduction is drastically reduced and electrical potential lines are obliged to concentrate at colder areas, as shown in Fig. 7. Important to the process is the cathode ceramic sleeve, called "reaction chamber," which offers, thanks to its geometry, the correct electrical stability to the plasma. The internal diameter of the reaction chamber is larger than the cathode diameter by few millimeters.
II
w
AAA—A^A-L-vW '-A/yV R cathode(a) • R cathode(b)
V
R plasma
R anode
(Reaction band)
Figure 16.
Equivalent circuit of the cell during plasma phase.
502
Figures 8 and 9 (X-ray photos) show the tungsten surface after a good test of 4000 s. Figure 8 shows very little etching of the surface, while Fig. 9 shows areas where tungsten melted, indicating a temperature higher than 3400° C. Important to creating a model is the realization that temperatures in excess of 1000°C are produced, and they sometimes as high as 3400°C. Such temperatures generate thermionic emission, which must be considered. We propose that as the temperature increases, electrons in the metal start to oscillate in a coherent way. This oscillation is attracted toward the metal surface by the surrounding positive potassium ions. In addition, at temperatures close to 3400°C, thermonic emission can generate as much as 500 A from the heated part of the cathode (see Fig. 10). Therefore, a considerable number of electrons are available to the surface region. We believe this condition is important to initiating the observed transmutation reactions. 4. Experimental Evidence Once a stable plasma has been achieved for more than 500 s, we can compare the input energy, electrical power, with the quantity of energy necessary to warm up and evaporate the solution water. Omitted from this calculation is energy associated with chemical reactions; energy related to the heating-up and fusion of the tungsten; energy used in expanding gas and steam leaving the cell; energy lost by thermal and electromagnetic radiation; and loss of heat through the insulation. Even though this extra energy is omitted from the calculation, the cell is found to produce more energy than is being applied. If the energy needed to warm-up the electrolyte to 100°C and then produce evaporation is taken into account, values of output/input = 1.2-1.4 are obtained. Using a scanning electron microscope (SEM), the presence of rhenium, osmium, gold, hafnium, thulium, erbium, and ytterbium are found on the surface of the cathode. These elements were not previously in the apparatus (see Figs. 12-14). 5. Thermodynamic Problems and Output Energy Measurement The cell is heated mainly by resistive heating and by radiation from the plasma at the cathode. The following formula is used to calculate the energy resulting from these processes: Quscita = TOH2O {T2 - Ti) CPH2O + mv 539,55.
With TOH2O is the solution initial quantity (200 cm 3 ), cpn2o is the specific heat at constant pressure, m v is the amount of water lost by vaporization (539,55) is the heat of valorization given in cal/g, and (T2 — T\) is the initial and final temperature of the cell. This method gives a precision of ±250 cal. Additional factors must be taken into account, including splitting of water into its elemental components. This involves the following reaction, which removes energy from the system: H 2 0(1) -> H 2 (g) + 0.5O2(g) => +68,000cal/mol.
503
Energy is used to oxidize tungsten at the anode, as shown by the following reactions: W + 0 2 -> W0 2 (c) = -137,180cal/mol, W + 3 / 2 0 2 -> W0 3 (c) = -201,180cal/mol, W 0 3 -> 3 0 + W(l) = -203,140cal/mol. These reactions remove tungsten from the anode and enrich the solution with tungsten oxides. Being exothermic, these reactions add heat to the solution. However, the amount of energy contributed by these reactions is very small. Strong electromagnetic disturbances in the frequency range between kHz and hundreds of MHz are generated (see Fig. 15). These signals originate from the plasma in spite of the surrounding liquid. The cell can be analyzed as an electrical circuit shown in Fig. 16. C p is the tungsten-potassium virtual condenser and Lp is the plasma inductance. This equivalent circuit allows the oscillations that produce electromagnetic emissions to be analyzed. The equivalent circuit shows a cathode resistance made of two terms (Ra and R^), which provide most of the ohmic heating. The highlighted point by the arrow shows the area called "reaction band," which, as explained above, maintains the cell current once a plasma has formed. A complete analysis of the emitted electromagnetic spectrum should allow the energy generated at i? a and i?b to be determined. At the moment these data are still to be determined. The work of expansion has not been evaluated because the volume of gas has the "AV," which appears in the equation: -^(expansion)
-*
i i
'-
This equation gives the energy associated with expansion of the generated gases when the pressure, P, is fixed. The thermal losses from the system are approximately 25% of the input energy (Qinput)- This means that when 100 cal is applied to the cell, 75cal. will be transformed into heat to warm the solution and 25 cal will be lost to the environment through the insulation. 6. Conclusions The plasma is able to initiate transmutation reactions. Future studies are underway to understand the mechanism of these reactions. We propose that these reactions are the main source of measured excess energy. References 1. Ohmori, T. and T. Mizuno. Strong excess energy evolution, new element production, and electromagnetic wave and/or neutron emission in the light water electrolysis with a Tungsten cathode, in Proceedings of the Seventh International Conference on Cold Fusion (Vancouver, Canada; ENECO Inc., Salt Lake City, UT, 1998).
504 2. S.R. Little, H.E. Puthoff, and M.E. Little, Search for Excess Heat from a Pt Electrode Discharge in K2CO3-H2O and K2CO3-D2O Electrolytes, September 1998. 3. T. Ohmori and T. Mizuno, Nuclear transmutation reaction caused by light water electrolysis on tungsten cathode under incandescent conditions. Infinite Energy 5 (27), 34 (1999). 4. D.C. Borghi, D.C. Giori, A. Dall'Olio, Experimental Evidence for the Emission of Neutrons from Cold Hydrogen Plasma(CEN, Recife, Brazil, 1957), Unpublished. 5. R.A. Monti, Low energy nuclear reactions: Experimental evidence for the alpha extended model of the atom. J. New Energy 1 (3), 131 (1996). 6. R.A. Monti, Nuclear transmutation processes of lead, silver, thorium, uranium, in Proceedings of the Seventh International Conference on Cold Fusion (Vancouver, Canada; ENECO Inc., Salt Lake City, UT, 1998).
T H E C O N D I T I O N S A N D REALIZATION OF SELF-SIMILAR COULOMB COLLAPSE OF C O N D E N S E D TARGET A N D LOW-ENERGY LABORATORY N U C L E O S Y N T H E S I S
STANISLAV V. A D A M E N K O A N D V L A D I M I R I. V Y S O T S K I I Electrodynamics
Laboratory
"Proton-21",
Kiev,
Ukraine
V L A D I M I R I. V Y S O T S K I I Kiev Shevchenko
University,
Kiev,
Ukraine
The problem of the stability of condensed targets in particular and stability of "usual" atomic form of matter in general in relation to the process of self-squeezing up of the collapsed state is studied.
1. Introduction One of the fundamental quests of modern science is to achieve the collapse of an electron-nucleus system of matter, followed by nuclear transformation. Earlier, such a problem was considered only in connection with the global phenomena of astrophysics (gravitational collapse, formation of neutron stars, bursts of supernovas, etc.). Recently, it has been found 1 ^ 4 that the state of collapse can be realized under terrestrial conditions in a laboratory with an energy supply of at most 1 kJ. Of great importance is the fact that a macroscopic quantity of matter can be involved in the state of collapse (at least 1018 atoms) rather than two separate nuclei, as it is happening in accelerators with extremely high energies. Thorough studies 5 have shown that the phenomenon of global self-compression of matter can be related to the Coulomb collapse of an electron-nucleus system. The conditions for such a collapse can be fulfilled only when a macroscopic amount of matter is preliminarily compressed up to the critical density corresponding to a degenerate relativistic gas. It follows from calculations 5 that the minimum specific energy introduced into a compressible plasma should be 0.6-2 MeV/electron to ensure the conditions for a collapse. This condition can be naturally satisfied in the gravitational collapse of a heavy star, 6 but it is very difficult to realize a collapse in ordinary laboratory conditions by using the traditional methods of target compression. We consider two different methods of compression of matter up to the critical density. The first method is related to the use of a large pressure Pj = H^/8ir of an azimuthal magnetic field Hv = 2 J/Re, which appears in a micropinch system under impulse compression of the channel of a current J up to a radius R. The latter can be 505
506
determined from the equilibrium conditions of the kinetic pressure of the electron gas and Pj. Our estimates showed that, with regard to the inertial forces, the process of impulse compression of a micropinch could induce a state of degenerate relativistic electron gas with a density sufficient to start the collapse process. However, analysis shows that the collapse on the basis of a magnetic micropinch has a low efficiency, and the experimental results obtained cannot be explained in this framework. (1) Due to the low energy of the input electron beam (at most 1 kJ), the amount of compressed matter in the zone of action of a micropinch is also very small and does not exceed No « 10 15 electrons and nucleons. At the same time, we observe a nuclear transformation of matter in the amount more than N\ s=s 1020 nucleons in each of the experiments we performed. (2) A micropinch channel looks like a very thin (less than 1 A) long thread, whereas the zone of action of a collapse always corresponds in our experiments to a macroscopic sphere. (3) A considerable part of the products of nuclear transformations in the domain adjacent to the collapse zone is a cold condensed matter (solidified drops or monolithic layers mainly consisting of a single chemical element) rather than atoms and molecules randomly dispersed and distributed over the volume or the surface. We have developed the concept for a second method of forming a collapse which consists in that the initial state of collapse is formed in a thin spherical layer containing NQ neutralized electrons. 7 This layer is accelerated against the center of the target, rapidly increasing its velocity. While this layer moves in the undisturbed solid target, there occurs the compression of the ion (nuclear) components of matter, neutralization of the charge of the electrons, and formation of an electron-nucleus collapse on its leading edge. On the backside of the spherical layer running to the target center, there occurs the destruction of the electron-nucleus collapse, a partial restoration of the structure of the target, and the fast adiabatic cooling of the products of nuclear transformations, which is connected with this restoration. This explains the observed peculiarity of a localization of synthesized elements. This concept shows that the entire volume of matter (about Ni 3> NQ nucleons), through which the spherical plasma layer is compressed to the state of collapse is moving. It is also involved in the nuclear transformations process. The action of a collapse in the form of an extremely compressed thin running layer stops at the target center by the formation of a spherical collapse, its inertial confinement, a series of nuclear transformations, and a subsequent decay. Below, we will show for the first time that the realization of a non-stationary self-compression of a part of the target up to the state of collapse in the form of a spherical layer can be related to peculiarities of the interaction of the bounded system of quasi-free electrons with the ion matrix of a target. In this case, the formal start of the process does not require a preliminary supercritical action. The justification of the possibility and efficiency of such a process requires a detailed
507
analysis of peculiarities of the interaction of degenerate electron plasma with ions of a target. This analysis is as follows below.
2. Peculiarities of the Interaction of the Bounded System of a Degenerate Electron Gas with a Multiply Ionized Target Consider the process of interaction of the degenerate electron gas with a multiply ionized target. We assume that the action of an external perturbation leads to the ionization of a portion of the atoms in some closed domain of the condensed target (in particular, in a thin spherical layer near the surface of the target with spherical symmetry). Another variant can be connected with the introduction of a bounded part of the electron beam, which forms a running layer of electrons, in the target normal to its surface from outside. In this case, during a certain time interval (not exceeding the time of inverse recombination of electrons and ions), the target contains the free electron gas with density ne and the totality of partially ionized atoms (ions) neutralizing the charge of electrons. If the kinetic energy of the gas is less than the Fermi energy, then electrons and ions are connected in the limits of this system by the metallic bond. In this system, the energy of the electron-nucleus interaction is defined by the interaction of the degenerate electron Fermi gas with ions. The total energy of the electron subsystem of a Wigner-Seitz cell5 is the sum of Coulomb attraction and repulsion of electrons and the ion core J7eQL, energy of correlation C/corr, non-linear part of the full Coulomb potential energy (7eQNL, exchange interaction C/"e)exch in the system of electrons and kinetic (Fermi) energy UeF of the electron gas UeS = £4QL + t^corr + E^eQNL + E^e.exch + Uep = [^Q(en) + UCOII + W Q ( e e ) + ZmeC2]KF 2
= {Zmec 4
1 3
5 3 2
- (9/10)(4 7 r/3) / Z / e ny
+ t/^exch - ZmeC2
+ UeQNL
3
2
+ (e m/h ) (-0.115 + 0.031) ln[(e2m/H2)
{Air/Zf^Z1'3/nl'3}}KF
+[3(37r 2 ) 1 / 3 /4^]Ze 2 ny 3 - Zmec2 + [87rZ 7 / 3 e 4 (3/47r) 1 / 3 /7m e c 2 ]ne 2 / 3 ; PF
KF= [ (P2c2 + mYfl2V2 dp/^h^m^2.
(1)
o Figure 1 shows this energy versus the ion's charge (for ions with charges Z* = 1-4). Two main effects are observed as a function of the ionization multiplicity Z* of an atom: (1) A shift of the position of the minimum defining the stable state of this system toward higher electrons density of electrons (and, as a result, in the density of ions in the region). (2) A sharp increase in the potential well depth defining the position of a stable equilibrium of the system of electrons and ions of the relevant multiplicity.
508 50 40 30 20 B3
10 0 -10 -20 -30 cm-3
Figure 1. Interaction energy between ions with a low charge and degenerate electrons in one Wigner-Seitz cell.
It follows from the results derived that the stable minimum of this system depends on the multiplicity of an ion. In particular, for Z* = 1, we get ne(z*=i) ~ 10 23 cm~ 3 , which corresponds to a typical concentration of electrons under metallic binding. The equilibrium concentration of electrons increases with the ionization multiplicity: for Z* = 2-4, we get, respectively, ne(Z'=2) ~ 3 x 10 23 cm~ 3 , n e (z» =3 ) « 6 x 10 24 cm~ 3 , and n e ( Z , = 4 ) « 10 25 cm~ 3 . The same trend (the sharp shift of a position of the energy minimum and the increase in its depth) is seen if we take a higher degree of ionization, i.e., if Z* increases. For example, ne(.z*=26) ~ 3 x 10 26 cm~ 3 for iron, whereas n e(z*=92) ~ 4 x 10 2 T cm - 3 for the heaviest stable nucleus (uranium with Z = 92). Assume that we have created the system (in a target) with a particular degree of ionization Z*, but its density ne at the time of creation was less than the optimum value n e (^»). Because any non-equilibrium system relaxes to a stable state, we may expect the fast self-compression effect in the region under consideration, up to this optimum density. These deformations of a target under a change in the charge state of its electronnucleus system raise a question: is it possible to realize the process of chain ionization of a target? Such a process corresponds to the following situation. Upon the self-compression of the medium from an initial state with electron density n e to a stable state with electron density n^z*) > ne corresponding to a specific value of Z*, there occurs a deformation of ions of the medium which leads to an increase in the ionization multiplicity (Z* + AZ*) corresponding to a higher optimum density ™e(Z*+AZ*)-
It is obvious that if such an effect is possible in a specific condensed target, then the process of self-compression of this target acquires the avalanche-like character.
509
For this purpose, it is sufficient to create a relatively small initial ionization of the target (a small value of Z*). After this, the very medium begins to ionize itself to Z* + 1 and to compress itself to n e (z*+i)- Then the effect of the deformation will induce an increase in the ionization multiplicity up to Z* + 2 and in the density of electrons up torc.e(z*+2)>etc. As a result of this avalanche-like mutual stimulation of the processes of ionization and deformation, the charge state of the target will rapidly reach the characteristics which correspond to the maximum (full) ionization with Z* = Z, and the completely ionized target will be a plasma compressed to the maximum density n e (z)Simple estimates showed that, under "ordinary" conditions of a solid, such a process is impossible. To draw such a conclusion, it is sufficient to determine the density of electrons, at which the destruction of the next atomic shell and a collectivization of its electrons occur. This threshold can be determined from the condition, by which the external shell of any ion with charge Z* < Z is completely broken, when the ion density becomes equal to the threshold value n icr w 0.5Z*(mee2/h2)3 « 0.5 x 1025 Z* cm" 3 . 6 This value of n\ corresponds to the threshold electron density n e c r « Z* n; cr « 0.5 x 1025(Z*)2 c m - 3 . For the deepest levels of multiply ionized atoms with Z* ss Z > 70-80, the threshold density for the destruction of a shell is equal to necr ~ 10 Z* nj cr ~ 0.5 x 1026 (Z*)2 c m - 3 . These results are presented in Table 1. Table 1. Z*
1 3
n e ( Z . ) , c m " (stable state of ion system with Z*) riecr(Z'), c m " 3 (threshold for destruction of the next atomic shell and formation of ion with Z* + 1)
10
2 23
2 x 10 2 6
3 X 10
3 23
5 x 10 2 5
6 X 10
4 24
8 x 10 2 5
10
26 2s
10 2 6
92 26
4 X 10 2 7
3 x 10 2 7
4 x 10 2 9
3 X 10
These estimates indicate that the concentration of electrons ne(z*) m the ionized matter, which corresponds to a stable state of an ion with charge Z*, is much less than the critical concentration of electrons neCr(z*)i a t which ions with a greater charge Z* + 1 are formed due to the self-compression of the metallic matrix. This result might be expected, because, otherwise, any metal would be extremely unstable. Indeed, the initial action of any arbitrary small input deformation would be sufficient to convert a metal into completely ionized super-dense electron-ion degenerate plasma by the process of self-compression. The analysis shows that, despite the clear conclusion, it is not final because it was drawn under certain conditions. In particular, the equilibrium condition presented above characterizes the state of the Fermi gas with zero mean momentum of electrons (though the square mean momentum turns out to be very large in this case). In the static case, this condition corresponds to only one stable state. It
510
is easy to verify that, in dynamical systems (in the presence of a non-zero mean momentum of the drift movement), one can control this condition and, hence, ensure the fulfillment of the condition of instability of a metal relative to the process of self-compression and the process of transformation of any material into a completely ionized electron-nucleus plasma! Consider the following model: a degenerate electron gas has density ne. If the nuclei neutralizing this gas are in the maximally stable (ordered) state, then a quasicontinuous distribution of momenta and energy in every Wigner-Seitz cell is set by the Fermi distribution with a definite limiting momentum pp. What happens if the motion of all the electrons will be defined by a simultaneous combination of values of the quasi-continuously distributed momenta, whose direction and magnitude correspond to a degenerate Fermi gas, and the drift momentum po = 7mv 0 ? In the co-moving (moving with drift velocity v 0 ) coordinate system, electrons are distributed in such a way that they fill all the energy levels from p = 0 to P F = P o > (3TT2/IV)1/3. Let us consider the case of a threshold drift pulse po > (37r2fi.3ne)1/3. In the laboratory coordinate system, the momenta of degenerate electrons in the scope of the Fermi layer App(9,ip,po) are distributed in the interval from po(0,ip) — App(6,ip,po)/2 to po(9,(p) + App(0,
Jd3p/(2Trh)3
2TT
-K
po(e,(p)+ApF(6,ip,p0)/2
= 2V fdap /sintfdtf 0
0
p2dp/(2irh)3.
/
(2)
p o (0,cp)-Ap F (0, V ,p o )/2
Consider the process of symmetric radial compression of a spherical layer with volume V = NOVQ, which includes NQ nuclei and Np = ZNQ electrons. Here, Vo = V/NQ is the volume of a Wigner-Seitz cell. In this case, the electrons in the volume of the spherical layer have, besides randomly oriented Fermi components of their momenta, the ordered radial component of the momentum p 0 = 7mv 0 e r , which is directed to the center of the system and is identical for all spatial angles 9 a n d
The formula for the total number of states Np = ZNQ in a compressed spherical layer with volume V is as follows: 27r
-K
7VF = 2V f dip /sintf dtf 0
0
Po+ApF(po)/2
/
p2 dp/(2nh)3
p 0 -Ap P (po)/2
2
= N0V0[p 0ApF(p0) + (App(p0))3/12]/ir2h3.
(3)
From this formula we derive the formula for the limiting momentum: PF(PO)=PO + APF(PO)A
(4)
511
PF(PO)
= {(^2h3ne) + [(67r2fi3ne)2 + Mp*]1'2}1'3 +{(67r2fi3ne) - [(6ir2h3ne)2 + 64pg]1/2}V3.
Consider two extreme cases (a small or large drift velocity). In the case where the drift pulse po is approximately equal to ApF(p0)/2 Po > {3ir2h3ne)ll3), relation (5) yields: pF = {^2)l'3hnlJ3
+ p3/3(37r2)2/3h2n2J3.
(5)
(i.e.,
(6)
This value of pF corresponds to the limiting (Fermi) energy: EF = Pp/2m = (37r 2 ) 2 / 3 /i 2 n 2/3 (l + 2p3/9ir2h3ne)/2m,
(7)
for a non-relativistic degenerate electron gas and to EF = pFc = {^2)1/3hcnl'3{l
+ pl/9-K2h3ne),
(8)
for an ultra-relativistic gas. In the other extreme case (for a very large drift pulse po S> (37r2ft3ne)1^3), relation (9) yields = Po[l + 7r2h3ne/2p3].
PF{PO)
(9)
This value of pF corresponds to the Fermi energy EF =
PFc
= p0c[l + (37r2)fi3ne/3pg],
(10)
for an ultra-relativistic gas. The total kinetic energy of all electrons in the volume of one cell is Po+Ap F (p 0 )/2
UeF =
(V0/n2h3)[(p2c2
I
+ my)1'2
- mec2]p2 dp
po-ApF(p0)/2
= Zmec2[KF(Pl,p2)-l}.
(11)
Here po+Ap F (p 0 )/2
KF(Pl,p2)=
{V0/Zmec2ir2h3){p2c2
J
+
mlcy2p2dp
po-ApF(p0)/2
= (m3ec3
/8Tr2h3ne){{(p2/mec)[2(p2/mec)2
+l][(p 2 /m e c) 2 + I}1'2 - Arsh(p 2 /m e c)} -{(Pl/mec)[2(Pl/mec)2
+ l][( P l /m e c) 2 + l}1'2
-Arsh(pi/m e c)}}; p%l = p0 ± ApF(p0)/2.
(12)
The presence of the ordered radial (drift) momentum also changes the value of the exchange energy of a degenerate electron gas, 5 which is described in this case as follows:
512 Po+Ap F (p 0 )/2
u,e,exch
2 2
~(4nZh e /ne)
f
d3Pl/(2-Kh)3
po-ApF(p0)/2 po+Ap F (p 0 )/2
x
J
d3p2/(2nh)3\p1-p2\2
po-Ap F (po)/2
= -(Ze2/4n3h4ne){[(p0
+ ApF(p0)/2)4
-(4/3)(po - ApF(p0)/2)[(p0
- (p0 -
+ APF(Po)/2f
ApF(p0)/2)4}
- (po -
ApF(p0)/2)3}}.
This shows that the exchange energy decreases with increasing drift momentum po, and its effect is small during very fast movement.
cm Figure 2. Numerical analysis of the change in the total energy of a degenerate electron gas for the low charges of ions Z* as a function of the kinetic energy of the drift motion of the electrons .EK in one Wigner-Seitz cell.
In Fig. 2, we show the results of a numerical analysis of the change in the total energy of a degenerate electron gas for the same charges of ions Z* as a function of the kinetic energy of the drift motion of the electrons EK = (PQC2 + m2cA)1/2 — mec2. These results are obtained on the basis of the general formula (1) modified with regards to the dependence of the result (11) on the drift momentum p0. It is seen from Fig. 2 that, already for a relatively small drift motion with an energy EK = 5keV, the energy minimum (the position of a stable state of the electron-ion system) shifts from n e (^« =2 ) « 3 x 10 2 3 cm - 3 , ne(z*=3) ^ 6 x 10 24 cm~ 3 , n e (z* = 4) ~ 1 0 2 5 c m - 3 characteristic of a static degenerate gas of electrons to n e ( Z » =2 ) ~ 4 x 10 25 cm~ 3 , n e ( Z . = 3 ) « 8 x 10 25 cm~ 3 ,
513
ne(z*=4) ~ 1-3 x 10 26 cm~ 3 which are 15-100 times more than those without drift motion, and approximately correspond to or even exceed the critical density, at which the collectivization of the next electron level of an ion occurs. Respectively, at the higher energies of drift motion (in this case, at EK = 50keV), the positions of the minima shift to the values ne(Z*=2) ~ 4 x 10 26 cm~ 3 , n e ( Z . = 3 ) « 6 x 10 26 cm~ 3 , ne(Z*=i) ~ 1 0 2 r c m - 3 which are much more than the threshold of destruction of the next (deeper) electron state. At such energy of drift motion of electrons, the avalanche-like ionization of atoms of the target and the avalanche-like self-compression of the target will occur. It is natural that the same effect will be observed for heavy atoms. In Figs. 3 and 4, we give the results of calculations of the total energy of interaction of ions of a copper target with the degenerate electron gas moving across the target with the drift velocity corresponding to the energy of drift motion £ K - In Fig. 3, we present the case of a relatively small energy _EK (lOkeV < £"K < 100 keV), whereas Fig. 4 shows the results of analysis for the greater interval (0.05 MeV < E^ < 3 MeV) of values of the kinetic energy EK of drift motion.
0.5
1.0
1.5
2.0
1028
cm -3 Figure 3. The total energy of the interaction of ions of a copper target with the degenerate electron gas moving across the target with the drift velocity corresponding to the energy of drift motion EK (lOkeV < EK < 100keV).
It follows from Fig. 3 that the increase in the drift energy leads to a continuous shift of the position and depth of the minimum of the total interaction energy. It is seen that, in the region of non-relativistic drift velocities, there exists a linear dependence between the equilibrium electron density ne defined by the position of the energy minimum Ues/Z and the drift motion energy EK (and also by the square drift velocity v2 = (dR/dt)2: ne/Ex = const. = (3z- It follows from this dependence that ne = {2(ii/me)v2 = cez(dR/dt)2. An analogous dependence holds
514 2.5 2
Cu target
E«(MeV): 0;0.05; 0.5; 1.0;1.5; 2.0; 2.5; 3.0
1.5 >•
1
N 0-5 0 0.5 -1 1.5 10*
10'
10'
iff9 cm
10d
10',32
10',33
-
Figure 4. The total energy of the interaction of ions of a copper target with the degenerate electron gas moving across the target with the drift velocity corresponding to the energy of drift motion EK (0.05 MeV < EK < 3MeV).
for other metals. In particular, the approximation coefficient for Cu derived from this calculation is a c u « 0.6 x 10 8 s 2 /cm 5 . Another important parameter is the depth of the potential well characterizing the total specific energy of interaction Ues/Z. The performed analysis yields that the latter increases approximately proportionally to the cube root of the drift energy \Uev/Z\~(EKy/3, in the region of non-relativistic energies and is described by the approximation formula Ue%/Z = —b {dR/dt)2/3. For a Cu target, the approximation coefficient is b w 3 x 10 _ 1 5 gcm 4 / 3 /s 4 / / 3 . The analysis of the behavior of the specific binding energy Ue-^/Z for relativistic drift energies (see, e.g., Fig. 4) gives the dependence Uex/Z = —kEa- For a Cu target, k « 1/6. When the density of a degenerate electron gas becomes higher than the equilibrium electron density ne(z), the system energy increases, at first, sharply. But, after achievement of the threshold density necr « 1Q36Z~2 c m - 3 , the energy of the system begins to irreversibly decrease, which corresponds to the state of collapse and the process of electrons falling on the nucleus. An analogous situation is considered in Fig. 4. However, at a very high energy E-& of drift motion in a degenerate electron gas, the situation is different. In the case where the position of a minimum ne(z) approaches the threshold density of a degenerate electron gas n e c r ~ 1036Z~2 cm~ 3 with increase in the drift motion energy EK, the behavior of the total interaction energy Wes changes fundamentally. As ne —> n e c r , we observe a very rapid and unbounded decrease in WeY. instead of its increase. The consequence of such a decrease in the interaction energy Wex is the irreversible collapse of the
515
electron-nucleus system which begins, in fact, at a small density of the electron gas and proceeds without any action of a potential barrier preventing or decelerating the collapse. The condition of such a mode of irreversible self-compression of a copper target requires that the kinetic energy of the drift motion be more than EK ~ 2 MeV. For targets made of atoms heavier or lighter than Cu, the threshold kinetic energy of drift motion will be, respectively, less or more than EK « 2 MeV. In particular, EK ~ 1 MeV for a target containing uranium, and EK ~ 6 MeV for a target containing aluminum. As was shown in work,5 such a Coulomb collapse of the electron-nucleus system causes an increase in the binding energy of this system and induces a possibility to realize the energy-gain synthesis of heavy and super-heavy nuclei with A > 300. It was also shown in that work that the practically complete screening of the charge of nuclei in the extremely compressed relativistic degenerate gas of electrons suppresses the action of a Coulomb barrier and accelerates the reactions of synthesis of heavy and super-heavy nuclei.
3. Surface Energy and Peculiarities of Motion of a Bounded System of the Degenerate Electron Gas in a Condensed Target The interrelation discussed above between the kinetic energy of drift motion and the possibility of a collapse of the electron-nucleus system raised the following question: can the bounded spatial system of the degenerate electron gas accelerate itself in the condensed medium up to such an energy, at which the conditions for the formation of a barrier less electron-nucleus collapse are fulfilled? Consider peculiarities of the manifestation of the surface energy on the boundary of a degenerate electron gas, in which the ordered ion lattice is positioned. The main condition for the stable existence of a neutralized degenerate electron gas is its equilibrium relative to the action of Coulomb forces of the interaction between electrons and ions and of Fermi forces defining the kinetic pressure. This condition defines the requirement of minimization of the volume occupied by the degenerate gas and is reduced to the condition of equality of the pressures caused by these forces (|df7eQi,/dVb| = |dC/ej^/dVb|) on both the surface of a Wigner-Seitz cell and the external surface of the whole region which contains the gas of degenerate electrons. Next by importance is the account of forces defining a form of the surface of the region containing the degenerate electron gas. If this form deviates from the spherical, the surface of the region is subjected to the action of a compressing pressure, which is analogous to surface tension and tends to decrease the surface area. We can find this pressure by using formula (1) for the total binding energy Ue-z/Z modified with regard for the effect of the drift movement of electrons to the center of the target.
516
For a spherical layer with volume V, the total binding energy is {UeT./Z)Vne. With the use of the above-derived approximation dependence Ues/Z ss —b (dR/dt)2/3, we obtain the total pressure on the plasma layer surface as Ps = Uevm « -b(dR/dt)2'3ne.
(13)
We note two main consequences of the action of the force of surface tension. It tends to minimize the area of a region containing a degenerate gas of electrons with the constant volume of this region. Because an analogous pressure will act from all the sides, the external surface of the system will try to finally take the form of a sphere. Under the action of the same force, the thin spherical layer will begin to decrease its area by moving towards the center of the target. Consider the result of the action of this force in the case where the gas of degenerate electrons occupies a volume in the form of a thin concentric spherical layer between two concentric spheres with radii R and R — AR (Fig. 3). Both surfaces (internal and external) are subjected to the action of the same pressure PeQ directed normally to the surface inward the layer. Due to the difference of the areas of the internal and external surfaces, the total (resulting) force F E = ~{A-KR2PJ:
- 4n(R - Ai?) 2 P s } sa -SwRARP^,
(14)
acts on the whole spherical layer and is directed to the center of symmetry of this layer, i.e., to the geometric center of the sphere. Under its action, the spherical layer with high density of degenerate electrons with a total mass of M e E = 4irR2ARmene will move to the center. The equation describing a radial non-relativistic motion of the spherical layer is d2R/dt2
= F E / M e E = -2b(dR/dt)2/3/Rme.
(15)
This non-linear equation is valid as long as the velocity of the squeezing ring of electrons remains non-relativistic. If we multiply both sides of this equation by (dR/dt)1/3, we can easily find the dependence of the actual velocity of motion dR/dt of the squeezing plasma layer on its radius R d{(dR/dt)i/3}/dt
= -(86/3m e )
With regard for the initial conditions dR/dt\t=o dR/dt = -{vl/z
(dR/dt)/R.
= VQ and i?|t=o = -Ro> we get
+ (86/3m e ) \n(R0/R)}3/4.
(16)
For a target made of copper, we obtain dR/dt = - K
/ 3
+ 10 13 {ln(i? 0 /i?)}} 3/4 , cm/s.
(17)
It is seen that, for RQ/R > 2.7, the radial velocity of compression of the plasma layer (even for v0 = 0) approaches the velocity of light (|di?/di| > 6.109 cm/s), and the correct description of the process of compression requires the use of a relativistic equation of motion.
517
Consider another limiting case that corresponds to the motion of a compressed plasma layer with a very high density of electrons (and, respectively, a high-local density of ions). Such a mode of compression corresponds to a relativistic gas of degenerate electrons. The relativistic equation of motion for this layer is d p s / d t = F s «-87r J RAi?P s ,
VK-C.
(18)
Here p E = jM-seV « Air~/R2ARmenec (19) is the total relativistic momentum of the squeezing layer, 7 - Lorentz-factor of moving relativistic electrons, Pg « (UeY,/Z)ne m —kE^ne - surface pressure of the relativistic degenerate gas, EK = jmec2. With regards to the fact that, for relativistic particles with 7 > 1 , their velocity remains almost constant and equal to c, the equation of motion for the plasma layer is reduced to the equation for the Lorentz-factor. Using the expression Rm RQ — ct we find the solutions of the equation of motion dj/dt
« -2kEk/Rmec
= -2kjc/(Ro
- ct)
with regards to the initial conditions (7(4 = t 0 ) = 7o 3> 1, R(t = to) = (i?0 — cto) for t = io) a s 7 (i)
« 7(*o)[(i?o - ct0)/(R0
- ct)}2k « 7(*o)[(iio - ct0)/(R0 EK{t)=y(t)mec2.
- ct)]l'\
(20) (21)
As soon as the energy of longitudinal (drift) movement of the annular plasma layer reaches the threshold value E^, the irreversible collapse of the electron-nucleus system occurs. The process of compression of a spherical electron layer is presented symbolically in Fig. 5. It follows from these estimates that the time Ai2 of passage of the compressed spherical plasma layer across the place of position of any nucleus in the matrix turns out to be sufficiently large to ensure the displacement of this nucleus for the time At\ to a new position which corresponds to the formation, for a short time, of a super-dense medium with the density of ions n; = ne/Z in the volume of the running self-compressing spherical layer. 4. Conclusion The peculiarities of the motion of a thin closed plasma layer with low density in the volume of a condensed target show that such a layer is squeezed with high velocity to the center of the target, by simultaneously ionizing the material of the target in its volume and by rapidly increasing its density. Because the main source of the motion of the layer is the force of surface tension of the bounded region containing the neutralized degenerate electron gas, the external and internal surfaces of this
518 AR(R)
J-JL
I I 1 1 I Nuclei in the matrix
I
Electron gas in the matrix
Hill A m
J—J
Squeezing electron gas in the | volume of a running plasma layer
•BHH\
Nuclei in the volume of a running plasma layer
Figure 5.
Consecutive phases of the compression of the running self-compressing spherical layer.
layer acquire rapidly the ideal spherical form. The linear velocity of motion of the plasma spherical layer can be close to the light velocity at the last stage of the compression. The density of the electron component of the plasma layer scanning the target corresponds at this stage to a relativistic degenerate gas, which makes it possible to realize the state of Coulomb collapse of electrons and nuclei, screening the charges of nuclei, and ensuring the nuclear synthesis. If the density of the degenerate gas of electrons exceeds the threshold value, a rapid synthesis of heavy and anomalous nuclei becomes possible in the scope of the plasma layer. Peculiarities of the interaction of the scanning plasma layer with atoms of the target are defined by a number of successive processes: the complete ionization of the medium at the leading edge of the layer; the compression of the nuclear component in the volume of the layer up to the equilibrium density leading to charge neutralization of the electron component and the formation of the state of electron-nucleus collapse with release of the binding energy, the cascade of nuclear transformations in the collapse zone, and the decay of this collapse immediately after the back front of the plasma layer. A part of the binding energy of the electron-nucleus system, which is released in the process of formation of the collapse, can lead to the additional acceleration of the scanning plasma layer. During the process of formation of the state of collapse, there occurs all the complex of nuclear transformations, whose products remain then near the place of their creation and correspond to a local position of the collapsing plasma layer. The decay of a compressed state of the electron-nucleus plasma with relaxation to a "normal" uncompressed state of the target matrix after the passage of the scanning wave of the super-dense gas of electrons is an endothermic process,
519
and leads to the cooling and localization of a part of heavy products of the nuclear transformations. In the central part of the target, there occurs the shock squeezing of the scanning plasma layer and the formation of the zone of spherical collapse. It is obvious that, in this region, the most essential nuclear transformations occur (including the synthesis of super-heavy nuclei), along with the emission of large amounts of energy (probably in the form of hard gamma-quanta and neutrinos). After the termination of the action of the inertial forces, there occur the irreversible destruction of the spherical collapse zone and the outburst of products of the nuclear transformations into the environment. In the future, we intend to carry out a more detailed study of peculiarities of the running of collective nuclear reactions in both the zone of the scanning ion layer and the central zone of a spherical collapse. The scenario presented above, despite the need for further refinement, explains the majority of results of many experiments with shock compression of matter and the synthesis of heavy, super-heavy, and anomalous isotopes and elements. It is assumed that only such a mechanism of synthesis explains the creation of stable super-heavy and other anomalous nuclei, the process of deactivation of any kinds of radioactivity in the collapse zone and creation of additional energy Q = 10 2 ... 105 Qo (in relation to the energy of driver Qo) observed in the experiments carried out at the Electrodynamics Laboratory "Proton-21." During the years 2000-2004, more then 10,000 experiments on super-pressing to a collapse state of monoatomic solid density targets by a special electron driver were carried out in Kiev Electrodynamics laboratory "Proton-21." Investigations were carried out at different coherent exposure conditions with various targets of controlled composition, made of light, medium and heavy elements with 12 < A < 210. All together, more than 20,000 element and isotope mass-spectroscope analyses of the targets were performed, including the following: EPMA, LMS, AES, SIMS, TIMS, and RBS. In all these experiments several types of anomalous phenomena were observed: (1) Fusion of light, media and heavy chemical elements (at 1 < A < 240) with abnormal isotopic ratios. In the majority of the newly formed chemical elements, we observed a significant deviation from the normal isotope ratio. For many elements, this ratio is changed by 5-100 times (it can increase or decrease). (2) Fusion of super-heavy transuranium elements (about 10 14 -10 15 super-heavy nuclei with A > 270 were created in each of the performed experiments). Most frequently are registered the super-heavy nuclei with A = 271, 272, 330, 341, 343, 394, and 433. (3) All created elements and isotopes (including super-heavy ones) were stable or quasi-stable. (4) Transmutation of any radioactive targets to stable-nucleus states in the collapse zone. The utilization efficiency of radionuclides per 1 kJ of the
520
driver energy corresponds to the t r a n s m u t a t i o n of about 10 1 8 radioactive target nuclei of any kind (e.g., 6 0 C o , 1 3 7 Cs) into non-radioactive (stable) isotopes of different nuclei. These phenomena can probably b e interpreted on the basis of t h e main common idea: creation and evolution of a self-organized and self-supported collapse of electron-nuclear plasma of initial solid-state density under the action of focusing electron driver, u p to a state of large non-stationary electron-nuclear clusters, with density close to t h a t of a nuclear substance.
References 1. S. Adamenko and V. Vysotskii, New projects and lines of research in nuclear physics (World Scientific, NY, 2002), pp. 383-391. 2. S. Adamenko and A. Adamenko, New projects and lines of research in nuclear physics, in Proceedings of International Symposium (World Scientific, NY, 2002), pp. 33-44. 3. S. Adamenko and A. Shvedov, New projects and lines of research in nuclear physics, in Proceedings of International Symposium (World Scientific, NY, 2002), pp. 355-361. 4. S. Adamenko, Visnyk NANU, Bull. Natl. Acad. Sci. Ukraine 2, 23-26 (2003). 5. S.V. Adamenko and V.I. Vysotskii, Found. Phys. Lett. 17(3), 203-233 (2004). 6. D.A. Kirzhnits, Soviet Phys. Uspekhi 104(3), 493 (1971). 7. S.V. Adamenko and V.I.Vysotskii, Found. Phys. 34(11), 1801-1831 (2004).
T H E SPATIAL S T R U C T U R E OF WATER A N D T H E P R O B L E M OF CONTROLLED LOW-ENERGY N U C L E A R R E A C T I O N S IN WATER M A T R I X
VLADIMIR I. VYSOTSKII Kiev Shevchenko University, Kiev, Ukraine ALLA A. KORNILOVA Moscow State University, Moscow, Russia
1. I n t r o d u c t i o n Ordinary water has a number of unique features, among which there are its stable spatial structure and long-term "memory." Numerous experiments confirm the existence of water memory, which is activated under the influence of various physical fields (e.g., magnetic field, mechanical impact, abrupt temperature, or pressure change) and may store information about such influence for many hours and days. Such activated water has altered physical and chemical (including biochemical) features. An increasing number of reliable experiments show that the continuous model is inadequate for describing the water structure. At the first glance, it appears that water, as a specific physico-molecular object, cannot have any long-term memory. It follows from simple estimates. For a long time, the continuous (quasi-crystalline) model of water was the dominant one. Within the framework of this model the spatial structure of potential energy for each one of H2O molecules is nearly a periodical three-dimensional system of pits and barriers. This relief is the result of a self-regulating movement of all water molecules, which represents a combination of two independent processes vibration movement in each one of potential pits and random (fluctuation) leap into a neighboring pit. The average frequency of vibrations in potential pits is approximately the same as the Debay frequency in a solid body (about WD ~ 10 1 3 s~ 1 ). The average duration of a leap into a neighboring potential pit is equal TO « 10~ 13 s. The average time of staying in one pit W=roexp(f)
« 1 0 " ° - lO""* s
(1)
is determined by the water temperature T and the energy of activation AW s=s 0.2 eV of the diffusion process (the height of the barrier between neighboring pits). Staying within the framework of this model it is easy to reach the conclusion that water 521
522
memory must be preserved for not much longer than the value (t), which is by many orders less than given in many experiments. There can be only two ways out of this logical dead end: either the experiments are not reliable, or the continuous model is incomplete (or wrong). 2. The Problem and the Possible Mechanism of the Water "Memory" An increasing number of reliable experiments show that the continuous model is inadequate for describing the water structure. More detailed studies have shown that the so-called "clathrate" model is the one closest to reality. In its final form this model was developed by Pauling (1959). * On the basis of the Pauling model there is the concept that unification of atoms of oxygen and hydrogen can create spatial flexible tetrahedral frames. Formation of a tetrahedral frame was due to the fact that the natural spatial angle between OH-links in a free water molecule H2O is equal to 104.5°, which is sufficiently close to the exact value of the tetrahedral angle 108°. In order to achieve an additional angle of 3.5° in this link an insignificant energy would be required, while the existence of an additional curve would considerably increase rigidity of the crystalline frame (a similar situation occurs, e.g., in pure construction material as preliminary stressed concrete). In the joints of the crystalline frame there are very large (in the scale of a water molecule) microcavities (microscopic empty spaces) with rigid atomic walls. The main elements of this structure are right polyhedrons linked to each other dodecahedrons. Such systems are called "clathrate hydrates." The entire frame is held together by hydrogen links. They fasten together a system of pentagonal dodecahedronic polyhedrons from ions of oxygen and hydrogen, which form the walls of the microcavities. Each one of the polyhedrons may be characterized by an inscribed sphere with a radius of about _RC w 2.6 A. All polyhedrons have 12 pentagonal facets, 30 edges connecting these facets and 20 vertexes with three edges converging in each one of them. At the vertexes of these polyhedrons, three are 20 molecules of water, H2O, each one having three hydrogen links. Any three polyhedrons may be unified into stable associates containing 57 molecules of water. Out of these 57 molecules, 17 have fully saturated hydrogen links and they form a tetrahedral hydrophobic central frame, while in four dodecahedrons there are 10 centers of formation of hydrogen links (O-H or O) located on the surface of each one. The space structure of the system of clathrate hydrates in water is presented in Fig. 1. Beyond this frame, there are quasi-free molecules of "regular" isotropic water, the features and the structure of them approximately match the continuous model. Microcavities are linked to the outer space by windows with diameter of about 2.5 A, which is slightly less than diameter of a water molecule {2Rw sa 2.76 A). As a result, each of the microcavities is separated from "external" amorphous quasi-free water by a circular potential barrier with width about 0.13-0.15 Abounding each window.
523
Figure 1.
The system of clathrate hydrates in water.
The relative quantity of molecules of "frame" water at room temperature is 20-30%, increasing at lower temperatures. The volume of these microcavities may be large enough to hold one molecule of H2O, CH 4 , O2, or N 2 . Due to the presence of a strong and symmetrical electrostatic field (symmetrical relative the center of microcavities), there is a certain ban on the formation of hydrogen links of water molecules with the walls inside the microcavities. In this case there is such a non-trivial phenomenon as repulsion of free water molecules from the walls of the frame also consisting of water molecules. (In other words, water molecules in the volume of water become hydrophobic!) The average density of a clathrate frame (without filling it up with water molecules) equals 0.80 g/cm 3 , i.e., the microcavities occupy 20% of the full volume of a structured water frame. If the microcavities are saturated with molecules of water the density of water would be close to l g / c m 3 . We shall demonstrate how the presence of a clathrate frame of water may lead to formation of long-term memory in it, and to recording and using information.2 Let us examine initial water in the state of thermodynamic balance with a certain temperature T. This condition is distinguished by maximal entropy. Such water is obtained by long boiling and slow cooling down, or by a very long-term storage. In this case the number of microcavities within the system of clathrate hydrates filled with water matches the Bolzman distribution accounting for statistical weights of H2O molecules' condition in microcavities and in amorphous water. It would be balanced or regular water. At the temperature of 4°C, 18% of all microcavities are filled with water. At normal body temperature (36.6°C) 38% of microcavities are filled, while at 55°C about 50% of microcavities will be occupied by H2O molecules. This pattern of distribution is related to several factors: (1) the Bolzman distribution at a given temperature,
524
(2) the repetition factor of degeneration of the initial and final state of an H 2 0 molecule in amorphous water near an entry window into the volume of a microcavity and inside it, (3) the ratio of the volume of all amorphous water and the volume of a clathrate frame. With changing temperature all three values change, which makes exact calculations of the dynamics of occupation of microcavities more difficult. However, it is obvious that in the volume of clathrate microcavities the energy of molecular links is close to zero (due to hydrophobic nature of interaction with the walls), while condition of an H2O molecule in the volume of quasi-amorphous water is determined by the depth of a potential pit, dictated by links with other water molecules. The depth of that pit corresponds to the energy of activation at diffusion AW ss 0.2 eV, which, in effect, reduces the level of energy of an H2O molecule with respect to condition of the same molecule in the clathrate frame by the value of AW. For these reasons, it becomes clear that the necessary activation energy to entering a microcavity AEu, and exit from it AEM — AE, would be different (Fig. 2).
(a)
t
(b)
A
f
May
Clathrate microcavity
W^ m Free molecules of D2O water
4' 2R j
(c) Potential energy of H 2 0 (D2O) molecule in clathrate microcavity
Direction of activation
Potential energy of H2O molecule in free (amorphous) water
Figure 2. Process of thermally stimulated activation (a) and deactivation (b) of microcavities of a clathrate water frame at increasing and decreasing temperatures, (c) structure of potential energy of molecules of amorphous and linked water in the volume of a clathrate microcavity and around its boundaries.
Based on this, the time that an "extra" molecule of water would stay in a microcavity and the time an "extra" vacancy in an empty microcavity exists would also be different.
525
With a violation of thermodynamic balance a redistribution of H2O molecules between amorphous water and microcavities takes place until a new balanced state is achieved. We shall demonstrate that a spontaneous transfer between these states is substantially inhibited due to the very small probability of tunnel penetration of H2O molecules through "narrow" windows, and the time of existence of each of these conditions turns out to be very long. We shall determine the time of relaxation in such a redistribution. Such relaxation corresponds to a transfer of water molecules in two possible directions: (a) from the state of amorphous water into the volume of a microcavity (if the initial number of water molecules in microcavities was smaller than the value of a variable determined by the Bolzman distribution, which may happen in case of a rapid heating of water); (b) from the state of "excess" water in microcavities to amorphous water (if the number of water molecules in microcavities exceeded the value for balanced state, which, e.g., corresponds to the case of a rapid cooling down of water). The process of relaxation of each of these states depends on thermodynamic probability:
" - " ( = & )
(2)
that one of the water molecules after its interaction with other molecules will receive energy AEM sufficient for short-term deformation (i.e., work on increasing energy of interaction between a proton and an ion of oxygen), which would be enough for a reduction of the water molecule's size to the dimensions of a window of a microcavity and, correspondingly, penetration of that molecule inside the microcavity. Since the frequency of collisions of a water molecule with the surface of any structured object in water is equal to the frequency of vibrations of molecules around a local position of balance WQ ~ 1/TO ~ 10 13 s _ 1 , the total probability of capturing a molecule in a unit of time into an empty microcavity is equal to F = W/TQ. From this expression, we can determine the average lifetime of an unbalanced (empty) state of a single microcavity in the volume of a spatial tetrahedral water frame (time of relaxation of a vacant spot in a microcavity):
^-jf-"""^)-
(3)
Plainly that time will determine the duration of water memory before the microcavity is filled (erased), e.g., when the water is heated. It is possible to calculate the value of AEyi, characterizing that process. The fluctuational movement of a proton in an H2O molecule in a direction perpendicular to the line of link OH constitutes that of a harmonic oscillator. The potential energy representing shifting of an ion of hydrogen by the value r with respect to the point of balance may be expressed in the form of energy of a harmonic oscillator: V(r) = M H w H r 2 /2.
(4)
526
Here MR- is the mass of an atom of hydrogen, W H ~ 3 X 1014 s _ 1 is the frequency of normal vibrations of a proton in a molecule of water in a direction perpendicular to the line of the OH link.2 Taking into account that the angle between the lines linking each of the protons with the nucleus of oxygen equals 2a PS 104.5°, we find that energy required for deformation of the outer dimensions of a water molecule by the value of AR « 0.26 A, sufficient for putting a molecule inside a microcavity would be M
^ R 2 „ L 1 eV. (5) 2 cos a This variable represents energy threshold AEu = V(AR) determining the process of water relaxation. This threshold greatly exceeds the thermal energy of water molecules, which is equal to k^T « 0.025 eV at room temperature. Then it can be seen that the time of relaxation TLW is strongly correlated with the threshold value for energy of deformation of a water molecule AEM and its temperature T. A big value of A.EM leads to a small probability of overcoming the barrier in the area of an entrance window to a microcavity. In the result, the probability of spontaneous deactivation of water is very small, which means a very long period of storing information. Let us make some quantitative estimates. At the temperature of water T = 293K (20°C) the time of relaxation (the duration of "water memory") is equal to Tiw ~ 10 days. With higher water temperatures time of relaxation decreases sharply, and it increases with cooling down (see Table 1). For an alternative direction of relaxation (transferring a single molecule of water from the volume of a microcavity into the volume of amorphous water), the time of relaxation T2W is also determined by an expression similar to Eq. (3), where energy of activation is different (AEM — AE « 0.9 eV instead of AEM « 1.1 eV). Moreover, it is necessary to remember that because the inner dimension of a microcavity is considerably bigger than the size of a potential pit for each molecule in the volume of quasi-amorphous water, the actual frequency of collisions of a water molecule with the walls inside a microcavity u>u ~ 1/ro will be lower, while period To will be, respectively, larger than in the volume of water. The results of calculation of time of relaxation T2W during a reverse transferring of molecules H2O from a volume of a microcavity into quasi-amorphous water are also presented in Table 1. It should be noted that in order to calculate values of Tiw and T2W we need to know the exact values for the energy of activation and the height of a potential barrier regulating the entrance into volume of microcavities of the clathrate frame. These parameters have been determined by us from model calculations. Respective values of Tiw and T2W may differ considerably in specification of these parameters. The obtained values of Tiw and T2W represent water relaxation from an unstable state to a stable one, corresponding to a specific temperature. If we examine this process from the point of view of information theory, the generation of an unbalanced distribution may be considered a process of recording information in a volume of water. We shall call such water activated. =
527 Table 1. Times of relaxation of water (duration of "water memory"). T (°C)
T1W
T2W
1 10 20 30 36.6 40 50 60 70 90
300 days 49 days 10 days 58 h 24 h 15 h 4.4 h 1.3h 27min 3min
30min 14min 4min 1.5 min 45 s 30 s 12 s 4s 1.5s 0.3s
A very long time of relaxation TJW allows us to assume that water is a two-level (or rather double-zone) bi-stable system with a long lifetime in each of those states. Such systems allow the recording and holding of information (in the form of ratio of occupied and vacant microcavities) as well as using that information effectively by altering the properties of water at time of transferring of a large number of H2O molecules and other atoms dissolved in water, as well as molecules and ions from the state of amorphous water into the volume of linked microcavities, or the other way around (Fig. 2). Although the time of reverse relaxation T2W at the exit of water molecules from the volume of microcavities turns out to be considerably lower than time of direct relaxation at the entrance to these microcavities, in any case, it is many orders of magnitude greater than the typical time of relaxation (1) (r) « 10 _ 9 -10 s due to fluctuations of the hydrogen link in the volume of amorphous water. It may also be noted that the process of activation of water may be conducted not only during its heating or cooling, but also through the effects of magnetic fields or ultrasound. Such periodic coherent influences can stimulate formation of quasistable clusters, each one of which unites several reciprocally arranged cluster frames. In such a system, the behavior of isolated water molecules in periodically situated microcavities is similar to movement of hydrogen in palladium, where a very high saturation of lattice is achieved. Periodic influences can also affect the parameters of the clathrate frame of water, altering, e.g., the transparency of the potential barrier in windows of microcavities. (This is the problem with tunneling a molecule H2O through a non-stationary barrier.) Moreover, a strong periodic magnetic field can stimulate transfers between energy levels, which characterize the state of H2O molecules in microcavities and amorphous water (e.g., due to multi-photon nonlinear processes during interaction with magnetic moments), which causes uneven populating of microcavities by water molecules and constitutes activation of water.
528
3. The Mechanism of Time-Dependent Self-Organization of Coulomb-Free Nuclear Reactions in Optimal Potential Wells in Dynamic Systems The same clathrate space structure applies to heavy water (D2O). The potential energy of the D atom in the central part of the cavity with "water walls" is close to parabolic. The possible mechanism of nonbarier nuclear reaction in optimal potential holes was described in Ref. 2. In such well the spectrum of quantum energy levels is equidistant and En = hwQ (n + 3/2),
n = 0,l,2,...
(6)
Let one atom X be in the center of such a well. When other atom Y gets into the well (e.g., due to diffusion), a complex X + Y appears in the well. In the free space (e.g., for a well with the size R —> 00) this complex would correspond to quasimolecule {XY). In the quantum system the situation is more complicated, because in such a system energy of total X-Y interaction V(r) is a sign-variable distance function (e.g., Ref. 2) which is important for the calculation of diagonal matrix elements: R
Vnn=
J
U^n{r)\
2
V(r)r2dr,
a=-^. mez
0
The main question is: Can this energy be a small perturbation and not influence the character of the atoms or nuclei movement and interaction in quantum system? For that purpose, the diagonal elements of interaction energy matrix should be small (a) and probability of interlayer transition because of this interaction should also be small (b). The probability of interlayer transition in the parabolic potential well becomes equal to zero automatically at the optimal moments of time r = 2sir/uio, s = 1, 2, 3,..., when the frequencies of all possible interlayer transitions
Figure 3. Correlation between energy spectrum of quantum levels En and spectral density | V(OJ)| 2 of perturbation energy V(t) for t < r , t = T, t > T.
529
u>nk = (n — k) u>o will correspond to zero spectral density of perturbation energy (see Fig. 2): 2 L : „ / . . _ ; o \ / / ^ . / n2M 2 = TV^nk[Bm(wT/2)/(w/2)] . (7) o Here atoms or nuclei interaction completely disappears and wave function of atoms is determined only by quantum potential field (well) properties. To zero the diagonal matrix elements of interaction energy (which is a signvariable function of inter-nucleus distance) Vnn it is essential that the size of the hole R be optimal. For the typical atom in the X-Y system this optimal size is
\V(u)\
2
/
TA
M . . _ / : . . i \ j i
Vnk(t) exp(iwi) dt
If all the above-mentioned conditions (a) and (b) are met, the independent from first atom X quantizing of the second atom Y in the optimal well takes place. In this case, the wave function of this atom -0n(O) in all even states will be different from zero in the center of the well, where the first atom X is located. This leads to a high probability A = C\ipn(0)\2 of nuclear fusion. In such a well, the spectrum of quantum levels of D atom is equidistant. In such a compressed, isolated system the energy of dd Coulomb interaction of two D atoms is a small amendment and does not influence the character of atoms or nuclei movement and interaction (including dd-fusion).2 Each such microcavity resembles a non-threshold microreactor in water volume. References 1. E. Pauling, Hydrogen Bonding D. Hadzi (Ed.) (Pergamon Press, London, 1959). 2. V. I. Vysotskii and A. A. Kornilova, Physical foundation of long-time water memory, Moscow Univ. Phys. Bull. 59 (3), 58 (2004). 3. V. I. Vysotskii and A. A. Kornilova, Nuclear Fusion and Transmutation of Isotopes in Biological Systems (MIR Publishing House, Moscow, 2003), 302 p.
E X P E R I M E N T S ON CONTROLLED D E C O N T A M I N A T I O N OF WATER M I X T U R E OF LONG-LIVED A C T I V E ISOTOPES IN BIOLOGICAL CELLS
V L A D I M I R I. V Y S O T S K I I Kiev Shevchenko
University,
Kiev,
Ukraine
ALEXEI ODINTSOV Institute
of problems
of NPP safety,
Kiev,
Ukraine
V L A D I M I R N. P A V L O V I C H Kiev Institute
of Nuclear
Research,
Kiev,
Ukraine
A L E X A N D R B. TASHIREV Kiev Institute
of Microbiology,
Kiev,
Ukraine
A L L A A. K O R N I L O V A Moscow
:
State
University,
Moscow,
Russia
In this work, the process of direct controlled decontamination of highly active long-lived isotopes by the action of growing microbiological systems has been studied. For the first time the accelerated controlled deactivation of C s 1 3 7 isotope was observed.
1. Introduction and Foundation of the Effect of Transmutation of Radioactive Waste in Biological Systems The process of decontamination (deactivation) of radioactive waste by action of growing microbiological systems is connected with the transmutation of long-lived active nuclei to different non-radioactive isotopes during growth and metabolism of special microbiological MCT ("microbial catalyst-transmutator"). The MCT compound is in the form of special granules that include: (1) concentrated biomass of metabolically active micro-organisms, (2) sources of carbon and energy, phosphorus, nitrogen, etc., (3) binding substances that keep all components in the form of granules stable in water solutions for a long period of time in any external conditions. The base of the MCT is microbe syntrophin associations of thousands different micro-organisms of different kinds that are in a state of complete symbiosis. These 530
531
micro-organisms are from different physiological groups that represent practically the whole variety of microbe metabolism and relevantly all kinds of microbe accumulation mechanisms. The state of complete symbiosis of the syntrophin associations results in the possibility of maximal adaptation of the micro-organisms' association to any change in external conditions. The typical reaction of the association to such aggressive change demands time for internal adaptation. This time is necessary for a mytagene change, which takes about 10 generations, corresponding to several days. During this time, there occurs a purposeful synergetic process of stimulation of the mutant formation of such micro-organisms that are maximally adapted to the changed aggressive conditions. The possible mechanism of nuclear transmutation in growing biological system is described in detail in Ref. 1. In our preview work,2 we studied the process of accelerated decay of activity of reactor water from first contour of water-water atomic reactor of Kiev Institute of Nuclear Research. The water with total activity about 1 0 - 4 Curie/L contained highly active isotopes (e.g., Na 24 , K 40 , Co 60 , Sr 91 , I 1 3 1 , Xe 135 , Ba 140 , La 140 , Ce 141 , and Np 2 3 9 ). The spectrum of gamma-radiation of this water is presented in Fig. 1.
Ce 1 4 1 Co60
0
500
1000
1500
Ey (keV)
Figure 1. Spectrum of gamma-radiation of distilled water from first contour of water-water atomic reactor (10th day after extraction from the active zone).
For the first time we have observed the fast utilization of several kinds of active isotopes to non-radioactive nuclei in the flasks that contained MCT. The results of investigation of the activity Q{t) of the same reactor Ba 140 , La 140 , and Co 60 isotopes in the experiment on transmutation (activity is (^cultures) and in the control one (Qcontroi) are presented in Fig. 2.
532
1
O(IVO(0)
0.9 -
4._._
^....-^......-f.....^.....^ ^control
0.8
\.
^cultures < d e C a V °
f C
°
6
°
i n b o t h
PUre
active micro-organisms)
\
0.7
a n d
water and in the water with presence of metabolically
0.6 0.5 0.4
Time of internal adaptation of microbe syntropin associations to action of irradiation
^
,
°co„tr„|(daCay0f
x
Ba 140 and La 140 in pure water)
^ :
0.3 140 j.
0.2 0.1
Q,'cultures ( d e c a y o f Ba and Laa 1 *" in pure water with presence of metabolically active micro-organisms)
Ok 25
30
t, days after extraction of water from the active zone of the nuclear reactor
Figure 2. Activity Q(t) of the same reactor B a 1 4 0 , La 1 4 0 , and Co 6 0 isotopes in the experiment on transmutation (activity Q cu itures m pure reactor water with presence of metabolically active micro-organisms) and in the control one (activity Qcontrol m the same pure reactor water without micro-organisms).
The La 140 isotope has short half-life TL & = 40.3 h and is non-stable daughter isotope of Ba 140 radioactive isotope that has a half-life of about r e a = 12.7days: Ba 140
La 1 4 0 +/r.
Initial activities of the Ba 140 and La 140 isotopes (on the 10th day after extraction of water from the active zone of the nuclear reactor) were Q B a-i40 = l-46.10- 7 Curie/L and Q L a-i40 = 2.31.10- 7 Curie/L. A possible path for radioactive Ba 140 isotope transmutation to the stable state is B a 1 4 0 + C 1 2 = S m 1 5 2 + AE. These reactions are energy favorable and the energy of reaction: AE = E{ABaZBa)
+ E(AC, Zc) - E{ASm,
ZSm) = 8.5 MeV is positive.
The Sm 2 + and Ca 2 + ions are chemically alike and have the approximately the same ionic radii of divalent state (Rsm ~ 1-2 A, RCd, ~ 1.06 A). The substituted element Ca is among several vitally necessary elements. Ions of created Sm 2 + elements can substitute Ca 2 + ions while microbiological cultures are growing.
533
2. Experimental Investigation of the Utilization of Long-Lived Active Isotopes in Growing Associations of Microbiological Cultures In our previous work,2 we observed and studied the process of deactivation of radioactive isotopes with short or intermediate half-lives (about 1 month or less). The aim of our new work was to study the process of direct controlled decontamination of a highly active water mixture of selected different long-lived active isotopes with many years half-life by action of the same growing microbiological systems (MCT). The research has been carried out on the basis of the identical distilled water that contained four long-lived reactor isotopes: Eu 154 (initialactivity 700 bq), Eu 1 5 5 (« 300 bq), Cs 1 3 7 (« 2.10 4 bq), Am 2 4 1 (« 1500 bq) In our experiment eight identical closed glass flasks with very thin walls and with 10 ml of the same active water in each were used. The MCT compound was placed in seven glass flasks.
"Microbial catalyst-transmutator" (MCT compound)
MCT + active water + KCI
MCT + active water + CaC03
Figure 3.
MCT + active water + NaCI
MCT + active water + FeSCU
MCT + active water + MgS04
MCT + active water + P
Control 1. MCT + active water
Control 2. Active water
Study of utilization of active isotopes at different conditions.
In six different flasks different pure K, Ca, Na, Fe, Mg, and P salts as single admixture were added to the active water. These chemical elements are vitally necessary to maintain life in any culture. Each these replacements completely blocks the channel of transmutation with the use of all biochemical analogs of the chemical element. The other way, these replacements act in connected with formation of optimal balance of microelements. The results obtained confirmed the importance of such replacements. Two additional flasks were used for control experiments: one flask contained the active water and MCT (but without additional salts) and in another one contained only active water (without salts and MCT). The cultures were grown at the temperature 20° C. The activity in all closed flasks was measured every 7 days using a precise amplitude, large scale Ge detector. During the process of measuring of spectrum, a special screened box with a very low level of natural ionizing radiation background was used.
534
3. Results of Experiments and Discussion The results of investigation of change of relative activity Q(t)/Q(0) of isotopes are presented in Fig. 4 and Table 1. We observed speeded-up decay of Cs 137 in all experiments with MCT and with the presence of different additional salts during more 100 days. In the control experiment (flask with active water) the law of decay was "usual" and the half-life was about 30 years. The most speeded-up decay with r* PS 310 days (accelerated by 12 times) was observed in the presence of Ca salt. In the presence of an abnormal (redundant) quantity of potassium in the nutrient media the process of cesium transmutation becomes very weak and the half-life of decay was roughly 10 years! The possible reaction of Cs 1 3 7 isotope utilization is C s ^ + p1
Baid8 + AE.
The result of this reaction is the creation of stable Ba 138 isotope. This reaction is energy favorable (AE = 5.58MeV is positive). The Ba 2 + and K + ions are chemically alike and have the approximately same ionic radii of divalent state (i?Ba ~ 1.4 A, RK « 1.33 A). Substituted element K is among several vitally necessary elements. Ions of created Ba 2 + elements can substitute K + ions in metabolic process while microbiological cultures are growing. Cs 1 3 7 without MCT (control) x = 30 years
Activity, 0(0/0(0) ^
1.00 0.98 --•
Cs 1 3 7 + MCT+KCL T* = 10 years
0.96 0.94
Cs 1 3 7 + MCT+NaCI T* » 480 days
0.92 41 0.90
Cs 1 3 7 + MCT x* = 380 days
Cs 1 3 7 + MCT+CaC0 3 x* = 310 days
0.88
0
10
15
20
25 f (days)
30
35
40
45
Figure 4. Accelerated deactivation (accelerated decay) of C s 1 3 7 isotope in "biological cells" in the presence of different chemical elements.
Table 1.
Deactivation of different active isotopes in optimal experiment (MCT + active water in the presence of C s 1 3 T + CaCOa salt)
Isotope
Energy (keV)
Start of experiments Nj (registered events per 10 3 s)
Eu154 Cs137 Eu154 Eu154
123.09 661.7 1004.5 1274
15500 266900 1221 1918
Intermediate finish of experiments (duration 100 days) N j , (registered events per 10 3 s)
Error (absolute /relative, %)
Natural decay (%) (per 100 days)
Change (%) ( N 2 Ni)/N2
15180 216800 1131 1929
±155 (±1) ±478 (±0.2) ± 3 6 (±3) ± 4 5 (±2)
-2.1 -0.6 -2.1 -2.1
-2.6 -24 -8 0
536
Such substitution is more effective t h a t "direct" replacement of potassium t o cesium because the ionic radius of cesium is Res * 1.65-1.69 A t h a t is larger t h a n the ionic radius of RK ~ 1.33 A of potassium. By the way such substitution (but for stable chemical elements) was observed earlier in experiments with microculture Blastocladiella emersonii.3 In these experiments the substitution of K + ions to R b + and B a 2 + ions have taken place. These ions can replace each other in transporting ions through the cell membrane. W h y does t r a n s m u t a t i o n efficiency improve with the increased concentration of calcium? Such a phenomenon is probably connected with the general problems of the metabolism of microbiological cultures: optimal growth of microcultures takes place with a balanced relation of microelements. T h e very phenomenon of low energy t r a n s m u t a t i o n of chemical elements and isotopes in biological systems - and the necessary conditions t o sustain this phenomenon - is lodged on the heuristic proposition t h a t if some of the required elements or microelements are not present in the living environment (or nutrient media), then if certain prerequisites are met the missing elements will be synthesized in biological transmutations. In fact, such an approach unambiguously suggests t h a t the ratio of all the necessary elements in each type of living organisms is fixed. These results reveal the non-trivial nature of interactions of different microelements. Changing the makeup of the nutrient medium makes it possible to control the speed of a culture's growth. W h e n at least one of the microelements is lacking in the nutrient medium, this hinders the development of the entire biological object. These fundamental results were investigated in details in Ref. 1.
References 1. V.I. Vysotskii, and A.A. Kornilova, Nuclear Fusion and Transmutation of Isotopes in Biological Systems (MIR Publishing House, Moscow, 2003). 2. V.I. Vysotskii, V.N. Shevel, A.B. Tashirev, and A.A. Kornilova, Successful experiments on utilization of high-activity waste in the process of transmutation in growing associations of microbiological cultures, in Proceedings of the 10th International Conference on Cold Fusion (Programm and Abstracts, 2003), p. 121. 3. J. Van Brunt, J.H. Caldwell, and F.M. Harold, Circulation of potassium across the plasma embrane of Blastocladiella emersonii: K-chanel, J. Bacteriol. 150 (3), 14491561 (1982).
A S S E S S M E N T OF T H E BIOLOGICAL EFFECTS OF "STRANGE RADIATION
E.A. PRYAKHIN AND G.A. TRYAPITSINA Chalyabinsk State University, Chalyabinsk, Russia L.I. URUTSKOYEV RECOM Company "Kurchatov Institute," Moscow, Russia A.V. AKLEYEV Urals Research Center for Radiation Medicine, Chalyabinsk, Russia
Results from studies of electrical explosions of foils made from super-pure materials in water pointed to the emergence of new chemical elements. An additional finding was the discharge of a "strange" radiation accompanying transformation of chemical elements. 1 Identical phenomena were revealed during tests of voltage limiters (VL) for breakdown. The intensive research work focusing on effects of "strange" radiation, and the use of voltage limiters for industrial purposes require that appropriate safety regulations be developed and applied in practice. However, currently, the mechanism involved in the interaction between "strange" radiation and a substance or a biological entity remains unclear. The two principal questions brought up in connection with the assessment of the biological effects of "strange" radiation: (1) is exposure to "strange" radiation safe for the personnel engaged in the studies? (2) Can biological systems serve as detectors of "strange" radiation? Therefore, the aim of research was to investigate the biological effects of the "strange" radiation. 1. Project Tasks (1) Estimate the key hematological parameters after exposure of experimental animals to "strange" radiation resulting from explosion of foils in water or aqueous solutions. (2) Study the genotoxic effects of the "strange" radiation. 537
538
2. Material and Methods 2.1. Experimental
Exposure
Pilot studies were performed at the RECOM RRC "Kurchatov Institute" in AprilMay of 2004. Animals used in the experiment were female mice of C57B1/6 line aged 80 days with body weight 16-18 g. The animals were exposed to radiation discharged during explosions of Ti foils in water and aqueous solutions. 1 The cages with animals were placed at 1 m from the epicenter of the explosion. As can be seen from Table 1, explosions were carried out on the 19th (three explosions), 20th (four explosions), and 22nd (three explosions) of April, 2004 (explosions 1373-1382, respectively). Table 1.
Schematic presentation of the experiment. expo-
Total number of explosions
Group
Number of sure days
Control 1 2 3
-
-
1 2 3
3 7 10
Number of animals per group 20 20 17 19
The animals were assigned to four experimental groups, each of 17-20 mice. The animals received experimental exposure within 1, 2, and 3 days of the experiment (Table 1). In total, the experimental groups were exposed to three, seven, and ten explosions, respectively. 3. Hematological Studies In order to identify the basic reactions of the hemopoietic system, the following parameters were estimated using conventional methods: number of nucleated cells in the bone marrow, number of leucocytes in the peripheral blood, cell composition of the bone marrow, the rate of bone marrow erythrocytes at different levels of maturation (polychromatopile-oxiphile), and cell composition of the peripheral blood. In the other experiment the number of CFUs was evaluated after acute whole body gamma-irradiation at a dose of 6 Gy. 3.1. Study of Genotoxic
Effects of "Strange"
Irradiation
To assess the potential genotoxic effect of "strange" radiation, the rates of bone marrow polichromatophile erythrocytes with the micronuclei were studied using the bone marrow slides from the hematology experiment. In addition we studied genotoxic effects of combined exposure to "strange" radiation acute gamma-irradiation at a dose of 2 Gy, which was given on the next day.
539 Table 2. Schematic presentation of the experiment. acute gamma irradiation.
Estimation of the CFUs after
Group
Number of exposure days
Total number of explosions
Control + 6 Gy 1 + 6Gy 2 + 6Gy 3 + 6Gy 6Gy + 3
-
-
1 2 3 3
3 7 10 10
Number of animals per group 20 20 17 20 20
4. Results and Discussion 4.1. Studies of the Effects of "Strange" Radiation of Nucleated Cells in the Bone Marrow
on the
Number
The number of nucleated cells in the bone marrow counted for the control group of C57B1/6 mice amounted to 38.6 + 1.6mln/femur (Fig. 1). In spite of the fact that exposure to "strange" radiation of experimental group Bl on the 19th of April, 2004, and of experimental group B2 on the 19th and 20th of April, 2004, brought about a certain increase in this value up to 42.3 + 1.9 and 42.4 + 2.1, respectively, these changes, however, did not reach statistical significance. Exposure of the experimental animals to ten explosions carried out within 3 days led to a further increase in this value. In this group the number of nucleated cells in the bone marrow was 45.1 + 1.7 mln/femur which exceeded significantly (by 17%) the respective values obtained for the control group (^student's = 2.79, P = 0.008). Thus, it has been shown by our experiment that exposure of animals comprising group B3 to explosions of Ti foils in water and aqueous solutions results in an increased number of nucleated cells in the bone marrow of C57B1/6 mice. Such changes were accompanied by an increase in the percentage and count of dividing cells in bone marrow. It can be assumed that these changes are induced by the following mechanisms: stimulation of stem cell division in the bone marrow, accelerated division of cells in a proliferating cell population within an organ, delayed maturation, decreased cell cycle time, decreased frequency of apoptotic cell loss, disturbances of cell migration Table 3.
Schematic presentation of the experiment. Study of genotoxic effect.
Group
Number of exposure days
Total number of explosions
Number of animals per group
Control 1 2 3 Control + 2 Gy 3 + 2Gy
-
—
1 2 3
3 7 10
-
-
3
10
20 20 17 19 10 10
540
Exposure days Figure 1. mice.
Numbers of nucleated cells in the bone marrow per experimental group of C57B1/6
from the bone marrow to the blood, or by a combination of two or several of the above-listed mechanisms. 4.2.
Studies
of the Population
of Bone Marrow
Stem
Cells
To understand the biological mechanisms of bone marrow changes we studied the reaction of bone marrow stem cells to "strange" radiation. In that experiment animals were exposed to acute whole body gamma-irradiation at a dose of 6 Gy after exposure to "strange" radiation. The spleen colony-forming units were analyzed at day 9 after gamma-irradiation. No significant changes were revealed in bone marrow stem sells in that experiment (Fig. 2). So, we can conclude that "strange" radiation did not influence bone marrow stem cells. Simultaneously, in the same experiment we studied the repopulation of bone marrow cells at day 9 after gamma-irradiation. This allowed us to reveal a decrease in bone marrow repopulation in the group of animals exposed to gamma-irradiation followed by exposure to "strange" radiation for 3 days (Fig. 3). 4.3.
The Ratio of Polychromatophil-to-Oxiphil Erythrocytes in Different Experimental
Bone Groups
Marrow
To study the involvement of changes in cell on the increase in total bone marrow cell count, we analyzed the ratio of erythrocytes at different levels of maturation (polychromatophil-to-oxyphil). We did not find statistically significant changes in the analyzed parameter, but we noted that the PCE/OPE ratio increased with time of exposure (Fig. 4). After subsequent gamma-irradiation at adose of 2 Gy, we found a significant increase in the P C E / O P E ratio as compared with the reaction of bone marrow cell to gamma-irradiation in the control group. These two facts allow us to
541
Experimental groups Figure 2. Number of CFUs in different experimental groups after gamma-irradiation of mice at a dose of 6 Gy.
6 Gy
B1 + 6 Gy
B2 + 6 Gy
B3+ 6 Gy
6 Gy + B3
Experimental groups Figure 3. Bone marrow cell numbers in different experimental groups after gamma-irradiation of mice at a dose of 6 Gy.
suppose that "strange" radiation leads to increased levels of immature erythrocytes in the bone marrow. 4.4. Studies
of the Genotoxic
Effects of "Strange"
Radiation
To evaluate the genotoxic effect of "strange" radiation, the rates of micronuclei in the bone marrow erythrocytes were analyzed. We did not reveal any statistically significant changes of the parameter. But in the experiment with combined exposure to "strange" radiation and subsequent gamma-irradiation, the rate of micronuclei
542
Control
B1
B2
B3
2 Gy
B3 + 2Gy
Experimental group
Figure 4. The ratio of polychromatophil-to-oxiphil bone marrow erythrocytes in different experimental groups.
was 1.5 times lower in comparison with the effect of only gamma-radiation. This type of reaction is called "adaptive response" in radiobiology (Fig. 5). It may be attributed to the activation of protein synthesis in cells and activation of DNA repair mechanisms.
1.6%
1.40%
1.4% 1.2% 1.0% 0.8% 0.6% 0.4% 0.2%
0.12%
0.0% Control
0.14%
0.11%
±
-r
BBBB
• • f
jUm^mmjMjII
MSMflBlHI
B1
B2
0.10%
B3
2Gy
B3 + 2Gy
Experimental group
Figure 5. Rates of micronuclei in polychromatophil bone marrow erythrocytes for different experimental groups.
543
4.5. Studies of the Effects of "Strange" Radiation Peripheral Blood Leucocyte Counts
on the
It can be seen based on the analysis of leucocyte counts in the peripheral blood of mice exposed to "strange" radiation, that none of the experimental groups showed statistically significant changes in the parameters studied. It is known that the occurrence of changes in peripheral blood cell counts lags behind the reaction manifested by changes in bone marrow cell counts by about 5 days. It can be suggested, therefore, that an increase in bone marrow cell counts would have been manifested by increased numbers in leucocytes of peripheral blood, if the exposure time had been prolonged. 4.6. Analyses
of the Peripheral
Blood Cell
Composition
The studies of the peripheral blood cell composition is a routine procedure applied for diagnosing various pathologic conditions in humans and animals. In our experiment the rates of peripheral blood neutrophils observed for the control group amounted to 15%. The experimental exposures led to a consistent increase in peripheral blood neutrophil counts. Thus, within a day after exposure to three explosions, the rate of neutrophils in the peripheral blood was 18%, within 2 days it was 22%, and at day 3 a statistically significant increase in the rate up to 25.5% was registered (Fig. 6). The regression analysis of the relationship between the rate of neutrophils and exposure time allowed estimation of a statistically significant (F = 13.53; P = 0.0005) effect of the factor on the parameter studied. The increase in the rate of neutrophils occurred primarily at the expense of mature segmented neutrophils, whereas the number of stab cells did not differ significantly from that found for controls. Along with the changes in the contents of neutrophils in the peripheral blood, the rate of peripheral blood lymphocytes was found to be reduced. A statistically significant decrease in this parameter to 68% was observed at day 3 of exposure. No statistically significant fluctuations in the rates of peripheral blood eosinophils and monocytes were observed in the experimental animals, however, attention is attracted to a reduction in the rates of monocytes with increasing exposure time. It can be suggested that after the analysis of the total sample is completed, such changes may reach statistical significance. The increase in the contents of neutrophils in the peripheral blood can be the result of several reasons: (1) an increased bone marrow neutrophil production (which is unlikely in our situation as there was not enough time for the manifestation of such effect), (2) incoming of neutrophils from the place of deposition, (3) decrease in neutrophil apoptosis rate. Thus, it can be concluded based on the results of our experiments that: (1) "strange" radiation stimulates proliferation of bone marrow cells with or without delay in maturation,
544
Exposure days
Figure 6.
The relationship between the rates of peripheral blood neutrophils and exposure time.
(2) it induces changes resulting in increased resistance to genotoxic exposures (gamma-irradiation and others), (3) "strange" radiation aggravates the clinical course of acute radiation disease if it is applied after gamma-irradiation, (4) it leads to changes of cells composition in the blood. 5. Conclusions These studies produced the following conclusions: (1) "strange" radiation - that results from the explosion of Ti foils in water and other aqueous solutions - has the capacity to produce biological effects. (2) Biological effect of "strange" radiation is manifested by an increase in the number of nucleated cells in the bone marrow. (3) "Strange" radiation leads to an increase in dividing cells in bone marrow. (4) "Strange" radiation resulting from ten explosions carried out within 3 days after exposure to gamma-radiation (6 Gy) leads to a decrease in bone marrow repopulation. (5) Assessment of the rate of micronuclei in bone marrow erythrocytes did not reveal any genotoxic effect of "strange" radiation. (6) Exposure of mice to "strange" radiation leads to 1.5-fold decrease in genotoxic effect resulting from additional gamma-irradiation (2 Gy). Such reaction may be described as an adaptive response. (7) Exposure to "strange" radiation can bring about an increase in the proportion of neutrophils in the peripheral blood of experimental animals. (8) It can be suggested by the results of the test exposures that "strange" radiation can affect human health.
545
(9) It has been shown by these preliminary studies that to gain more insight into the biological effects of "strange" radiation, further investigation would be necessary. References 1. L.I. Urutskoev, V.I. Liksonov, V.G. Tsinoev, Observation of transformation of chemical elements during an electric discharge, Ann. Fond. L.de Broglie 27, 701 (2002).
POSSIBLE N U C L E A R T R A N S M U T A T I O N OF N I T R O G E N IN T H E EARTH'S A T M O S P H E R E
MIKIO FUKUHARA Institute
for Materials Research, Tohoku University E-mail: fukuhara@imr. tohoku. ac.jp
An attempt to give a possible answer to a question why nitrogen exists so abundantly in Earth's atmosphere and how it was formed in Archean era (3.8-2.5 billion years ago) is presented. The nitrogen is postulated to be the result of an endothermic nuclear transmutation of carbon and oxygen nuclei confined in carbonate MgCC>3 lattice of the mantle with an enhanced rate by attraction effect of catalysis of neutral pions, produced by electron emission: 12 C + 1 6 Q _ 27T0 -» 2 1 4 N. The excited electrons were generated by rapid fracture or sliding of carbonate crystals due to volcanic earthquake, and many of the neutrinos were derived from stars, mainly the young sun. The formation of nitrogen would continued for 1.3 billion years from 2.5 to 3.8 billion years in Archean era, until the active volcanism or storm of neutrinos ceased. The transformation is possible by the combined effects of the screening attraction of free electrons and thermal activation in deeper mantle. The possible nuclear transmutation rate of nitrogen atoms could be calculated as 2.3 X 10 6 atom/s.
Key words: Nuclear transmutation of nitrogen, Atmosphere of Earth, Carbonate in mantle, Neutral pion-catalysis, Neutrinos from young sun.
1. Introduction When we examine the composition of the atmosphere of the sun's planets and their 61 satellites, we note that the nitrogen concentration is rather low (~6%) on average, with the exception of the Earth, Titan, and Triton (Fig. I) 1 ' 2 . Earth has extremely high concentration of nitrogen of 78%, in Titan and Triton the concentration would be smaller than 2 x 10 _ 6 % and 5 x 10^ 6 % of the Earth's one, respectively.3 Since rocky planets (Mercury, Venus, the Earth, and Mars) having inner orbitals had formed by accretion of solid planetesimals in the same region of the developing solar system at almost the same time, 4 we cannot imagine that abundance of nitrogen is derived from the planetesimals with abundance of nitrogen as the secondary atmosphere, after the primary, captured atmosphere was released.5 A significant question for the origin of abundance of nitrogen has not been entirely resolved, and has been overlooked without consensus. 546
547
Exterior planets
Sun Mercury Venus Earth Mars
Interior rocky planets Figure 1.
"ijllfc'
/."IP*
Jupiter
Saturn
Uranus
Neptune
Pluto
Solar planets (The Planetary Society of Japan).
2. Appearance of Nitrogen in Early Earth When we carefully investigate the variation of atmospheric gases during the Earth's history, based on an assumption calculated by many research groups (Fig. 2 ) 6 - 1 0 , we find that the decrease in carbon dioxide composition is accompanied by a gradual accumulation of nitrogen into the atmosphere in the Archean era, before the generation of atmospheric oxygen derived from photosynthetic activity by organic matter, starting around 2 billion years ago. 11 The disappearance means the formation of rocks and mantles containing carbon dioxide due to weathering of igneous rocks. The main parts of carbonaceous rocks are distributed on and near the Earth's surface. Thus, the consumption of the carbon dioxide, i.e., formation of carbonates, seems to correlate with the formation of nitrogen. Thus we note the possibility of nuclear transmutation between carbon and oxygen atoms in carbonate crystals to form nitrogen.
1.8
i
1.6 X
1.4 *
•
.
*m
.c 1.2 a a) o 1 E
i CO2 by Owen et al. 6 CO2 by Ohmoto7 CO2 by Kasting8 N2 by Budyko et al. 10 N2 byBertaux O J bv Kastina8
- -» - -—• - - —"— •—**— - • ••- -
X K
*
0.8
*"-.
t
0.6 i
^r
0.4 V
£
c a) o c
0 O
0.2 •
i
m
m
1
•r'
rffC
-4.5
j
Hk*' *" -M
-3.5
>*~
-2.5
„
"•"
-1.5
-0.5
Time before present (billion years) Figure 2. The composition change of atmospheric CO2, N2 and O2 gases from the primitive to present times of the Earth.
548
3. Dynamic Interaction Between C and O Atoms in Magnesite and the Formation of Nitrogen In a previous paper, 1 the reason why the Earth's atmosphere has such a high concentration of nitrogen was ascribed to a possible endothermic nuclear transmutation of carbon and oxygen nucleus pairs confined along three [l-\/30] directions in a (111) plane of rhombohedral MgC03 crystals existing in the mantle crust (Fig. 3). Since the carbonate deposited near the surface of the Earth is a candidate material available for nuclear transmutation, dolomite, CaC03 • MgC0 3 must be taken up as the main carbonate of Archean era. 12 However, we select a magnesium carbonate MgC0 3 (magnesite) instead of dolomite, due to lack of crystal lattice data of dolomite under high pressure over 50 GPa.
Figure 3.
Configuration of CO3 group atoms in (111) magnesite crystal planes.
The nitrogen 14 N is a seven-up state whose isospin wave function is antisymmetric. According to the theory of fundamental processes,13 it is necessary for the transformation to move seven charged pions and six neutral pions from oxygen nucleus to carbon one, and to leave two neutral pions from oxygen one for modulation of the n, p force in nitrogen nucleus.
Proton, neutron interaction
18 71
7 71
3 2 7c"
25 K~
25
1871°
7 7C°
3 2 7C'
24TCC
2 4 7tC
TI"
Pion interaction
549
T h e dynamic interaction is presented by the following nuclear reaction: 12
C +
16
0
-
2TT° = 2 1 4 N ,
(1)
based on neutral pion catalyzed fusion, 14 2
D +
2
D + 27T° =
4
He.
(2)
Pions are responsible for all low-energy nuclear interactions; 1 5 the pions within the nucleus allow nucleonic species to bond together and t r a n s m u t e into each other. 1 6 Kenny 1 7 has pointed out t h a t the nucleus is charged by electron capture into neutral pion and t h e n decays to produce heat energy. His electropionic mechanism rests on mass alone and sacrifices b o t h baryon conservation and quark consistent pictures of elementary particles. In the case of a deuteron with a lower mass, we have reported the following formula, 1 8 e_+
2
D - ^ 7 r ° + ^ + 7,
(3)
where v and 7 are neutrino and photon, respectively. T h e excited electron e* was generated by rapid fracture or sliding of carbonate crystals due to volcanic earthquake, and a large number of neutrinos v were derived from stars, mainly the sun. Since the neutral pion does not experience a Coulomb barrier, compared with the charged pions, it can easily enter within effective nuclear force field of C - O pairs at close proximity. T h e effect of neutral pion on the nuclear reaction in solid states has been almost overlooked, as far as we know. T h e neutral pion is provided by emission of two excited electrons derived from the carbonate lattice, 1 3 e->e*,7, 7
+
7
(4)
= 7r°.
(5)
Here we consider the nuclear reaction of Eq. (1), using low-energy nuclear interaction based on the electropionic attraction. From Eqs. (2)-(5), we got the following formula: 12
C +
16
0 + 2e* + 1v- - • 2 1 4 N +
4
He,
(6)
with help of the electropionic attraction due to the excited electron capture and neutral pion catalysis. In the Archean era, many neutrinos would be come from young sun, 1 9 or from the flares of i-tauri stars. 2 0 Although the neutral pion is recognized as a non-exchange p a r t in nuclear strong field, it clearly plays a decisive role in nuclear t r a n s m u t a t i o n of carbon-oxygen nuclei pairs as catalysis of dynamic nuclear interaction. We assume t h a t the formation of nitrogen and helium had continued for 1.3 billion years in Archean era until the active volcanism or the storm of neutrinos ceased. As far as we know, no previous paper has treated this subject, and the formation rate have not been made clear yet. T h e possibility needs to be confirmed.
550
According to the symmetry meson theory, 21 we can write the interaction energy of two nucleons at separation r as follows:
U
(R) = - § .
(?)
where C is the coupling constant. Since the addition of two neutral pions increases the attraction force by a factor of fourteen in the interaction range of 14 times, we get a condensed C - 0 distance 2r2, 2r 2 = 0.517 x 2ri = 0.517 x 0.974 x 2r 0 = 0.074 nm,
(8)
on the basis of Eq. (7). This value would be lead to fusion of carbon-oxygen nuclei before nitrogen formation. The fusion rate R was calculated as R = 9.254 x 1 0 ' 6 f/s/cm 3 . 22 The Earth's nitrogen is present in four pools. 23 lithosphere (10 23 g, atmospheric (3.9 x 10 21 g), terrestrial (4.8 x 10 17 g) and aquatic (2.3 x 1019 g). Then we can calculate the formation rate R' for 1.3 billion years from 2.5 to 3.8 billion years in Archean era, 1 34 x 10 23 ' = 1 4 x 1 , 3 0 0 , 0 0 0 , 0 0 0 x 3 6 5 x 2 4 x 6 0 x 6 0 * 2"3
R
X 1(fi a t
°m/s-
(9)
4. Nuclear Transmutation Rate of Nitrogen for Electrostatic Screening Attraction and High-Temperature Effects 4.1. Confinement
by Screening
of Condensed
Electrons
If the outer shell electrons of carbon and oxygen atoms in MgCOs lattices behave as free electrons, the resulting screening effect serves as relief of Coulomb repulsive force between carbon and oxygen nuclei. We apply the TF approximation to the screening effect for MgCOs lattice of 55 GPa 24 at around 1200 km below surface of the Earth. For a many-electron atom, TF theory 25 gives (in atomic units) V(r) = -—$-(r/b), (10) r where V(r) is potential energy, and Z is the atomic number. The density of MgC03 at 55 GPa can be estimated as 10.09 mg/m 3 , using density-pressure relationship. 26 Thus we can assume the C - 0 bond distance as 2r\ = 0.0948 nm, being 36% less than the equilibrium one (2ro = 0.147 nm). 2 7 However, this distance is still large for distance (0.079 nm) 1 6 required as dynamic nuclear reaction. 4.2. Rate of Reaction
at High
Temperature
Since the temperature at around 1200 km below the surface in the present Earth is estimated as about 2473 K, 28 we then consider the effect of temperature on the reaction rate k. Using the Arrhenius equation 29 , we can write a ratio of the rates at temperature T0 and T\ as follows: h. k0
=
ZipB/HCTi-To/TiTo) T0 •
/m K
J
551
In comparison with T0 = 300 K and 7\ = 2473 K, we get ^ = 8.2.
(12)
According to the first principle, the following potential form expresses the repulsive interaction between atoms; 15
(13)
U{R) = - A ,
where B is an empirical parameter. Taking the effect of temperature on the reaction rate into consideration, we get the shrunken distance 2r 2 = 2 x 0.839n = 2 x 0.839 x 0.645 x r 0 = 0.0795 nm.
(14)
This radius is still somewhat larger than the critical one (0.079 nm). 4.3. Critical Pressure-Temperature Transmutation
Curve for
Nuclear
Since the nitrogen transmutation is possible by the combined effects of screening of free electrons and thermal activating, we finally calculate the critical temperature as a function of pressure, using both screening and the effect of high temperatures. These results are shown in Fig. 4, along with an actual temperature-pressure line in mantle. 30 A form expresses the relation between critical temperature T and critical pressure P for the nuclear transmutation, T = 7386 x i o - ° 0 0 8 F .
(15)
The two curves intersect at 58 GPa and 2520 K, corresponding to the shrinkage of 35.4% and 22.4%, respectively. Thus, the nuclear transmutation due to two-body confinement of carbon and oxygen nuclei in carbonate MgC03 lattice of deeper mantle was explained by combined effect (50% shrinkage) of screening by free electrons, and temperature enhancing the reaction rate. This point corresponds to an upper portion of lower mantle, being 2285 km below the surface in the present Earth. 12 5. Other Mechanism for Possible Nuclear Transformation of Nitrogen Based on the previous sections, with a view to inquiring the abundant nitrogen in the Earth, we propose the possible nuclear transformation of nitrogen on the basis of confinement of carbon and oxygen nuclei in carbonate crystals: one is due to physical catalysis of neutral pions and neutrinos, the other is due to the combined effects of screening attraction of free electrons and thermal activation in deeper mantle. However, we think of another possibility for the nuclear transformation by electrolysis of a heavy water solution of carbonic acid H2CO3 with deuterated minerals derived from heavy water, under high temperature and high pressure in the inside of the Earth. The driving forth is piezoelectric power generated by the
552
4000
3000 •» ** "
id o a E
^v
2000 - - -
1000
Actual curve
— — - Critical curve
0 0
20
40
60
80
100
Pressure (GPa) Figure 4. Critical temperature-pressure temperature-pressure curve in mandle.
curve
for
nitrogen
transmutation
and
actual
rapid fracture or sliding of rocks due to volcanic earthquake. The details will be described in a later paper. 6. Conclusion The decrease in carbon dioxide composition in Archean era of the Earth was accompanied by a gradual accumulation of nitrogen in the atmosphere. The formation of nitrogen is distinctively associated with the existence of rocks and mantles containing carbon dioxide. Thus we assume that the formation of nitrogen was ascribed to a possible endothermic nuclear transmutation of carbon and oxygen nucleus pairs confined along three [l\/30] directions in a (111) plane of rhombohedral MgC03 crystals existing in the upper mantle crust, 12
C+
16
0 - 27T° = 2 1 4 N.
(1)
The confinement is explained by an attraction effect (48% shrinkage, 2r2 = 0.047 nm) based on catalysis of neutral pions, thanks to combined effect of electron emission derived from the carbonate lattice and many neutrinos coming from stars, especially from the young sun. The critical distance for the transmutation is less than 0.079 nm. The formation rate of nitrogen atoms at upper mantle containing of crust is estimated at 2.3 x 106 atom/s. The formation of nitrogen and helium may have continued for 1.3 billion years in Archean era, until the active volcanism or storm of neutrinos ceased. As another possibility, we think of nuclear transformation by electrolysis of a heavy water solution of carbonic acid H2CO3
553
with deuterated minerals under high temperature and high pressure inside of the Earth. References 1. M. Fukuhara, IL NUOVO CIMENTO 27C, 99-113 (2004). 2. Y. Koide, D. Hirata, H. Yamashita, and T. Sato, Database of Planetary Science, Res. Rep. Kanagawa Prefect. Mus. Nat. Hist, Kanagawa, pp. 13-29 (1987). 3. J. Mitton, The Penguin Dictionary of Astronomy (Penguin Book, London, 1991), Table 6, p. 349. 4. J. F. Luhmann, J. B. Pollack, and L. Colin, Sci. Am. 68-75, (1994). 5. A. Benlow and A. J. Meadows, Astrophys. Space Sci. 46, 293-300 (1977). 6. T. Owen, R. D. Cess, and V. Ramanathan, Nature 277, 640-642 (1979). 7. H. Ohmoto, Kagaku 14, 360-370 (1994). 8. J. F. Kasting, Precamb. Res. 34, 205-229 (1987). 9. S. J. Mojzsis, G. Arrhenius, K. D. McKeegan, T. M. Harrison, A. P. Nutman, and C. R. L. Friend, Nature 384, 55-59 (1996). 10. M. I. Budyko, A. B. Ronov, and A. L. Yanshin, History of the Earth's Atmosphere (Springer-verlag, New York, 1985) p. 2, 16, 128. 11. L. Van Valen, Science 171, 439-443 (1971). 12. R. Jeanloz and T. Lay, Sci. Am. 26 (1993). 13. R. P. Feynman, The theory of fundamental processes (Benjamin/Cummings Publishing Company, London, 1961), p. 37, 41. 14. M. Fukuhara, Fus. Sci. Tech. 43, 128-133 (2002). 15. D. F. Measday and G. A. Miller,Ann. Rev. Nucl. Part. Sci. 29, 121 (1979). 16. S. E. Jones, E. P. Palmer, J. B. Czirr, D. L. Decker, G. L. Jensen, J. M. Thorne, S. F. Taylor, and J. Rafelski, Nature 338, 737 (1989). 17. J. P. Kenny, Fus. Tech. 19, 547 (1991). 18. M. Fukuhara, Fus. Tech. 34, 151 (1998). 19. L. -A. McFadden and T. V. Johnson, Encyclopedia of the Solar System, P. R. Weissman, L. -A. McFadden, and T. V. Jhonson (eds.) (Academic Press, San Diego, 1999) p. 68. 20. A. Unsold, Der Neue Kosmos, 2nd edn. (Springer-Verlag, Berlin, 1974) p.226. 21. R. T. Bush and R. D. Eagleton,J. Fus .Energy 9, 397 (1990). 22. M. Fukuhara, in Proceedings of the fourth meeting of japan cold fusion research society (Morioka, 2003) p. 63. 23. B. A. Stankiewicz, and P. F. von Bergen, Am. Chem. Soc. Symp. Ser. 707, 1 (1998). 24. T. Katsura, Y. Tsuchida, E. Ito, T. Yagi, W. Utsumi, and S. Akimoto, Proc. Jpn. Acad. 67, Ser. B , 57 (1991). 25. J. Schwinger, Phys. Rev. 24, 2353 (1981). 26. S. D. Hamann, Physico-Chemical Effects of Pressure (Butterworth Scientific Publications, London, 1957) p. 57. 27. O. Kennard, International Tables for X-ray Crystallography (International Union of Crystallography, Kynoch Press, Birmingham, England, 1968) p. 276. 28. S. Glasstone and D. Lewis, Elements of Physical Chemistry ( D. Van Nostrand Company, 1960) p. 632. 29. C. Kittel, Introduction to Solid State Physics, 6th Edn. (John Wiley & Sons, New York, 1986) p. 62. 30. E. Ohtani and T. Irifune, Basic Measurement and application of Solid Planet Material Science, H. Takeda, M. Kitamura, and M. Miyamoto (eds.) (Science House, Tokyo, 1994) p. 187 (in Japanese).
E V I D E N C E S O N T H E O C C U R R E N C E OF L E N R - T Y P E PROCESSES IN ALCHEMICAL T R A N S M U T A T I O N S
JOAQUiN PEREZ-PARIENTE Instituto de Catdlisis y Petroleoqutmica, CSIC, Marie Curie 2, 2804-9 Cantoblanco, Madrid, Spain E-mail: [email protected]
1. Introduction The relevance of experimental aspects of alchemy has been neglected for long in academic milieu, but in recent years more thoughtful studies of texts belonging to middle age and early modern European alchemy evidence the presence of coherent and relevant laboratory practices. 1 However, the central core of western alchemy, the quest for the Philosophers' Stone (PS), the substance claimed to transmute base metals into gold, remains, needless to say, elusive. While no book will ever tell us how to prepare such substance, it is nevertheless also true that detailed reports on alchemical transmutations, often authored by witnesses of such events, can be profusely found in the alchemical literature. 2 Taken into account numerical parameters of alchemical transmutations such as the weights of starting base metal, gold, and PS, and the duration of the transmutation experiences, it has been reported elsewhere that the transmutation processes follows a specific pattern similar to that generally observed in conventional catalytic reactions. 3 The objective of this work has been to proceed to a rational/scientific examination of alchemical transmutations. The approach used has consisted, first, in the identification of patterns in large sets of alchemical processes that contain sufficient quantitative information (weight of involved substances, time, etc.) Second, the patterns, if present, should be self-consistent, i.e., similar to those described in the alchemical texts for analogous but non-related different phenomena. 2. Transmutation Procedure and Alchemical Objects According to the alchemical authors, the universal transmutation takes place by means of the PS, sometimes called in the alchemical texts "Universal Medicine," for it can heal the "imperfect" metals of their "illness." A small portion of this substance added or "projected" upon a melted metal or hot mercury is able to convert it into pure gold or silver, in relatively short time, not exceeding in general 1 h, or even few minutes in most reports. The noble metal obtained from the transmutation experience, either silver or gold, was used in some cases to cast coins 554
555
or medals to commemorate the event. Some of them are still preserved in several museum collections across Europe, waiting for systematic physicochemical analyses using advanced facilities. However, some of them turned to be composed of nearly pure silver or gold.4 Other pieces of noble metals of alchemical origin are described in alchemical literature, but descriptions of their chemical and/or physical properties are extremely scarce. One of the very few examples of such products has been recently brought to light.5 The well-known 17th century British scientist, Robert Boyle, reported the density of a certain piece of a metallic substance of alchemical origin to be 25. No metal or alloy with such extremely high density is actually known, but no experimental mistake on his side can account for this surprising result, as in the same text he accurately reported the density value of gold, namely 19. The text is as follow. "... I was once possessor of a piece of Gold which was affirmed by the person it came from to me to have been made by projection... You will not hear without some surprise namely that this Gold was endowed with a considerable greater specific gravity or as some call it, Ponderosity, than the gold that I have met with either from Mints or among Refiners, for whereas good coined Gold does often weigh but between 18 and 19 times as much as common water that it is equal to it in Bulk, and I remember not to have found that even well refined Gold was Equivalent in weight to 20 times its quantity of the same liquor, I found that this Gold amounted to the weight of 25 times its bulk of water... " Indeed, Boyle used density measurements extensively to identify different chemical substances. We can but speculate on the nature of such metal-like object. There is a general trend for the density of chemical elements to increases with the atomic number, and taken into account the atomic number-density relationship of known elements, the metal studied by Boyle would corresponds to a transuranic or superheavy element. It would be interesting to determine, by using that density relationship, whether hypothetical nuclei belonging to the predicted nuclear "Island of Stability" would have density of 25. It is also interesting to remark that all authors who came in contact with samples of PS noticed its extraordinary high density, an observation that is frequently highlighted in alchemical texts. 3. Catalytic Pattern of Alchemical Transmutations In a typical transmutation by projection, several numerical parameters that described the processes are available. A certain amount of the PS (Wps) is added to a certain amount of a base metal having a weight of W-u contained in a crucible heated at temperature T. After a certain period of time t, the content of the crucible is removed, identified, and weighed (Wf), The reaction temperature T is just characterized but no measured, by expressions like "boiling quicksilver," "melted lead," and so on. The weight of the starting base metal W\ and the resulting noble one W{ are often reported, but the greatest difficulty in analyzing alchemical transmutations resides in the knowledge of the weight of the PS used and the duration of the transmutation experience. In many cases the use of small
556
quantities of PS is reported, but no weight is given. Taken into account all these comments, few of the recorded transmutation events detail the values of the four parameters. I have identified some years ago a set of eight different transmutation events that meet the requirements described. These events have been analyzed in a previous publication. 3 It has been observed that the duration of the transmutation spread over a large time interval. In some cases, the transmutation is described to take place "instantaneously," 6 while in others more than l h is required. Second, variations of several orders of magnitude of the weight ratio between the resulting noble metal and the PS are reported. This weight ratio can be defined as the "transmuting power" of the PS, and seems to be characteristic of every sample of this material. In other words, not every sample of PS has the same capacity to transmute into noble metal a given amount of base metal. In some cases, a minute amount is sufficient, while in others much larger amounts are needed. I have found new records of alchemical transmutations that contain sufficient quantitative information as to be analyzed in the same way as the eight prior examples were. Table 1 contains the characteristics of these new examples relevant for this study. These new cases under examination range from 1604 to 20th century. I wish to stress that none of these examples has been selected according to factors other than those under consideration here, and I have confirmed from different sources the accuracy of the data. This hold for the alchemical transmutation performed by the late French alchemist Eugene Canseliet in 1922 as well as for those carried out in India in the forties. The description of one of the alchemical transmutations performed in Delhi in 1942 is given as follow:11 "In the month of Caitra (name of the month according to the Hindu calender corresponding to March-April) of the Vikrama Samvat 1999 (1942 AD), one Sri Krisna Lala Rasa Vaidaya Sastri, originally hailing from Punjab came from Risikesa to Delhi to demonstrate the practical method of preparing gold out mercury. On this occasion, the secretary of Mahatma Gandhi, Sri Mahadeva Desai, Gosvami Ganesa Datta, and Sri Jugala Kisora Birla (the noted industrialist of India) were present. In front of them, 200 tolas or 2.5 seers (ltola is approximately 12 g) of mercury was mixed with 1 tola of the powder of a drug (identity undisclosed) and the whole thing was kept over fire for half an hour. Thereafter, the mercury became gold. This process was repeated, and as such 18 seers of gold was prepared." The new events have been plotted together with the old ones in Fig. 1. It can be observed that in most cases they are grouped around the values expected from the former set of data. Therefore, the transmuting power-time correlation seems to be reinforced by the new events. As can be seen in Fig. 1, there is an inverse correlation between the transmuting power of the PS and the duration of the transmutation. Very active PS samples require just few minutes to accomplish the transmutation, whereas for less efficient samples, its contact with the base metal contained in the crucible at high temperature should be longer.
Table 1. Ex.
Year
Reference name
1 2 3 4 5 6 7
1603 1627 1675 1675 1922 1941 1942
Seton P.J. Fabre Seyler Seyler Canseliet India India
Characteristics of alchemical transmutations. 1 ounce ~ 30 g; 1 grain = 0.053 g. Type of transmutation P b -> Au H g ^ • Ag
Pb -» Au H g ^ Au H g ^ Au
Wi
Wt
WPS
W{/Wps
Time (min)
References
3.5 ounces 1 ounce
3.5
0.5 grain 0.5 grain
-
120 g 12 g
4,000 1,100 1,000-4,000 10,000 6,000-4,000 96-64 200
15 30 Inst (<1) 15 1 45 30
7 8 9 9 10 11 11
12g 2,400
-
-
20-30 mg 125-187 mg 12g
558
The pattern described in Fig. 1 is similar to that generally found by conventional catalysts of chemical reactions. Highly efficient catalysts lead to high reaction rates, and are usually able to transform a large amount of the initial reagents. On the contrary, an increasing amount of catalyst is required to catalyse the transformation of a given amount of starting chemicals into products, and the reaction time should be often prolonged to achieve the desired transformation, as less active catalysts are used. Moreover, Ref. 3 describes independence evidences found in alchemical literature in support of this pattern.
10000 -
1000 -
100
-.
20000 «
lV/l^ps = 6310r 0 ' 8
15000-
> ^
•
100005000-
L
• *
©
'*~ "*"-~-~~~~"» 40
* 60
Time
80
100
(min)
Figure 1. Transmutation power vs. time. Top: Linear fit (full line) of reported data in a log-log plot and 95% confidence band (dotted lines). Linear regression of data has been performed using logarithmic scales for both transmutation power and time. The calculated slope, y-intercept and correlation coefficient were - 0.80 (standard error = 0.17), 3.80 (standard error = 0.20) and 0.83, respectively. Open symbols indicate data that were considered as outliers and excluded from the analysis. Bottom: Reported data (symbols) and fitted curve (line) using linear scales.
It is interesting to notice that such action of the PS on the base metals is consistent with the alchemical view on the evolution of metals. The alchemists conceive the transmutation as an acceleration of the ripening of base metals towards
559
the more perfect gold, which takes place in Nature by means of a slowly maturation process inside the Earth's womb. 4. Weight Variation Differences between the weight of the starting base metal and the weight of the gold (or silver) obtained at the end of the transmutation process are often noticed in the texts, but no satisfactory explanation for such observation has been given so far. Weight decreases are reported but, more surprisingly, weight increases are reported as well. The recorded weight variations are of ±20%, at most. It should not be forgotten that the transmutations are usually carried out in an open crucible, exposed to the surrounding atmosphere. Therefore, exchange of matter and energy can take place in the system unrestrictedly. Analysis of available data evidences
I 50 40 30 20 10
0 -10
A atwt.
A wl.
-1.7 -1.8 -4.8 82.6 82.6 -4.8 -2.4 -47.9 69.8 69.8
-0.2 0 0 20 20.1 0.1 -6 -23 25 16
-20 -30 -50 40 -30 -20 -10 0
10 20 30 40 50 60 70 80 90
Atomic weight variation (%)
Figure 2. Weight variation as function of the atomic weight. Numerical data on the right columns taken from Husson. 8 Dashed lined: atom-to-atom transmutation.
a consistent weight variation pattern, which is a direct function of the difference in atomic weight between the base and the noble metal (Fig. 2). According to the plot, whenever the starting base metal has an atomic weight smaller than that of the resulting noble metal, either gold or silver, then the weight of the noble metal is higher than that of the initial base metal. This occurs for example when copper is changed into silver. The opposite is found when for example lead (at. wt. = 207) is changed into silver (at. wt. = 107). In this case, a weight decrease is recorded. It has been also plotted in the figure the hypothetical variation of weight for atom-toatom transformation, i.e., every atom of the starting metal is changed into a noble metal atom. In this case, the value of the slope is just one. It can be noticed in the figure that the "experimental" slope is lower than one, i.e., the weight increase is
560
smaller than that expected for atom-to-atom transformation. This behavior makes the total atoms of noble metals present at the end of the transmutation to be smaller than the number of atoms present in the starting base metal, if an increase of weight takes place. This correlation suggests that nuclear fusion/fission events would take place simultaneously in an appropriate balance during the process. Moreover, the increase of weight must be due to reaction with atmospheric gases, and a fusion reaction should account for an increase in the number of nucleons when copper is changed into silver, for example. But, on the other hand, nuclear fission should also occur simultaneously, for some atoms should split off in smaller components to explain the decrease in the total number of atoms present in the system at the end of the transmutation. The opposite phenomenon is observed when a heavy nucleus of base metal is changed into a lighter one corresponding to either silver or gold. An appropriate balance of endothermic and exothermic nuclear reactions should account for a nearly zero energy balance, for no explosive release of energy is ever reported in the texts. Interestingly, an anomalous weight increase recorded 500
400
CD
300
200 0
1
2
3
4
5
6
7
Days
Figure 3. Alchemical experiment carried out by Canseliet.
in the course of an alchemical experiment non-concerning with transmutation has also been reported by the 20th century French alchemist Eugene Canseliet. 12 In his process, carried out in 1951, two substances of undisclosed chemical composition and weighing 4.15 and 160.55 g, respectively, were placed in a crucible (weight = 148.90 g) and heated in an oven at very low rate for 7 days, in such a way that after a week a temperature of 500°C is reached. The reported weight-time relationship is depicted in Fig. 3. A weight increase of 127 g is obtained at the end of the process. If we consider that the weight of the crucible, made of refractory earth, remains basically unchanged, then the initial substances increase their weight by nearly 80%. Only the air oxidation of light elements such as Mg or Al to form the corresponding MgO and A1 2 0 3 could account for such result. However, as this
561 experiment is claimed t o replicate the ones performed by Middle Age alchemists, I believe we could safely exclude the possibility t h a t b o t h elements were used by Canseliet. Indeed, no evidences on an early discovery and use of such elements have ever been reported by historians of chemistry.
5. C o n c l u s i o n s Alchemical laboratory processes involving the substance called Philosophers' Stone seem to follow specific activity patterns, which make alchemy appears as a consistent system of experimental practices. However, the behavior of this substance cannot be understood within conventional approaches to the ultimate constitution and properties of m a t t e r . It is believed t h a t this new approach to study the alchemical experimental procedures not only would shed new light on the true nature of alchemy, b u t might be useful as well in exploring new avenues in t h e transformation of matter.
References 1. W. R. Newman and L. M. Principe, Alchemy Tried in the Fire (University of Chicago Press, Chicago, IL, USA, 2002). 2. S. H. Giildenfalk, Sammlung von mehr als Hundert Wahrhaften Transmutationsgeschichten (J.G. Fleisher, Frankfurt and Leipzig, 1784). 3. J. Perez-Pariente, An investigation into the activity pattern of alchemical transmutations, J. Sci. Exploration 16, 593 (2002); Reprinted in Infinite Energy 10 (57), 10 (2004). 4. V. Karpenko, Coins and medals made of alchemical metals, Ambix 35, 65 (1988). 5. L. M. Principe, The Aspiring Adept. Robert Boyle and His Alchemical Quest (Princeton University Press, Princeton, 1998), pp. 261-262; Fragment 8 of Robert Boyle's Dialogue on the transmutation of metals. 6. J. B. van Helmont, Ortus Medicinae, 4th ed., 1667, p. 452. 7. E. Olivier, Bernard Gilles Penot (Du Port), medecin et alchimiste (1519-1617), in Chrysopoeia, Vol. V (Edidit, Paris, 1996), p. 627. 8. P. Jean Fabre, Alchymista Christianus, Tolosae, 1632, Quoted in B. Husson (Ed.), Anthologie de I'Alchimie (Pierre Belfond, 1971), p. 48. 9. J. J. Becher, Magnalia Naturae (London, 1680). 10. Atorene, in Guy Tredaniel (Ed.), Le Laboratoire Alchimique, 1981, p. 63. 11. Vaidya Bhagwan Dash, Alchemy and Metallic Medicines in Ayurveda (Concept Publishing Company, New Delhi, 1996), p. 23. According to the author, this text, written in Hindi, is inscribed in a marble plaque fixed in the wall of the yajna vedi (altar for the fire sacrifice ceremony) behind the Laksmi Narayana temple (also known as Birala temple) in Delhi. Dr. M. Srinivasan, private communication. 12. E. Canseliet, in J. J. Pauvert (Ed.), L'Alchimie expliquee sur ses texts classiques, 1972.
HISTORY OF T H E DISCOVERY OF T R A N S M U T A T I O N AT T E X A S A&M U N I V E R S I T Y
J.O.-M. BOCKRIS Molecular Green Technology, College Station, TX 77845, USA
1. Background Until 1989, I had been a publisher of high temperature physical chemistry, electrochemical and environmental research papers. I was a physical chemist and my contact with nuclear chemistry was only in using it in some tracer techniques. The Fleischmann and Pons announcement of March 1989 was of interest partly because of its radical nature, but also because I had known Martin Fleischmann since his days as a student at the Imperial College of Science and Technology in London. I had easy access to Fleischmann and I therefore could instruct my co-workers (about 20 at the time) about the technique used in the Fleischmann and Pons work. It was around 3 weeks before we were able to detect strong concentrations of tritium in the solution after prolonged electrolysis and thus prove, 1 for the first time, that the speculation which Fleischmann and Pons had made about their excess heat was indeed correct and that a nuclear reaction was occurring at or in an electrode in • the cold. We continued to work on the new nuclear phenomena, in 1991 discovering excess He 4 in our palladium cathodes. Later in 1991, I received a phone call from a Joseph Champion. He told me that the long initiation times which I had recorded in my papers could be avoided and that he could "turn on" what he described as a "radioactive gas" in less than 1 h. Champion invited me to visit his laboratory (which was in a trailer on the grounds of the University of Tennessee). I could operate his apparatus and see for myself. I asked Dr. Ramesh Kainthla and Mr. Omo Velev, senior researchers in my laboratory, to visit Champion and see if his statements could be confirmed. Upon return to Texas A&M, they told me that Champion had left them alone in the so-called laboratory, pointed to the apparatus, gave them a few instructions about turning it on, and left them alone. They measured 40% of the excess heat that he had said was obtainable. Earlier (1990) I had received a letter from a Roberto Monti. He complained that he had not got a reply from writing to Fleischmann and Pons and he decided to write to me instead. His letter concerned a theory which he said would easily rationalize the synthesis of tritium from deuterium and moreover indicate conditions under which many elements in the periodic table could be transmuted to neighboring elements in the cold. On reading the letter, I thought that the writer must be 562
563
elderly and out of touch with theoretical chemistry, for what he said was clearly impossible, indeed, it sounded like a claim to alchemy. I replied, humoring the writer and promised to meet with him in the forthcoming Cold Fusion meeting in Como in Italy (1991). When I met, Monti I was astonished to find that he seemed to be a bright normal person about 40-year old and speaking in a vigorous and seemingly informed manner. He had an established position in an Italian Research Institute in Bologna. His emphasis was not on the reactions which Fleischmann and Pons had carried out but on his own work where he claimed that he was able to carry out transmutational reactions. In spite of my impression that Monti was a normal scientist, I still regarded transmutation with extreme scepticism. 2. The Funding of Transmutation Work at Texas A&M University The next step was initiated by another phone call from Joseph Champion and this time he said that he had been looking for money so that he could bring his work to the University. His work, which he now claimed was metal-metal transmutation similar to Monti's (entirely independent) claim was at a stage whereby it needed independent confirmation. He had been working at a Mexican university for some years. He named a professor there with whom he had been collaborating. He had been to Merrill Lynch and asked if they knew of a client who had money to invest in a speculative venture and thus obtained the name of Mr. William Telander. I invited Champion to come to Texas A&M University and describe the work he had been doing. Champion turned out to be a big chap and looked more like a football player than a scientist. He had owned a laboratory in Houston, Texas, testing and repairing electronic equipment. He had a degree in electronics and no qualifications in chemistry or physics. He also told of experiments he had done relevant to a Hydrogen Economy. He had ideas about a process for the desalinization of sea water. Champion said that he had come across a method by which transmutation could be carried out. The method originated from a person called Keller who had lived in a small town in Washington state. Keller had worked after WWII with two colleagues and found he could make gold in ounce quantities. Troy Becker, one of Keller's colleagues, had been imprisoned on the allegation of making a false deposition. On release, he again had set up a laboratory to re-establish his work. However, a visit from the FBI told him he was not to research the production of gold, if he did he would again be imprisoned. Champion had taken a description of the process given him by Keller to the University of Gjanamantu in Mexico because producing gold in the United States was apparently unlawful. He had had some success. I asked and obtained his laboratory books. They were difficult to decipher being partly in Spanish. I called the Professor at the Mexican University. He seemed reluctant to describe his collaboration with Champion. The experiments had been done elsewhere and Champion had come to him only for the analysis. He had received powders with "before" and "after" written on the containing bottles. He certainly had found noble metals in
564
the "after" powders and none in the "before." He was skeptical, he had no evidence that the change was due to some process of Champion's. Champion said, in this first interview in my room at Texas A&M, that he had other ideas about how to bring about transmutation. It was not necessary to carry out the "thermal method" (later on called the explosion or impact method) which originated in Keller's laboratory. He then produced a folder which contained a minor thesis which he asked me to read. It was supposed to be the theoretical basis to an alternate, original method. But this was ideas only and had never been tried out. I studied the document. It contained much mathematical detail. However, I did understand where Champion was coming from. He relied on the fact that certain nuclei had quadrupole moments with frequencies in the range of chemical frequencies (~10 14 cps). By subjecting such material to radiation in the range of the quadrupole frequencies, he thought he would be able to obtain transmuted material, new species. Thus, the incident frequencies from instruments producing fields having frequencies overlapping those in the nucleus would cause the nuclei to absorb energy and this would build up to amounts which would cause nuclear fission to occur. a The meeting with Champion was then followed after some weeks by the arrival of Mr. William Telander, who had shown interest in having Champion's proposals tested out. He seemed to be a genial person, self-confident and relaxed. He lived in the Napa Valley in California and had inherited from his mother a chain of restaurants which he had sold.b This was the source of his wealth which he had invested mainly in Europe. Telander stated that he had an office in Zurich in Switzerland and I asked for its telephone number (I called it several times but was told that Telander was "on travel"). I explained to Telander the University system in respect to gifts. The donor had to assert that the gift was a free gift which Texas A&M could spend in any way it wanted. However, it was legal for the donor to state a preference as to how the money would be spent. The University, of course, respected the wishes of the donors in the hope that more support would come. Eventually US$100,000 came a Much later, around 1995, I came into contact with the Russian nuclear physicist, Kucherov, working at ENECO, a company in Salt Lake City which had originally been formed to continue the work of Fleischmann and Pons and in which I had brought shares at the foundation. He had published on nuclear reactions in the cold before he left Russia and now proposed (indeed) to carry out transmutational reactions by a method which seemed to me to be remarkably similar to Champion's. Of course, Kucherov had made a more detailed theory than that which Champion showed me. He sought to obtain the activating energy not from instruments producing electromagnetic fields (as Champion) but from the frequencies of hydrides which existed after saturation of Pd and other metals with H or D. I heard Kucherov proposing this at the Cold Fusion Meeting in Vancouver but I do not know of any realization of the work at ENECO (though I know it was tried out). b Later, in discussing possible support with an Investor in Boston, I mentioned Telander and he exclaimed "oh, the restaurant man." But my wife was skeptical of Mr. Telander's story because his shoes and watch were of a quality less than that expected for a wealthy man. We drove to College Station Airport one evening, but found a private jet described by Telander was indeed parked there.
565
out of the conversation and as Mr. Telander seemed so relaxed and so genial I promptly suggested US$200,000. He said "Fine." What we had to do then was to introduce the idea to the University. I went to my boss, Dr. Michael Hall, and told him about this "peculiar approach." We laughed about the ridiculousness of the idea of transmutation in 1992 but nevertheless, I convinced Dr. Hall that he should give support in the acceptance of the gift which we simply called "inorganic reactions" because I wanted to be able to apply the gift widely. Gifts at Texas A&M are dealt with through an agency which is separate from the agency which deals with the government grants. Gifts involving research have to be supported by the head of the department involved, and then finally the proposal goes to a Dean (in this case Dean Kemp) who accepts or rejects the funding. There is advantage in funding work in this way rather than through the channels traveled by the government grants because the overhead on the "gifts" is less (e.g. 5% instead of 33%). However, the donor cannot have any control over the use of the funds. There was a pause of about 6 weeks between Mr. Telander's latter formalizing the gift and the University's acceptance. Eventually, the Dean concerned said yes and we could go ahead. 3. Champion's Electromagnetic Excitation Experiments Mr. Telander put up Champion as the man who would do the laboratory work under my supervision and he was accepted by the University as a "guest worker" in spite of the fact that he did not have a degree in Chemistry. There then arrived a big computer programmed to give information on the nuclear properties of any element. Champion sought the frequency of the quadrupole oscillations which took place in certain nuclei. The other apparatus was an electrolysis cell in which the material Champion hoped to transmute was in the form of an electrode, opposite which, on either side, were the radiating plaques from which he sought to stimulate the transmutational reactions. It was about three weeks before we got everything going. In the following weeks, we were subject to claims from Champion who would come out of his laboratory (where he was working alone) and claim in an excited voice that he had a precipitate and this could be what he was looking for new species. We took samples of these precipitates for X-ray analysis and on one occasion seemed to see what resembled internuclear distances for gold. However, it did not replicate and I finally, after perhaps 12 months of trying, stepped in and told Champion, it does not work! Joseph Champion was frank in agreeing that he had not got anything out of his electromagnetic stimulation method. It is noteworthy that he had been left alone in this laboratory, the door was usually shut and had he wished to perpetrate a fraud, it would have been a most easy thing for him to have put something into the solution which he could have claimed arose from transmutation. Mr. Champion and his wife were living in a hotel, at Mr. Telander's expense (no salary). When he admitted that he had not been able to make his method work, it would have been possible, indeed expected, of Mr. Telander to say, "Well, I told you nobody would
566 Radiation April 21, 1992 250
200 -
E 150 -
o O
100
10
Figure 1.
15
20 25 Time (h)
30
35
40
45
/3-Radiation from a preliminary run of April 21, 1992 (negligible nobles).
believe it, now you yourself do not believe it so that's that. Get out." When he admitted the electromagnetic stimulation method did not work, Champion stated that he had a method which he knew would work because it had worked in the University in Mexico. This was what we later called the explosion method and which I later called the impact method. 4. The Impact Method Champion's outline of the impact method was simple. One took certain quantities (these are detailed below) of lead chloride and mercurous chloride, mixed them with potassium nitrate and graphite power, an explosive mixture, put the mixture in a coffee pot and set off a mild explosion by means of a propane flame. There were fumes, so the experiments were done in a fume hood. The temperature rose shortly for a few seconds and could be measured by means of an optical pyrometer. I had used these in early work in London and retained some sense of color and temperature. I estimated the temperature of the reacting mass to reach 1000° C for a few seconds but it is possible that there were sites within the powder where the temperature could have reached much higher. According to the method Champion brought from Keller, one then had to wait 3 days, after the explosion had occured. There was a certain backing for the fact that in the mixtures a decay of some nuclear process was taking place (Figs. 1 and 2). The lifetime of this decay corresponded to an isotope of platinum and we shall see below that there is some independent verification of the existence of this intermediate. The procedure was lengthy. The mixtures (compositions, see below) had first to be made and powdered. Then for about 1 h one had to kneed it in a pestle and
567
Thermal 13 December 9,1992
c 'E
& 2000 CO 4-»
c 3 o O 1500 0 Figure 2.
50
100
150
200
/3-Radiation from later run, December 9, 1992 (negligible nobles).
mortar and then shake the powder overnight. I had been cautious about the way the experiment would be carried out. I was suspicious: the claims seemed outrageous. The likelihood of fraud had to be considered. I reminded myself that Champion and his wife were enjoying hotel life at Telander's expense. It seemed prudent to suspect deception. Therefore, for the first experiments I donned a white lab coat and goggles, entered the laboratory and took the samples myself. I had tubes with rubber stoppers which contained about 20 g of the mixtures with which we had started before the explosion, and then corresponding tubes of the mixtures after the explosion, and the 3 day wait. I ended up with about 12 tubes because I was insistent that several analytical companies should be used. I speculated that wealth might be turned into "strong influence." But this was not going to be likely if the analysis was done in Australia or Canada or South Africa, and in these countries I had relevant contacts. I therefore arranged for the analysis to be carried out in a laboratory in Nevada, where a great deal of testing of minerals occurred; a standard analytical laboratory in Ottawa, Canada, the government CSIRO organization in Melbourne, Australia, and, for the second set of experiments, the Institute of Metallurgy in Johannesburg, South Africa (particularly used to analyzing ores for noble metals). I decided to exclude Champion from experiments aimed at replication of his impact method. I asked Dr. Guang Lin (an experienced physicist) and Dr. Ramesh Bhardwaj (an experienced chemist), both senior postdoctorals working with me on other projects, if they would devote half their time for a few months to working on
568 Table 1.
Summary of experimental results
Experiment Main results obtained in April-June 1992 Thermal 1 Thermal 2 Thermal 3 Thermal 4 Thermal 5 Thermal 6
Two times increase of P t was observed. One fire assay experiment showed the existence of visible Au 250—450 ppm of gold present in the product. An increase in Pd was also observed The weight of precious metal after cupeling from the chemical mixture with Hg was three to four times heavier than that without Hg, in the original mixture A large amount of gold, about 550 ppm was found The gold concentration in the product was about 178 ppm No gold was found in either experiment (with and without Hg in the raw material)
the "Philadelphia Project." 0 Zoran Minevski, a graduate student, also assisted in the experiments from time to time in the work. It is important to note the physical arrangements because they bear upon the possibility of fraud. Thus, the laboratories in which my work was carried out lay in a certain corridor in the old Chemistry Building of the Texas A&M University contained five laboratories on one side of the corridor and offices on the other. They were of varied sizes and the arrangements we made during the experiments was that Mr. Champion was not to enter the laboratories at any time. He occupied an office in the corridor while the experiments were ongoing. However, Mr. Champion certainly had a part in the experiments because Lin and Bhardwaj turned to him rather than me when they wanted advice as to the technique used. My part was supervision. I spent some time each day checking up on what was happening, examining lab book results, having discussions in my room with Champion, Lin, Bhardwaj, and later with Monti (see below). Minevski's contributions were sporadic as he had his thesis work to do. The preparation of the powder for ignition generally took about 1 day. The second day was the critical one in which the actual explosiond was carried out and then the resulting mixture was left in the fume hood for 3 days. During these days samples were taken and tested for radioactivity. In Figs. 1 and 2 are some plots we made of the j3 emission. The half-life came to about 18 h. Results of the experiments which were carried out in the first group have been described by Lin and Bockris and the following statement about six experiments corresponds to their account. 2 5. Unexpected Elements Six experiments, named Thermals 1-6, were performed in Texas A&M University from April 30, 1992 to June 15, 1992. The experimental results are summarized c
T h e project was named "The Philadelphia Project" because of the legend (later made into a movie) that during WWII a destroyer was levitated from Philadelphia Navy Yard to that in Boston. This was thought to be an impossible event, and as the attempt to realize alchemical transmutation looked to be something impossible it seemed a reasonable title for it. d Explosion is a big word for what was observed. The mixture in a coffee pot was placed in the fume hood and ignited with a propane torch. There was an audible WOOMPH sound and the mixture glowed red hot. About half of it was expelled from the coffee pot.
569
briefly in Table 1. Loss of about half of the material during the "explosion" has been considered in the table and the following text. 5.1. Thermal
1
This experiment was fired on April 30, 1992. The weight of chemicals in the experiment was 1671 g, and the chemical composition of mixture is listed in Table 2. Twenty-two grams of the raw chemical mixture (before firing) were sent out for analysis, and 1649 g of the mixture were fired using a propane-oxygen torch. The mixture after ignition burned with a yellow flame and the reaction appeared to die down in 3-4 min. The total product after firing was 783.4 g. Both the raw material and product were sent to Bondar-Clegg in Ottawa and to the CSIRO Laboratories in Melbourne, Australia for analysis. Bondar-Clegg used a fire assay and an ICP method. The CSIRO used ICP and atomic absorption. The remaining product was also analyzed by our team in Texas A&M University using a fire assay method, neutron activation analysis and absorption spectroscopy. In some runs precious metals were sought by additional methods, including XPS, EDS, ICP, and mass spectroscopy. Both the results from Bondar-Clegg and CSIRO showed no gold, and the analysis results by our team with different methods also showed no gold, except for a specific fire assay run where visible gold was found and verified by EDAX, 148 ppm of gold (with respect to the raw material) was observed by ICP measurement. Three pin-head size particles which had the appearance of gold were seen and one tested for Au (X-rays). The results from Bondar-Clegg and from CSIRO showed twice times increase in Pt in the fired product. An X-ray experiment also showed a Pt signal. Neutron activation in Texas A&M showed a small signal for Au and Ir. 5.2. Thermal
2
The Thermal 2 experiment was fired on May 22, 1992. The weight of the chemicals in the Thermal 2 experiment before firing was 1715 g, and the chemical composition Table 2.
The chemical composition of the Thermal 1 mixture.
Chemical composition
Weight (g)
Results from
C KNO3 S SiC-2 FeSO-4 Cd Hg 2 Cl 2 PbO Ag AgNC-3 Ni Pd
300 900 80 120 100 30 100 50 4.99 6.2 20 9.78
Johnson Matthey, 300 mesh, 99.5% Baker, 99.2% Spectrum EMScience, 60-200 mesh Chempure Johnson Matthey, 325 mesh, 99.5% Fisher, 99.98% Johnson Matthey, 99.99% Johnson Matthey, 100 mesh, 99.95% Johnson Matthey, 99.998% Johnson Matthey, Grade I Engelhart
570 Table 3.
The chemical composition of the Thermal 2 mixture.
Chemical composition
Weight (g)
Results from
c
300 900 80 120 100 20 100 50 4.9 20
Johnson Matthey, 300 mesh, 99.5% Baker, 99.2% Spectrum EMScience, 60-200 mesh Chempure Johnson Matthey, 325 mesh, 99.5% Fisher, 99.98% Johnson Matthey, 99.99% Johnson Matthey, 100 mesh, 99.95% Baker, reagent
KNO3 S Si02 FeSO-4 Cd Hg 2 Cl 2 PbO Ag CaO
are listed in Table 3. There are two differences between Thermal 2 and Thermal 1. The first is that CaO was used in Thermal 2 to replacement of Ni. The second is that Pd was not used. Although, the total weight of the chemical mixture 1715 g only 1655 g was used for the firing. The weight of the product was 849 g. Both the raw material and product were sent to three labs (Bondar-Clegg in Ottawa, Chemex in Nevada, and Mintek in South Africa) for analysis. The remaining products were treated by means of a fire assay method and analyzed in our laboratory in a similar way as used in Thermal 1. Chemex used a fire assay, ICP technique. The gold composition had increased from 0.3 ppm (with respect to the raw material) to greater than the detection limit (100ppm) in the product. Bondar-Clegg used a fire assay, ICP technique. The gold concentration increased from 0.12 to 450 ppm (with respect to the raw material) in the product. Mintek used four different methods to analyze the samples (see table below). The gold concentration increased from 4 ppm in the raw material to 420 ppm. An interesting feature is that an increase of Pd was observed in all three analyses. The increases of Pd were from 0.5 to 1.3 ppm by Bondar-Clegg, from 0.4 to 2.1 ppm by Chemex, and from 0.3 to 1.3 ppm by Mintek. The analytical results in our laboratory were the following. Three sets of experiments were performed. The first set used 126 g of product, and 0.4ppm (with respect to the raw material) of gold was detected. The second set use 131 g of product power, 253 ppm gold was detected. The third set used 481 g of product, 240 ppm of gold was obtained. Table 4.
The chemical composition of the Thermal 3 mixture.
Chemical
Weight (g)
Results from
Mineral 1 PbO C KNO3
100 20 150 450 30 20
Action mining Johnson Matthey, 99.99% Johnson Matthey, 300 mesh, 99.5% Baker, 99.2% Spectrum Fisher, 99.8%
S Hg2Cl2
571
5.3. Thermal
3
The next experiment, Thermal 3, used a component of mineral sand instead of pure chemicals. The mineral (Mineral 1) contained no (i.e. <0.1ppm) gold and silver. The total weight of chemicals in the Thermal 3 experiment before firing was 770 g, and the chemical composition is shown in Table 4. Thermal 3 was fired on May 27, 1992. On the same day, another comparison experiment was fired, which had the same chemical composition but contained no mineral. Thirty grams of Thermal 3 product and a comparison product were treated. The fire assay treatment from Thermal 3 products contained 3 mg of precious metal (50ppm), compared to 0.8mg of bead (13ppm) from a comparison sample. No further analysis of the Thermal 3 product was performed. 5.4. Thermal
4
Thermal 4 had the same chemical composition as Thermal 3 except that the mineral sand 2 contains 1.6 ppm of Au and 4.8 pm of Ag. The experiment was fired on May 30, 1992. The total weight of the mixture was 770 g. The product powder weighed 360 g. Part of the product, 100 g, was treated by means of the fire assay method. Visible gold beads about 47.3 mg, was obtained, which was equivalent to 1700 ppm of gold (with respect to the mineral sand). 5.5. Thermal
5
Thermal 5 was a repetition of the Thermal 2 experiment. The total weight of the chemical matrix was'1615g. The weight of the homogenized powder after ignition was 841 g. The fire assay, ICP method gave 178 ppm of gold (with respect to the raw material). 5.6. Thermal
6
Thermal 6 experiment had two independent parts. The first part was the same as Thermal 4, and the second part containing all the chemicals but no Hg2Cl2. The two parts were done in the same experimental conditions. Both parts were fired on June 8, 1992. However, the fire assay method gave no gold in either part of Thermal 6 experiments. The remainder of this paper does not originate in the paper of Lin and Bockris.4 6. Analyses The Nevada group used cupeling, a metallurgical method which attempts to isolate the actual metal concerned from the ceramic crucible in which it is formed. Second, normal chemical (wet) analysis. Third, spectroscopic analysis. A neutron activation analysis carried out in the reactor group at Texas A&M. Other methods were also used. For example, at the South African National Institute of Metallurgy used mass
572 Table 5.
Analysis of Thermal 2, carried out at the South African National Institute of Metallurgy.
Sample
Ru
Rh
Pd
Ag
Ir
Pt
Au
Method
NT-2A
<1
1.8
1.8
436
0.03
-
986
0.03
2.7
-
-
0.18
848 (719)
1.4
1.1
-
< 0.1
0.2
471
0.13
2.2
-
0.12
-
830 (642) (824)
A 0.3 g sample and N a 2 0 2 fusion, dilution and ICP-MS A 10 g sample, fire assay, P b collection. Pressure dissolution of prill,ICP-MS A 1 g sample and N a 2 0 2 fusion, Dowex 50Wx8 column separation (3x); dilution, ICP-MS A 1 g sample and N a 2 0 2 fusion, dilution, ICP-MS
0.85
0.01
493
0.08
< 0.1
15.8
0.02
0.34
-
-
0.03
8.4
0.78
<0.1
-
< 0.1
<0.1
<1
< 0.5
0.34
-
0.09
<0.1
0.5
0.07
NT-2B
<1
< 0.1
A 0.3 g sample and N a 2 0 2 fusion, dilution, ICP-MS A 10 g sample, fire assay, P b collection. Pressure dissolution of prill, ICP-MS A l g sample and N a 2 0 2 fusion, Dowex 50Wx8 column separation (3x); dilution, ICP-MS A l g sample and N a 2 0 2 fusion, Te/SnCl 2 precipitation and ICP-MS
spectroscopic, ICP analysis, (cf. results from the US Company, see below) as well as other methods were used. At Texas A&M we used ICP and fire assay but also neutron activation analysis. Occasionally, X-ray and electron dispersive analysis were used. There was some indication of a small amount of other noble metals, particularly in the South African National Institute of Metallurgy's results and these analyses are particularly significant because workers at this institute analyzed gold in ores down to 0.1 ppm. In the sixth experiment described, gold was found in five. In one, visible quantities of gold were found (tiny pinheads). About 0.01% Au is found in South African ores used commercially, but even 1 g/ton (1 ppm) is found to be of interest. The fruitful experiments were carried out between April 30 and June 15, 1992. Thus, the average experiment took around a week. There were sometimes pauses due to apparatus breakdowns, the 3 day wait together with the times used in sending and receiving samples from analyzing organizations used in some experiments. 7. Further Work The work paused in June 1992, but it was continued in an irregular way through February 15, 1993. Between December 2 and January 15, 1993, Dr. Bhardwaj
573
worked alone and carried out 11 runs. 6 In the meantime, and from about midsummer of 1992 to Christmas of 1992, the transmutation-oriented work was slowed by two factors. Lin and Bhardwaj had to return to their official projects and continued working on them to catch up with the time they had taken off in contributions to the Philadelphia project. However, there was another reason for the delay in further experiments to seek noble metals. We were interested more in the mechanism of what seemed to be happening than whether we got noble metals or not. We sought a meeting with Professor Joseph Natowitz of the Cyclotron Institute at Texas A&M University, an eminent nuclear chemist. Natowitz told us that one of the things we should be observing if the transmutation which we claimed took place, was 7-radiation. We therefore set out on a quest to detect 7-radiation in the fired product, but there we fell upon hard times because although people had been helpful in lending us nuclear detection equipment up that point, when it came to help with the gamma experiments, little was forthcoming. Eventually we did obtain a 7-detector from outside the university but detected only trace indicating 7-radiation from the products which, in some cases, did give /3-radiation. The later experiments carried out by Dr. Bhardwaj were negative and the question arises as to why the original experiments, were fruitful, could not be repeated. The cause may be the absence of the 3-day pause, but in my opinion there may have been a psychological component. Dr. Bhardwaj is a serious and studious man, and it is likely that he was offended by the secular ways of Telander and Champion. Thus, Mr. Telander, when in College Station, was fond of holding dinners which often were prolonged, wine being drunk copiously, and many people being invited, including Bhardwaj and Lin, but also some women friends of Mr. Telander. Dr. Bhardwaj saw these people in their enjoyment of alcohol, during which it is reasonable to suppose that some of the conversation would be deemed unfitting for the studious person. Bhardwaj may have thought that nothing claimed by Champion and the funder of the work we were testing could be true. Much later, Bhardwaj told us that he had reported details of the work to an FBI agent who had visited all concerned and who of course, held the opinion that the whole thing was a fraud. By December 1992 Bhardwaj may well have thought it embarrassing to have signed off on five experiments indicating noble metal formation from cheap metals and was not displeased when the later results (without the 3-day wait) were unsuccessful.
e
Two days per experiment! Dr. Bhardwaj was then working alone during the Christmas vacation. In these experiments, Bhardwaj looked only for gold and used local spectroscopic methods in the University so that pauses for sending and receiving the analyses were avoided. He appears not to haved used the 3-day pause as in the technique used by Champion. In fact, Bhardwaj's final position on the summer experiments had become negative during Christmas 1992 and some emotion had added to the caution he normally showed in his work. Thus, I recall his bursting unannounced into my office around February 1993. He threw a series of Lab Notes on the floor, saying angrily, "It doesn't work. See!"
574
8. Confirmatory Work There are only three independent workers which, to a degree, confirm the impact method as causing a nuclear change and this is the work of Filimov and Kobets 11 who presented their work at the Cold Fusion meeting in Vancouver (1998) where they showed that by causing an explosive compression of the powder, new isotopes could be found. Cau 12 reported a confirmation. A report from a US company (see below) offers some support.
9. The Successful Results of Summer 1992 Thus, experiments, in which due care was taken for the 3-day pause, did show an enhancement of the gold in three of them in concentrations of 100-550 ppm and there was evidence of small concentrations of other noble metals in another. The first two sets of results were confirmed by multiple and different methods of analysis carried out by various organizations. These organizations agreed in their analysis qualitatively, but differed quantitatively by up to 50%. There is a tradition among older mining engineers that if one explodes an ore there is an order of magnitude increase in the noble metals extracted from the ore. However, whether this is a transmutational effect or an effect of "shaking" of metals out of the ores, is not clear. Two of the four successful experiments were carried out with pure materials (no ores) showed that it seems unlikely that this explanation would be the basis of what we observed. There were repercussions of this work and it was attacked later in the local press in College Station and in Newsweek as a fraud. (Interestingly, when, later, I had multiple confirmation of metal to metal transmutation, the local newspaper did not find confirmation of the discovery it had pilloried to be interesting enough to report.) It seems fair to claim that in the summer of 1992 at Texas A&M University and in particular on May 22, 1992, the obtaining of noble metals from mixtures of cheap materials was observed. One cannot say "established," because this means that several groups would have to get the same kind of result. 8 As of 2003, what is now being called "The Monti Method" is said to have been confirmed in Italy and in Taiwan. The emphasis now is of course in nuclear waste remediation. One piece of information which tends to support the contention that noble metals were indeed transmuted from simple metals arose as follows. In June 1992, Telander and Champion took the process to a well-known company in the United States which deals only in noble metals production. The company agreed to carry out experiments themselves which would confirm or deny the validity of what had been claimed. I was lecturing in Australia at the time, but I was in contact by telephone with the people in College Station and learned that a week before the time I am just about to report, the instructions for the technique were given to the Research g
Much information on the details of related experiments is available in my archives.
575
Director at the company concerned. Now, I phoned this man from Auckland, New Zealand and asked him about the degree of success that he had had in testing out the experiments. He was very enthusiastic and said that it was remarkable, his researchers had succeeded using mass spectroscopy to identify the intermediate isotope which were present during the wait period. He appeared to be satisfied that the process worked. When I returned to the USA, however, I got a phone call from this man. On this occasion he said that this whole business of transmutation was nonsense and I should never report that there had been any verification of it by his company. I interpreted this as a political reaction of a company which lived by processing precious metals made from low grade ores. 10. The University's Reaction The reaction of the University to the Philadelphia Project was at first silence. I had told the head of the Department of Chemistry what we were trying to do and kept in touch with him by occasional talks. He had, of course, expressed high skepticism and made the reasonable condition that if we did obtain anything which could be published, it should first of all be replicated by another group. However, in November 1993, the quiet time was broken by the publication of a letter which a former employee of the Research Foundation at Texas A&M (let go by that organization) in the local newspaper, expressing disgust that "alchemy" was being practiced in a State university in 1993. Whether the employee actually believed that medieval alchemy (rather than a modern attempt to replicate it) was being practiced seems doubtful. She had been the assistant to a Dean of Science who had set himself up as a critic of the work. It is noteworthy that the letter was published 7 months after the work had stopped. The letter gave rise to much warlike drum beating. There were articles in the national press which hinted broadly that I, too, must be involved in a fraud. I consulted a lawyer and he told me that I should not deny allegations because my ability to sue those libeling me would disappear were I to become a public figure.11 Another matter which lead to the University's negative reaction arose from the fact that Mr. Telander invited Lin and me to visit Mexico city to present the work to a group of technical journalists. It was a 9:00 a.m. meeting in a hotel in which there were maybe 20 journalists present. Telander, Champion, Lin, and I gave brief, 5 min, presentations of the work that we had done and, e.g. I said that if metal to metal transmutation were confirmed, it would be a major innovative step in nuclear science and have consequences for the theory of the nucleus. The meeting lasted about 1 h (there was discussion) and then Lin and I returned to College Station. The Mexican press reported this meeting widely and the fact that I had made a statement about transmutation and that I was a professor at Texas A&M University was featured. This caused Dean Kemp, the Dean who accepted the h Thus, in US law, public figures, e.g. well-known politicians, can be libeled, but individuals are subject to the laws of libel.
576 40
30
"3 -5 20
• -Electrode 1 A -Electrode 2 I -Electrode 3
10
0 0
2
4
6
8
10
Time (h) Figure 3.
Iron formed from arching spectroscopically pure carbon rods.
US$200,000 which Mr. Telander had donated, to make a formal accusation against me for "misconduct in research." There was a kind of trial within the University in which my judges were four distinguished professors. I hired a lawyer and he took much trouble to study the case and provide me with a booklet showing the plus and minus of my case, what I might be asked and what would be appropriate answers to give and etc. The accusations against me were that I had "conspired" with William Telander to obscure the intention of the research related to be the Philadelphia Project. I was accused of exaggerating the research findings. The defense was based upon letters which had been exchanged between William Telander, Joe Champion, Michael Hall (the head of the Department of Chemistry) and me. One letter by Telander refers to the focal point of the research being "on the single phenomenon which has implications in the accelerated production of precious metals." This document, which clearly stated the object of the work, had been faxed to the Department Chairman on April 16, 1992, and it must have been therefore seen by Michael Hall. It has the official stamp of the Provost and Vice Provost of the University dated April 20, 1992, indicating that it had been seen by these officials. There were other documents between myself and the head of the department and I made clear to Dr. Hall that we were examining Champion's alleged process. Dr. Duwayne Anderson, the vice president in charge of research at that time came to watch the firing of one of the experiments. A memo dated August 10, 1992 from me to Dr. Hall informed him that we had produced more than 100 mg of precious metals in some experiments. The four distinguished professors which were set to investigate my handling of this research had done their job well (examined 1000 documents!) and used voice enhancement machinery to hear all elements of a conversation which took place between a reporter of the Dallas Morning News who came to investigate the affair,
577
Dean Kemp and myself. This was an interview which took several hours. One of the determining documents which the distinguished professors brought out was a rough draft in my own handwriting of a letter which I had written in a New York Hotel. It was a letter to Mr. Telander telling him he must not exaggerate the significance of the success we had had, that it was not commercial grade as yet, and etc. How the committee got hold of this letter draft, I do not know, but I found that a number of things were disappearing from my offices in the University at that time. I suppose people came at night and removed them and my letter draft to Mr. Telander must have been among them. This letter showed that I did not exaggerate the research findings but on the contrary pulled back Mr. Telander who indeed did want to hint that the artificial production of commercial amounts of gold had been would be possible.1 On January 31, 1994, there was a letter of "complete exoneration" from the committee of distinguished professors who had tried me. I was congratulated by a few people in the Chemistry Department, but a group in the Inorganic Division of the Department of Chemistry felt that the inquiry had not been broad enough and my true sin was that I had not exposed the work to peer review in an established journal (to attempt this would, of course, been useless because no one would have agreed that the results were possible). The latter group did not give up and a 2 year persecution of me began. It was based on the implied threat of an ad hoc Committee formed to investigate whether I had done anything which would justify firing me (recall that I was a tenured Distinguished Professor). I have told the principal story of this investigation in a paper. 10 At any rate, finally in May 1995 I received a rather cold letter from the Acting Provost saying that the Committee had decided (after a year of meetings) that I had done nothing outside the Rule Book of the University and that a "change of personnel" was not contemplated.
11. Later Experiments I have made clear that the successful experiments we did here were largely done during the summer of 1992, in April-June. In September, Joseph Champion and his wife left College Station and shortly after were started work in a Chicago facility. Their objective was to scale up the process up.
12. The Contributions of Dr. Roberto Monti Dr. Monti came over from Italy in May 1992 at Telander's invitation (and my suggestion) and worked with us during the summer experiments in which we got five experiments which contained some results which showed that a chemically assisted nuclear reactions occurred. Dr. Monti re-emerged, so to speak, in early February 1993 and said that he was certain he could produce new gold. I personally paid his fair to come from Canada to Texas and he arrived in February 1993. The last experiment which he performed is dated 27 February 1993.
578
Dr. Monti worked in the laboratory in collaboration with Dr. Bhardwaj.J However, all in all the result of their collaboration was disappointing. There were indeed blips of gold which we saw in those days and one mixture exhibited radioactivity, but there was nothing that we could claim compared with what we had in the summer. I therefore wrote to Nancy Meechum, one of Mr. Telander's lawyers, and told her that we had not been able to reproduce the experiments on which we had reported positively at an earlier time. 13. Intervention of the SEC in California Around March 1993, we were disturbed by alarming news, namely that the SEC in California had accused Mr. William Telander, of having used money given to him for investment by others in a way which differed from that which he had offered them. Up to this time, we had thought that the financial support from Telander came from his own pocket. However, we now learned that Telander had advertised a scheme in California that he could obtain high interest levels by using the process of arbitrage in Swiss Banks. If one is a person who has a million dollars to invest (and not less) one can go to certain Swiss banks and use currency difference for gain. For example, perhaps (whilst in Zurich) one bought a million dollars worth of gold in Hong Kong where the price was US$300 per ounce whilst the price in London at the time is US$301 per ounce so one could sell the gold bought in Hong Kong in London with a gain of a dollar per ounce of the gold. One can see that with million dollar sums of money to use in this way, one could make more money than by investments available in the USA (for this kind of process can be done repeatedly during a year). Directly, the University knew of the SECs suspicions, and we were told that the grant Telander had given the University could no longer be spent. There was, to Table 6. Time (h)
1 3 5 10
Values of iron in the carbon detritus after arcing: Series II
Electrodes
Weight of carbon
Iron (*K)
Iron in Carbon (ppm)
Weight of carbon (mg)
Iron (*K)
Iron in Carbon (ppm)
Weight of Carbon (mg)
Iron (*g)
Iron in Carbon (ppm)
24.5 79.1 140.9 a
3.43 9.62 1.1 a
140 121.6 8 a
30.3 83.6 142.7 a
1.4 22.8 4.5 a
46.2 272.7 31.8 a
25.1 86.3 a 286.1
1.94 15.0 a 39.9
77.3 173.8 a 139.5
a: Experiments not done. Jin a letter of August 6, 2003, Dr. Bhardwaj disputes my conclusion that in his "final" tests which he made of the impact method, the 3-day pause had been neglected. I find the number of runs which Dr. Bhardwaj claims to have made over the Christmans vacation of 1992 (11 in my memory; 16 in his) inconsistent with a 3-day pause.
579
my memory, US$48,000 left in the funds at this time and of course we had people hired whose salaries came from this grant. Luckily, the news arrived on a Friday at the end of the month when everyone had been paid. This gave me a month to find money for the researchers I was employing and whom I could no longer pay from the money which Telander k had provided. I was able to continue employment of my co-workers because of support of work on Transmutation by ENECO which was a company arising from the original Fleischmann and Pons work in Salt Lake City, and also I was permitted to use a small amount of EPRI money for continuing work on Cold Fusion (see Table 6). 14. The Conversion of Carbon to Iron In mid-1993 I knew that we had converted deuterium to tritium (this had been confirmed in 20-30 laboratories by this time). 1 I felt that there was some evidence in four or five experiments, that we did indeed get tiny quantities of gold and noble metals from lead and mercury. I wanted therefore to continue to probe the transmutation area but I did not want to do it in experiments connected with gold because it gave rise to such a furor of criticism, I thought the best thing was to change to another system. At this time Monti wrote to say that he himself had seen the conversion of carbon to iron. At first this seemed to me a most unlikely transmutation reaction. However, Monti claimed that not only he had seen this transmutation reaction work but also at the Baba Atomic Research Center in Bombay, India, work was being carried out in which they had seen not only iron but also nickel and cobalt formed from spectroscopically pure carbon. A postdoctoral, Sunderesen, from the Bhaba Mr. Telander landed in jail. There was a lot of legal language which was involved in the charges against him but it came down to the fact that he promised his investors to use their money in a certain sense and he did not use it in that sense. He was condemned to 4 years in jail. I have not met him since that time though I did have a telephone conversation with him after he left jail. As far as Joseph Champion was concerned, I saw him lastly in September 1992. On December 11, 1992, we had a call from one of Telander's secretaries who said "The boss is on the way. He's flying over. He's got big news for you." We met Telander at his private jet at the airport in College Station, took him back to the laboratory. He said he was dissatisfied with Mr. Champion's handling of money which he had put in an account in Mexico City which could be drawn on jointly by Telander and by Champion. It was of the order of US$100,000. He did not claim that Champion had done anything illegal with this but that he had withdrawn money unilaterally and that he had spent it on personal living and not new work on transmutation which Telander thought he was going to do. Telander devised a charge against Champion for some unfinished legal business which he had in Arizona. It was to do with the fact that Champion had signed a check on a bank account which he had closed and the check would not be paid. The next we heard of Joseph Champion was that he was in jail in Arizona, that he had agreed to the charge for a lesser sentence. Of course the fact that the two people who had worked with us were now both in jail, though for sins which were disconnected with claims of transmutation technology, was nevertheless a deadly blow because, of course, the story which spread was that Champion was a fraud and that he had been put in jail for fraudulent attempts to make artificial gold. Presumably, I was to be regarded as a fool who had be deceived by Champion's nonsense. 'I stopped counting when I reached 47 papers on tritium.
580
Atomic Research Center, Bombay, working with me, struck an arc between two spectroscopically pure carbon rods in water and after sparking interruptedly for 10 h, observed small amounts of deposits which Of course, one had to be sure about the iron content of the carbon rods before oreing and this we did by multiple analyses. There is no doubt that the iron which we analyzed at the bottom of the beaker was much more in quantity than the total iron in the spectroscopically pure rods. We did this with varying times of arcing and there seemed to be an increase of new iron with the time of arching. It depended on the oxygen content. One deoxyginated the solution, the reaction did not happen and we ended up, with the help of Dr. Lin, by suggesting the process of what was the following: 2 6 C 12 + 2 8 0 1 6 —• 6 26 Fe 56 + 2 He 4 . George Miley, the editor of Fusion Technology at this time had been a doubting spectator on the brink of the work on transmutation. I had a number of discussions with him and his attitude was to be interested but to say that he could not publish transmutation work because he would be soon be out of his job as editor of the journal. Gradually, however, Miley's attitude changed and, of course, as is now well known, he became a forefront person in research on transmutation reactions. He has published several confirmatory papers himself in which his own ability as a nuclear physicist has come to the fore. He has utilized more advanced methods, particularly determining the isotope abundance frequency of the new material, so that he is now (in the USA) a leader (because of his reputation in nuclear physics) of the new world of transmutation. 3 Finally, therefore, Dr. Miley did accept the paper by Sundaresen and myself. 15. Nuclear Reactions Inside Palladium Saturated with Hydrogen Zoran Minevski was a graduate student when I asked him if he would be willing to work on damage within palladium as part of his Ph.D. Thesis. He evolved hydrogen on palladium for several weeks and then examined the interior of the palladium at various depths. He removed the surface by argon ion bombardment and therefore was able to analyze by means of XPS surface and EDAX (deeper) the substances present inside the electrode. He varied potential, time, and temperature, and registered damage electron microscopically and by means of Normarski polarized light microscopy. We settled down to look at new substances observable as electrolysis proceeded. We understood that there would be deposits on the surface from impurities in the solution. We made an analysis of the solution by IPC and found that the new materials on the surface corresponded to those in the solution. We then examined what the EDAX had given us. This method penetrates deeper then XPS and hence avoids registering the surface impurities. Results are give in Table 7. This was still the days of skepticism in respect to transmutation in general. We asked ourselves whether these new materials had diffused into the palladium from
581 Table 7.
Concentration of impurities.
Elements at 1 fi depth (atomic %) Element
Virgin Pd Johnson Matthey ICP
Mg Ag Si CI K Ca Ti Fe Cu Zn Pt Pd
< 1.0 x 1 0 " 4 < 1.0 x 10~ 4 8.0 x 1 0 " 4 9.0 x 3.5 x < 3.0 < 4.0 4.5 x < 4.0 1.0 x 99.80
10~ 4 10"3 x 10"4 x 10"4 10"3 x 10"4 10"2
Present work EDS
* * * * * * * * * * * 98.10 ± 1.0
Electrolyzed Pd 3 weeks EDS
6.7 ± 1.0 1.9 ± 1.0 10.2 ± 1.0 3.0 ± 1.0 1.1 ± 1.0 19.9 ± 1.0 1.6 ± 1.0 10.5 ± 1.0 1.9 ± 1.0 4.2 ± 1.0 7.1 ± 1.0 31.9 ± 1.0
*Lower than measuring limit of EDS.
the solution but they would have had to diffuse several hundred angstroms, and this seemed inconsistent with known diffusion coefficients of metals in the cold. We worried about fissures in the electrode but again this would only have brought the same materials deep into the metal as we had seen from the surface impurities, the origin of which we knew. Finally, therefore, we came to the bold conclusion that Minevski had established that when one saturated palladium with hydrogen one did create new materials therein (Table 4). This was a discovery (1993). It resonates with the work of Kucherov in Russia, who reported something similar at the Cold Fusion meeting in Maui in late 1993. Kucherov had not named his "impurities" transmutation. We were prepared for it more than others because of the work we had done in finding tritium and helium; the work we had done on lead and mercury into gold and the observations of new materials from carbon arcing. The work we did with Minevski5 was a forerunner of much work done later by George Miley3 and his group at the University of Illinois and by the people in the University of Hokkaido in Sapporo, Japan, 7 ' 8 by Mizuno, Ohmori and Notoya. The work by these nuclear physicists was better than the work we had done earlier. They did isotopic abundance analysis on the new materials which we did not do, but we had made an ICP examination of the solution and this they did not do. Thus, at Texas A&M between 1992 and 1993 we were able to discover metal to metal transmutation, lead and mercury to gold and noble metals, iron from carbon and (widely confirmed) palladium into various metals. 16. Joseph Champion's and Roberto Monti's Contributions Joseph Champion is, of course, a black sheep because of years wasted in jail. However, much he owed to Keller, it is true to say that the outburst of work on trans-
582
mutation in the cold, which has by now is occurring worldwide, was triggered by the work we did at Texas A&M in 1992 and that would not have been carried out without Champion's persistence and Telander's curiosity (although cf. out earlier 1989 finding of tritium from deuterium). The part played by Roberto Monti was seminal in encouraging me to take up what seemed at the time a most unlikely research project. Monti was a credited physicist and his intellectual influence on me was more than that of the claims of Champion and the funding of Telander. The early work of Lin, Bhardwaj, Sundaresen, and Minevski must also be recognized. They dived into very rough water and contributed at a time when admission to be working on transmutation attracted ridicule and vitriolic articles in the press. 17. Kevin Wolf's Work I went to a cold fusion meeting in Nagoya in Japan in late 1992 and at the meeting there I heard about work by Kevin Wolf of the Cyclotron Institute at Texas A&M. The rumor was that he had observed new radioactive isotopes in one of his electrodes after prolonged evolution of deuterium thereon. The difference between the Kevin Wolf work of December 1992 and the work which I did later with Minevski (1993) was that the Kevin Wolf new elements were radioactive whereas ours were not. The radioactivity of the materials claimed by Kevin Wolf made it easy to analyze and there was a visit by Tom Claytor from Los Alamos to Texas A&M to discuss mechanism with Kevin Wolf and also work done at Los Alamos, using gamma ray analysis, to identify the new isotopes in Wolf's electrods, obtained, it was stated at the time, by electrolysis. This seemed to be a powerful piece of evidence for transmutation in metals. Indeed, for a time Kevin Wolf's announcement had more effect than ours for Wolf was an established nuclear chemist. Indeed, there was another factor: we were prohibited from publication of our results from the summer 1992 work because Telander had made us sign an undertaking not to publish the work for 3 years. Kevin Wolf also decided not to publish his work. He talked of a letter he had from Tom Schneider, his program manager EPRI, in which there were given seven reasons for not presenting the work at a Meeting. But the reticence of Wolf naturally raised questions and one questioner was Tom Passell, a Program Manager at EPRI. Tom took an interest in Kevin's work and indeed he was the first person to present it in the cold fusion meeting in Monte Carlo in 1995. There was, of course, a question about Tom Passell presenting something which had been carried out by someone else. Apparently, he had a legal right to do this as the work belonged to EPRI, the sponsor and, of course, could not be kept secret. I invited Passell to re-present the work in the first transmutation meeting I held at Texas A&M in 1995. This all went into the background as the years went on and I assumed that Kevin Wolf had indeed been No. 2 in the observation of metal to metal transmutation. However, Tom Passell had suspicions about Kevin Wolf's work. These were based upon his reports to EPRI, which were never published, and it appeared that in them he had described how he got these radio elements in more detail. Passell had
583
come to the conclusion t h a t it was doubtful t h a t Wolf had got t h e m by evolving hydrogen or deuterium on palladium b u t instead by classical radio chemistry. One would have simply to irradiate t h e palladium in a certain way and t r a n s m u t a t i o n would indeed take place in a textbook manner. In fact, in 2003, Passell carried out such radiation and got the very same new radioactive elements as Wolf had seemed to have obtained by means of electrolysis. Did Wolf intend t o deceive or was he bent upon a charade, it being revealed at a time of his choosing t h a t the elements came into existence by classical means? At any rate, at present, Wolf (who died in 1997) is still thought t o have been No. 2 in the discovery of transmutation in the cold. Passell will probably not bring to light his recent findings.
1 8 . T h e M e e t i n g o n T r a n s m u t a t i o n at T e x a s A & M U n i v e r s i t y in 1995 My colleague Dr. Guang Lin was keen on extending knowledge about workers in other countries who were following us in getting results indicating t r a n s m u t a t i o n in the cold. I went to my boss who at t h a t time was Professor Emile Schweikert. He readily agreed to an international meeting on the subject being held in the Chemistry Department at Texas A&M. Im glad to say t h a t when he was later criticized for allowing the meeting, he stuck to the t r u t h and agreed t h a t he had indeed sanctioned the meeting. We came u p with a list of invitees and got no refusals to present. T h e principal people whose papers we finally heard were as follows. (1) Tom Passell, who presented the work of Wolf as though they were Cold Fusion experiments. (2) Ohmori from the University of Hokkaido in Japan who reported finding iron on the electrode surface during hydrogen evolution. He had analyzed the isotopic distribution of the iron isotopes and found that the Fe /Fe was much great than that of the natural ratio. (3) John Dash from Portland State University reported experiments which are qualitatively similar to those of Ohmori. He analyzed his palladium cathodes by SEM and determined that after evolving H2 on there, silver and cadmium were present in spots on the palladium surface. Large concentrations of gold were also found in dendrites protruding from the platinum. (4) Kucherov reported experiments which he had carried out in Moscow with Karebut and Savatimova. He was cautious in claiming that he had observed transmutation but finally in the end said he could find no other explanation. However, he made no attempt to distinguish the impurities on the surface, from those in the solution and no attempt at isotopic abundance measurements. (5) Notoya from the University of Hokkaido presented results which suggested that calcium had been formed from potassium during aqueous electrolysis experiments. (6) Rabzi from the Ukranian Academy of Sciences presented transmutational results which bore some relationship to those which we had done earlier in collaboration
584
with Champion. For example, he heated rapidly lead (99.5% pure) and found that this yielded several different elements including 0.2% of gold. (7) Mizuno applied high current densities to a ceramic at about 500°C and not only produced excess heat but also new materials including Al, Bi, Sn, Gd and Dy. He measured the isotopic abundance ratios and found them to be significantly different from the natural ones (Refs. 7 and 8). (8) A contribution from Monti described the suppression of the radioactivity of thorium oxide. Monti's method was similar to the method worked on in the summer of 1992. He could reduce the activity from 900 cpm to about 100 cpm in 4 days of a series of sudden heatings. Possibilities of de-naturing radioactive wastes appears and have been further developed by Monti and separately by Hal Fox (2003). T h e meeting at Texas A&M in 1995 was marred by an event which showed the hostilely of certain Professors in the Chemistry Department. On the second day of the meeting Professor F.A. Cotton accompanied by two colleagues, approached the meeting, showing anger, and made unplesant comments calling the participants at the meeting "all gooks." This was unfortunate because the two people who were standing outside the lecture theater and to whom Professor Cotton apparently addressed his remarks were Professor Hagelstein from M I T and Dr. Ward, an employee of the Department of Energy, who made a speech at the meeting indicating t h a t he thought the D O E would fund some work of this kind. I was due to go t o Australia directly after the meeting but nevertheless did write a letter to the President of the University complaining about Professor Cotton's interruption. 19. T h e M e e t i n g o n T r a n s m u t a t i o n in C o l l e g e S t a t i o n in 1 9 9 6 Lin and I thought t h a t it might be a good idea to hold a second meeting on transmutation, particularly as interest in the subject seemed to be growing. I once more approached the Department Head, Professor Emile Schweikert again but by now the rules had changed. Our colleagues in Chemistry h a d decided t h a t requests for such a meeting should pass through a committee which consisted of 12 members of the department. I duplicated a comprehensive review of cold fusion by Ed Storms which contained more t h a n 100 references and h a d a copy distributed to each committee member before the meeting. I made a brief presentation saying t h a t this was new work and t h a t it was going on around the world, there had been a number of confirmations of new nuclear reactions. I hoped t h a t they would allow the new science to be heard. T h e voting was 12 to 0 against. I called one of the people on the Committee I had known longer t h a n some and asked him what the discussion had been about after I had left the room. He said t h a t everyone on the committee knew t h a t it was impossible for nuclei to be changed except under conditions of very high energy exchange. Hence, the members had concluded t h a t the work t h a t I wanted to have presented was either a joke or a fraud. We held the meeting in the local Holiday Inn. Because of the assault made by Professor Cotton and his colleagues on the first meeting we thought t h a t a more
585
violent one might be made in this meeting and therefore hired a deputy from the police department to be present outside the door of the meeting in order to quell any attempt by members of the Chemistry Department to suppress the presentation of new ideas by violence. The papers of '96 meeting have been published in the Autumn edition of New Energy of that year. George Miley co-chaired the meeting with me. Monti was present and attacked one of the speakers with a vigor which was thought to be too strong. Mizuno and Miley presented papers which supported the work Minevski and I had done and thus made the likelihood that transmutation in Pd-H systems is highly probable. Many members of this second meeting expressed disgust at the refusal of the Chemistry Department Committee to allow them to present their papers in the University, a clear example of the suppression of new ideas. 20. Transmutation in 2003 The meetings of 1995 and 1996 at Texas A&M in College Station, Texas were pioneer meetings. Transmutation of metals has spread around the world and is now an accepted part of the so-called cold fusion science. Transmutation work is particularly carried out in Russia and Japan. The most remarkable addition to the transmutation work is that being carried out at Mitsubishi Inc., where a million dollar laboratory has been built and a number of interesting transmutational results have been confirmed. There seems to be financial support for an investigation of nuclear waste remediation by an electrochemical approach. 21. Concluding Remarks The work described in this paper is of interest not only for the pioneer character of the results obtained (and the complex steps by which a new field came to be) but also because it is an example of the need researchers have to attack their research with an independent mind, not bound by knowledge of the past. Science has an always moving frontier. It is the duty of all research scientists not only to look ahead but to step over the boundary which denotes the frontier of the time.™ Acknowledgments I, first, thank Roberto Monti for having suggested to me (1990) that transmutation outside the hydrogen isotopes (cf. my publication of 1989 on tritium) might be possible, and Joseph Champion for having brought to my laboratory a method for obtaining transmutation. I thank Mr. William Telander for the support, about US$140,000 of which was used in the research (the remainder is with the Univerisity). My postdoctorals Bhardwaj and Lin were courageous in agreeing to devote m
M y attitude is not held by all scientists. For example, I received a letter (1993) from a Professor in the Inorganic Section at Texas A&M. I was advised that if I were able to regain credibility after what I had published, then I should be careful to stick to what is in the book in my future researches!
586 half their time over about 7 months in the investigations. Dr. Bhardwaj worked further for about 1 m o n t h with Dr. Monti in 1993. Several other students (in particular Nigel Packham, Jeff Wass and Zoran Minevski) worked on the foregoing work on hydrogen isotopes: Some postdoctorals were involved, particular Dr. Ramesh Kainthla and Dr. Dalibor Hodko. Dr. Sunderesen worked on it too but he also worked on the carbon to iron transmutation. All are to be duly thanked. References 1. N. Packham, K. Wolf, J. Wass, R. Kainthla, and J.O'M. Bockris, J. Electroanal. Chem. 270, 451 (1989). 2. G. Lin and J.O'M. Bockris, J. New Energy A u t u m n , 27 (1996). 3. G.H. Miley, in: F. Scaramuzi (ed.), Proceedings of the Eighth International Conference on Cold Fusion (Italian Physical Society, Bologna, Italy, (Lerica), 2000), Vol. 1, p. 419. 4. R. Sundaresen and J.O'M. Bockris, Fusion Technol. 26, 261 (1994). 5. Z. Minevski and J.O'M. Bockris, Infinite Energy 5 / 6 , 67-68 (1995). 6. J. Kucherov, I Karebut, F. Savatimova, and J. Kucherov, in: Proceedings of the International Conference on Cold Fusion (Maui, 1993). 7. T. Mizuno, T. Ohmori, K. Azuni, T. Akinoto, and A. Takahashi, in: F. Scaramuzi (ed.), Proceedings of the Eighth International Conference Cold Fusion, 2000, Vol. 1, p. 279. 8. T. Omari and T. Mizuno, in: Proceedings of the Seventh International Conference on Cold Fusion (Vancouver, 1998), Vol. 1, p. 279. 9. T. Passell, Private Communication, June, 2003. 10. J.O.-M. Bockris, Accountability Res. 8, 103 (2000). 11. V. Filimov and V. Kobets, in: Proceedings of the ICCF7 (Vancouver, April 1998), p. 56. 12. M. Cau, Paris, Private Communication.
C O N C E R N I N G T H E MODELING OF SYSTEMS IN T E R M S OF Q U A N T U M ELECTRO D Y N A M I C S : T H E SPECIAL CASE OF "COLD FUSION"
MORTEZA ABYANEH School of Science and Environment, Coventry University, Coventry CV1 5FB, UK MARTIN FLEISCHMAN Bury lodge, Duck Street, Tisbury, Salisbury, Wilts SP3 6LJ, UK EMILIO DEL GIUDICE IN FN, Via Celoria 16, 20133 Milano, Italy GIUSEPPE VITIELLO Department of Physics, University of Salerno, Salerno, Italy A question we are asked repeatedly is: "what are the causes of the opposition to your belief in the reality of the phenomenon of 'Cold Fusion' ?" This question is normally asked in the context of the statement that according to the conceptual framework of quantum mechanics this phenomenon should be impossible (a view which we share). Our answer has always been based on the question: "but what about the modeling of such systems in terms of the conceptual framework of quantum field theory (QFT) [in particular, Quantum Electro dynamics (QED)]?" This is always met by the insistence that quantum mechanics shows that "cold fusion" is impossible. We conclude that most scientists do not understand that quantum mechanics is only a semiclassical approximation to QFT. This pointless dialogue* and the insistence on the primacy of Quantum Mechanics (as opposed to QFT) in the modeling of the systems in the Natural Sciences, Diagram 1, is unfortunate because it obscures the investigation of systems in the more normal fields of the Natural Sciences, Diagrams 1 and 2 (these systems were investigated both prior and after the start of work on "cold fusion," see also the systems discussed in Ref. 1). A brief indication of the work which has led to the formulation of the concept of QED coherence is given in Appendix A under the aegis of the revolutions in our understanding of the Natural Sciences which has taken place since the latter part of the 19th century. In the main part of the text, we will indicate how the choice of suitable systems (here the study of (ii) the kinetics of nucleation and phase growth on microelectrode a
Perhaps, more correctly described as two monologues conducted in parallel. 587
588 QED in chemistry Prior to 1989
Suppose this is also true for nuclear physics
(i) Kinetic of fast reaction in solution at short space times (1960)
t I
(ii) Kinetics of nucleation and phase growth (1965-)
(iii) Voltage-gated transmembrane ion currents (1975)
Compression and shear of metal lattices, Bridgman 1930's "cold explosions"
Coherent and k, incoherent structures
t 4
(iv) Wall-phase turbulance (1978)
Compression of metal deuterides
t7
(v) Surface x-ray diffraction ( 1 9 8 0 ) /
I
Use of eV perturbations to create structures at the GEV level
Chemistry
Diagram 1. The scheme of research, which lead to the start-up of the "cold fusion" project.
substrates, 2 ~ 7 veloped from in solution at can be found found in Ref.
Diagram 1) allows us to make direct comparisons with concepts deQ E D coherence (brief comments on (i) t h e kinetics of fast reactions short space-times and (iii) voltage-gated transmembrane ion currents in Refs. 8 and 9). Comments on (v) surface X-ray diffraction can be 8.
Post-1989 (vi) Ionic solutions
(ix) Surface enhanced Raman spectroscopy (SERS)
(vii) Cyclotron resonance of electrolytic conductivities
(x) Emergence of mind from living matter
(viii) Catalysis
(xi) Glasses (xi ) Enzymatic activities
Diagram 2. Topics interpreted in terms of QED after March 1989 (the announcement of the work on "cold fusion").
Figure 1 illustrates the initial stages of the deposition of an incoherent deposit during the nucleation process and the subsequent development of coherence. According to the concepts set out in Appendix A, the very initial step (the deposition of t h e first a t o m or molecule) must follow t h e q u a n t u m mechanical (non-coherent) paradigm (the number of species is fixed at JV = 1 and
589
/"\ O
^
/"S %J
/"% w
7
w? mw mw^ww
Development of coherence ^
z
Incoherent deposits Figure 1. A possible model illustrating the deposition of an incoherent deposit during the initial stages of the nucleation process and the subsequent development of coherence.
the phase is indefinite). This will also be true for a number of the succeeding steps whereas coherence will develop in the later stages. b It is important here to contrast this view of nucleation and phase growth with the conventional view based on the classical and quantum mechanical paradigms. In the conventional view, the surface energy is regarded as being continuous down to atomic dimensions and nucleation is regarded as being controlled by the difference in surface energies of adjacent states, see Fig. 2 (see e.g., Refs. 11-13). With numerous approximations, we obtain a first order rate constant governing nucleation (i.e., the plots labeled k = 0 in Figs. 6-8). On this view, phase growth is governed by a further rate constant. By contrast, the concepts developed from QED show that phase growth is due to the development of coherence. The development of the use of microelectrodes (here the circular cross-sections of wires embedded in insulators) with typical areas in the range 1 0 - 8 to 1 0 - 6 cm 2 allows us to study the statistics of the birth of the first nucleus of the new phase. Figures 3 and 4 illustrate the formation of the first center of the new phase of aPbC>2 on a circular substrate of 5 x 1 0 - 7 cm 2 formed from a carbon fiber embedded in glass. The deposition of a-Pb02 is a slow reaction, 2 ' 3 ' 5 ~ 7,14 and, in consequence, the subsequent growth of the center is kinetically controlled, Fig. 4 {ill2at). Data of this kind allow us to investigate the statistics of the birth of the first nucleus. The interpretation can be based on the solution of the relevant master equations; 5 we have found that the most useful methodology is the direct simulation of the experiments using Monte Carlo methods 5 - 7 although it has also proved useful to investigate limiting patterns of behavior. Figure 5a illustrates the general birth and death model which should apply to the model of nucleation formulated according to the classical/quantum mechanical models of nucleation while Fig. 5b illustrates the pure birth model of this process. b
T h e description given in Fig. 1 should not be taken literally. The important point is that there is no long-range order in the initial stages of the deposition; this long-range order can only develop in the later stages.
590
{rrlri) Figure 2. Plot of 8(Ag)/zer) vs. ( n / n * ) 1 ' 3 for three-dimensional nucleation according to the classical/quantum mechanical paradigm Here S(Ag) is the electrochemical free energy difference between adjacent states and n* is the number of species in the critical nucleus.
In each case it has been assumed that A3 is much larger than the previous rates of birth (or death) so that phase growth initiates at this stage. It has been argued that if nucleation is studied at very high overpotentials (as applies to the systems /(nA)
f(s) Figure 3. The initial stages of the deposition of a single center of a - P b 0 2 on a 8 /im diameter carbon microelectrode at an overpotential of +400 mV. Solution composition: 1 M sodium acetate, 1 M acetic acid, and 0.1 M lead acetate.
591
/ 1 / 2 /(nA) 1 / 2
f(s) 800
900
1000
1100
Figure 4. The data in Fig. 3 plotted as i 1 / 2 versus time t (the linear plot represents the kinetically controlled growth of a single center of a - P b 0 2 ) •
investigated here), then the rates of birth will greatly exceed the rates of death so that we can restrict attention to pure birth models. It will be evident that the model of Fig. 5b should apply to the initial stages of nucleation according to the QED paradigm (Fig. 1) and that this is also equivalent to the Monte Carlo calculation for an infinite set of simulations.
A
(a) Spontaneous growth
x. (b) Spontaneous growth Figure 5. Models for the formation of a single cluster on a microelectrode substrate: (a) by a "birth and death" process; (b) by a "pure birth" model with identical rates of birth at each step. In each case it has been assumed that A3 is much larger than the preceding rates, AQ, A I , and A2.
592
As is well known the pure birth model can be solved exactly (step-by-step) giving Pfc(T) =
^ f
exp(-Ai),
(1)
where Pk(T) is the probability of observing a cluster of size k at time t. The probability of forming a cluster of size greater than k (the size of the critical nucleus being k) in a given time interval 0-t is then given by E ^ ) fc+1
= l-E^exp(-Ai). 0
(2)
•>'
Details of the Monte Carlo simulations have been given elsewhere. 5-7 The nucleation processes of Ag and Hg (which have also been studied here) are fast processes and the subsequent phase growth is close to diffusion control {iat1/2). It is of interest that the classical mechanism of nucleation has not been found to hold (i.e., k = 0) in any of the systems so far studied (a-PbC>2, Ag and Hg). Instead we see that the mechanism predicted by QED holds for a-PbC-2 (with critical cluster sizes 2 and 8 in different potential ranges, Fig. 6a, b), Ag (with critical cluster sizes of 1, 3, 5, and 6, Fig. 7) and Hg (with critical cluster sizes of 1 and 3, Fig. 8). The linear-linear plots (Fig. 9) are better representations of the fits to the model than are the double logarithmic representations (Fig. 6) and the linear representations have also been used for the cases of the nucleation of Ag and Hg (Figs. 7 and 8). We note that the Monte Carlo simulations (100 nuclei at each potential for the case of a-Pb02, 400 nuclei for the cases of Ag and Hg) are in close accord with the "pure birth" model (effectively an infinite set of simulations) for the cases of a - P b 0 2 and Ag so much so that we must conclude that the "noise" generated in systems
Figure 6. (a) Comparison of \nJ2t+l Pj(T) versus ln(T) as given by the model of pure birth with the experimental data for the formation of 100 nuclei of a - P b 0 2 at r\ = 340 and 400 mV. (b) Inclusion of the data for nucleation at r/ = 380 mV (if) in the results shown in (a) with the assumption of an increase in the rate of electrocrystallization following the birth of the nucleus. 6
593
ZP/7) k+ 1 '
Figure 7. The formation of 400 nuclei of silver at 77 = - 2 0 0 m V (k = 1), - 1 9 0 m V (fc = 3), —180 mV (fc = 5). Comparison with the models of pure birth.
following the QED paradigm is less than that which would be predicted by the classical/quantum mechanical paradigms. 6 ' 7 There appear to be some significant deviations from the "pure birth" model for the nucleation of Hg, which may be attributable to kinetic complications for the deposition process of Hg. 1. Some interim conclusions The work, which we have described on the nucleation of three systems, should be regarded as a first step in the modeling of these processes in terms of the QED
Figure 8. The formation of 400 nuclei of mercury at rj = - 2 0 0 , - 1 8 0 , - 1 6 0 , and - 1 4 0 mV (k = 1) and at 77 = - 1 2 0 and 80 mV (fc = 3). Comparison with the models of pure birth.
594
paradigm. In particular, we have not defined the transition from the incoherent to the coherent state, c we have not as yet explained the low "noise" of systems following the QED paradigm; the range of systems and the range of conditions studied in each system is very restricted, etc. We estimate that we would need to publish ~25 papers in this area alone and that the situation is broadly similar for any of the other topics listed in Diagrams 1 and 2. This is a task beyond our means. d Nevertheless, we believed that we had laid one of the foundation stones of this subject area by 1983 and, in that year, we decided to embark on the most extreme application of QED, the question of whether we could induce nuclear transformations of D + compressed into Pd lattices. It is important here to note that we posed two questions at the outset: (i) Would the nuclear transformations of D + in such host lattices be different to those observed in low-density plasmas? (ii) Would we be able to obtain definitive information about such processes? It is important to note that we expected the answer to (i) to be "yes" but that we also expected the answer to (ii) to be "probably not." However, the outcome ran radically against our expectations.
1
0.8 P
a: "D C
to
£
0.4
0.2
5
10
15
20
Figure 9. The linear-linear plot representation of the data in Fig. 6a and b for nucleation at r) = 400 and 340 mV; Comparison with pure birth models for k — 2 and 8.
c
Work on the transition for the deposition of a-PbC>2 at an overpotential of +380 mV shows that it should be possible to define conditions, which would allow the mapping of such transitions. d Particularly when we recall that publications invoking the QED paradigm are strenuously opposed by Referees, Journal Editors and the Scientific Public at large.
595
Pd wire
Glass Figure 10. Schematic of Coehn's original experiment 1 6 for measuring the electrodiffusion of hydrogen along a palladium wire.
10
20
30
40
50
60
70
Zeil (Stunden) Figure 11. Some of Coehn's original results showing the effects of negative and positive potentials in increasing the velocity of electrodiffusion along the length of the wire.
2. Some comments on "Cold Fusion" The work discussed in the first part of this paper has been outlined to illustrate the fact that the work on "cold fusion" was not undertaken in an intellectual vacuum.
596
This is all the more true when we consider the background more directly relevant to this topic. Diagram 1 illustrates that we were aware of the work carried out by Bridgman in the 1930s and early 1940s.15 Bridgman found that the energy stored in a lattice by intense shear and compression could be released in "cold explosions" in which the stored energy was converted into the kinetic energy of fragments of the lattice (powders). We believed (and we still believe) that such a process can only be understood within the framework of QED and regarded this work as the true antecedent of this field of study. 6 The second factor relevant to the topic of "cold fusion" was our knowledge of the work of Coehn on the electrodiffusion of hydrogen in the Pd lattice. (Deuterium had not yet been discovered at the time of Coehn's investigations of this topic. 16 ' 17 ) Figure 10 illustrates these original investigations. Figure 11 shows some of Coehn's original results. Hydrogen deposited electrolytically at the center point could be made to move more rapidly than by diffusion alone towards the apices of the zigzags of the wire framework by applying a negative potential to the wire (using a subsidiary current flow) and more slowly than by diffusion alone by applying a positive potential, Fig. 11. Application of a field in the opposite direction at a chosen time (20 or 17 h in Fig. 11) could reverse the direction of this movement. As we said at that time: "this opens the way for some of the ultimate experiments in Physics" (the effect of the vector potential on the motion). The motion of the hydrogen species appeared to satisfy the Nernst-Einstein relationship, i.e., the species were present as protons in the lattice. As we have pointed out since that time, 18 the more recent work (for a summary up to 1972, see Ref. 19) appears to be subject to several misconceptions (which do not affect the work carried out by Coehn). The importance to the work on "cold fusion" lies in the fact that the studies of Coehn would open the way towards the implementation of "solid state devices." We will make some further comments on this subject area below. The third factor, which influenced our choice to start work in this subject area, was our knowledge of some of the early literature of the subject. The following page is the text of the first paper on the fusion of deuterium by Oliphant, Harteck, and Rutherford, which started the whole subject of fusion. 20
e
Note in particular that Bridgman's investigations give a rationale for the conversion of energies at the eV level (i.e., chemical energies) into energies of the fragments at the GeV level (pertinent to nuclear transformations) that may explain the "uphill" processes, which have been observed (see below). We do not intend to discuss this work further except to note that this work raises some uncomfortable questions (which actually preceded the decision to start work on "cold fusion").
597
March
17,
1934
Nature
413 cleus of mass 4.0272 and two charges. This
Transmutation Effects observed w i t h H e a v y Hydrogen We have been making some experiments in which diplons have been used to bombard preparations such as ammonium chloride (NH 4 CI), ammonium sulfate [(NH 4 ) 2 S0 4 ], and orthophosphoric acid (H3PO4), in which the hydrogen has been displaced in large part by diplogen. When these D compounds are bombarded by an intense beam of protons, no large differences are observed between them and the ordinary hydrogen compounds. When, however, the ions of heavy hydrogen are used, there is an enormous emission of fast protons detectable even at energies of 20,000 V. At 100,000 V the effects are too large to be followed by our amplifier and oscillograph. The proton group has a definite range of 14.3 cm, corresponding to energy of emission of three million volts. In addition to this, we have observed a short-range group of singly charged particles of range about 1.6 cm, in number equal to that of the 14 cm group. Other weak groups of particles are observed with the different preparations, but so far we have been unable to assign these definitely to primary reactions between diplons. In addition to the two proton groups, a large number of neutrons have been observed. The maximum energy of these neutrons appears to be about three million volts. Rough estimates of the number of neutrons produced suggest that the reaction, which produces them is less frequent than that which produces the protons. While it is too early to draw definite conclusions, we are inclined to interpret the results in the following way. It seems to us suggestive that the diplon does not appear to be broken up by either a-particles or by proton bombardment for energies up to 300,000 V. It therefore seems very unlikely that the diplon will break up merely in a much less energetic collision with another diplon. It seems more probable (that the diplons unite to form a new helium nu-
nucleus apparently finds it difficult to get rid of its large surplus energy above that of an ordinary He nucleus of mass 4.0022, but breaks up into two components, one possibility is that it breaks up according to the reaction D i V D i ^ H ^ + Hi1. The proton in this case has the range of 14 cm while the range of 1.6 cm, observed agrees well with that to be expected from momentum relations for Hf particle. The mass of this new hydrogen isotope calculated from mass and energy changes is 3.0151. Another possible reaction is D 1 2 + D i 2 ^ H e 2 3 + n01 leading to the production of a helium isotope of mass 3 and a neutron. In a previous paper, we suggested that a helium isotope of mass 3 is produced as a result of the transmutation of Li under proton bombardment into two doubly charged particles. If this last reaction were correct, the mass of He is 3.0165, and using this mass and Chad wick's mass for the neutron, the energy of the neutron comes out to be about three million volts. From momentum relations the recoiling He 2 particle should have a range of about 5 mm Owing to many disturbing factors, it is difficult to observe and record particles of such short range, but experiments are in progress to test whether such a group can be detected. While the nuclei of Hi and He appear to be stable for the short time required for their detection, the question of their permanence requires further consideration. M. L. Oliphant P. Harteck Rutherford Cavendish Laboratory, Cambridge March 9 The text the first paper on the fusion of deuterium.
598
We always quote this paper 20 because we believe that it would not be published in more recent times; there are too many loose ends. The importance of this work lies partly in its own rights and partly in the feet that it led to the investigation of the "Hot Fusion" process, in a Wilson cloud chamber (work also carried out in the Cavendish laboratory): 21 (i) D+ + D+
-> 3 He 2 + + n 3
(ii) D+ + D+ --• T+ +
J
'
H+
"Hot Fusion"
(hi) D + + D+ --+ 4 He 2 + + 7 , (iv) D + + D+ --> 4 He 2 + + Heat
"ColdFusion."
A surprising feature of this measurement (also seen in the tracks reported in a subsequent paper 22 ) was the observation of a significant number of tracks for reaction (ii) at 180° (whereas the tracks should have been at -160°). As Dee 22 observed, Fig. 12, tracks at ~180° could only be explained by the fusion of species, which had lost most of their energy in the target. Our resurrection of this study has been studiously ignored (see however Ref. 23) and it is possible that we paid too much attention to these results. As reactions (i)
Figure 12. An example of Dee's 2 2 measurements of the tracks of 3 T + and 1 H + produced in one of the fusion reactions.
599
and (ii), above, only took place to minor extents, we decided that the excess heat had to be generated in a process such as (iv).f Processes (i)-(iii), observed in "Hot Fusion," are predicated on reactions in incoherent structures and, as we were basing our research on the possibility that we might observe the effects of coherence, it was clearly advisable to use a methodology which would not be bound to the reactions applying to incoherent systems.
We therefore decided to use calorimetry as the
main basis of our research.8'11
Cathode connection Anode connection
jGas outlet ^^Thermister """/connections ('
Kel-f closure
Heater connection Water bath level
r
Electrolyte level Silver mirror
vacuum jacket—pi ,i •Short thermister Capilary shields
Metal film ^resistance meter
Long thermister Anode
Figure 13.
f
- Cathode Kel-f support plug
An isoperibolic calorimeter used in our experiments on thermal balances.
We could detect the generation of 4 He but could not relate this to the rate of production of excess enthalpy; see further below. s T h e choice of calorimetry as the main method of investigation had the further advantages of high accuracy and low cost (we were financing the early research at our own expense) as well as avoiding the drawing of attention to the nature of our work. We had had earlier experiences of the negative reactions to the interpretations invoking the use of QED. We note here that the need to develop thermal balances for processes investigated in the Natural Sciences appears to have been forgotten in modern Science. Of course, our thinking on this topic was ignored by the main critics of our work who insisted that "cold fusion" had to follow t h e pathways laid down by research on "Hot Fusion." Such muddle-headed thinking is a characteristic of much modern science which wishes the number of species and the phases of wave functions to be independently determinable whereas they are in fact linked by an uncertainty principle, Equation (A.6).
600
Figure 13 illustrates the type of isoperibolic calorimeter, which we adopted for the main part of our work. We note that the precision and accuracy are set by the error limits of the temperature measurements of the cell contents and the and the surrounding water baths (3 x 10~ 3 °C in temperatures of ~30°C giving errors lying between 0.01 and 0.1%) provided a method of data processing is adopted which does not increase these errors. The instrumentation and methods of data analysis have been extensively described1' > • (e.g., see Refs. 24 and 25). It will be evident, however, that our expectations with regard to the measurement of thermal balances have not been realized. This is due in part to the presence of the phenomenon of positive feedback, which we illustrate by measurements carried out in the "New Hydrogen Energy (NHE) Group" k in Japan, 27 Fig. 14 (see also Fig. 21a, b). With increasing time/temperature the shape of the calibration plot changes in such a sense that an increase in temperature leads to an increase in the rate of excess enthalpy generation (Fig. 14). If this phenomenon is not avoided (or taken into account explicitly) we will draw the inevitable conclusion that the instrumentation is inaccurate (whereas we have simply demonstrated the phenomenon of positive feedback). Once the presence of this phenomenon is recognized, we can choose conditions, which lead to the driving of the cells to the boiling point, Fig. 15 (here by the raising of the cell current). In 1994, we could show that such boiling conditions could be maintained for ~30months by using a dual calorimeter, Fig. 16, in which the lower section was used to achieve boiling conditions, which were maintained using condensation in the upper section. Boiling conditions were maintained using excess heat generation at specific rates of 2-4kWcm~ 3 which were somewhat in excess of the break-even value 1 . 28,29 Use of the standard type of calorimeter, Fig. 13, led to the "boiling to dryness" of the cells such as that illustrated in Fig. 17. 30 It should be noted that the heat rejection was maintained to the surrounding water bath (at 30°C), Fig. 13, in these experiments so that the cells could only
'The existence of these accounts has not prevented the many critics of "cold fusion" from attributing ludicrous errors to this instrumentation. We note that the cause(s) of these errors have not been specified; the attitude appears to rest on the belief "we know that 'Cold Fusion' is impossible, so the instrumentation must have such errors." We note that our many critics have often attributed to us statements, which we have not, in fact, made. We always said; "if we had said this or done that, then the criticisms would have been justified." The incorrect statements are then heavily criticized - they are never withdrawn. The important point appears to be the making of the criticism. We note that it seems to be a general phenomenon in modem science that incorrect statements are not withdrawn. ^Scientists appear to have lost the ability to design experiments "from scratch." The attitude appears to focus on the stringing together of "off-the-shelf" equipment. For the particular case of the measurement of thermal balances they also appear to have lost the ability to classify experimental equipment into "ideal" and "non-idea" types. 2 6 The isoperibolic calorimeter (Fig. 13) is an "ideal reactor." k A s our measurements are distrusted, we prefer to illustrate our account by results obtained by other research groups. 'We note that the thermal efficiency of the systems was poor but the steps necessary to improve this thermal efficiency could easily be specified.
601
E(V)
Temp (°C)_ 55.49
* 7.933
54.77
7.857
54.05
] 7.781
53.33
.I 7.705 Wfi *\i,
..:%•: !
fr:i 7.(
52.62
"i... 7.553 1399611 1434051 1468491 1382391 1416831 1451271
54.77 •—
Time (1000s) Figure 14.
The later stages of the experiment, Fig. 21, showing the effects of positive feedback.
remain in the vicinity of the boiling point provided"1 the specific rate of excess enthalpy generation exceeded ~ 2 5 0 W c m - 3 . An interesting improvement in these experiments was achieved by arranging for heat rejection to take place to a "bath" at 90°. 31 In this case, excess enthalpy generation could be observed for 7days (Fig. 18). 3. Some further comments on "Cold Fusion" It will be apparent that the material which has been commented on in this paper has been highly restricted and aimed at the illustration of the question whether "cold fusion" could be developed into a practicable source of energy. A question of key importance is clearly; "what is the nature of the nuclear reactions responsible for the generation of excess enthalpy?" As has been pointed out above, there was some evidence for the generation of 4 He but the results obtained were highly erratic. Figure 19 illustrates the first systematic investigation (using mass spectroscopy as a means of detection). We have been frequently asked: "why are the results so m However, note that the thermal efficiency is parlance of "Hot Fusion."
co, i.e., the system is close to "ignition"
the
602 100.00 _ ( , < M »>
—
.
—
—
Demosj
j, f
o d d o
0.00 L_ 0
— I 500
,—t„I,,. — L — . 1000
1500
12000
1 2500
Time/100s F i g u r e 15.
I l l u s t r a t i o n of t h e b e h a v i o r of a cell b e i n g d r i v e n t o t h e b o i l i n g p o i n t of t h e e l e c t r o l y t e .
irreproducible?" The answer appears to be that the experiment is subject to the high background level of 4 He in laboratory atmospheres and, moreover, that 4 He is retained in the host lattice and is released erratically.11 There have been several investigations of the generation of 4 He since that time and we note especially the measurement of 4 He trapped in the lattice. 33 There is a further factor that may affect the formation of 4 He. Several studies have shown the generation of isotopes by markedly endothermic reaction (see especially Ref. 34); processes, which we believe can only be understood by invoking QED in extended coherence domains. The nature of these processes clearly requires further investigation. This brings us to the central problem, which we believe requires further investigation at this time. It will be apparent that the work carried out by one of us (M.F.) has only dealt peripherally with the question which we believe to be of central importance to the development of the subject namely, the effect of the potential in the lattice on the motion of D + and the associated generation of excess enthalpy (see the description of the relevance of the work of Coehn 16,17 given above). The study described in Ref. 18 demonstrated that the kinetics of this motion could best be understood in terms of the driving of the 7-phase 35 towards the outgoing interface of the electrodifTusion system. It is likely that this 7-phase (or else of the lattice
"Note that there is a considerable literature devoted to the decoration of imperfections in lattices by 4 He generated by a-particle irradiation. It is evident that such decoration requires a limited mobility of 4 He in the lattice.
603 Insulating cap Constant temperature bath
Upper condensing section Thermister ports
Viewport
Lower reaction section
Figure 16. The dual calorimeter (the ICARUS-9 calorimeter) used in the investigation of the prolonged excess enthalpy generation.
in which both tetrahedral and octahedral sites are occupied) is the source of the excess enthalpy generation and this hypothesis became the central theme of the research carried out by the group at Frascati. 36 This work focused on the generation of excess enthalpy and the simultaneous generation of 4 He in very thin "wires" of Pd (cross-sectional dimensions 2 x 50/mi), the so-called "bustrophedic" structures (Fig. 20). This work demonstrated the simultaneous generation of excess enthalpy and of He. A surprising feature of the experiments was the eventual melting (boiling?) of the Pd observed near the most negatively polarized ends of the structure. Order of magnitude calculations of the rates of excess generation required to achieve such conditions give values lying between 0.5 and 5.0MWcm" 3 . Corrections of the rates of heat transfer to allow for the effects of electrolytic gas evolution give values lying in the range 5-50 MW c m - 3 . The generation of excess enthalpy at such levels clearly requires further investigation.0 It is possible, also, that a switch from electrochemical compression of D+ in the lattice to the use of solid-state devices (or else of devices using both effects) 4
°We note that civilian applications of the methodology would require the rates of excess enthalpy generation to be restricted to ~10 kW c m " 3 . Present day production of Pd is sufficient to allow the conversion of a substantial part of the worlds energy needs to "cold fusion" systems. It is relevant that more than 50% of the worlds energy consumption takes place at temperatures below 70°.
604
Cell 1/2 dry
100
o
Cell remains
o CD i_
at high
2
temperature
0 Q.
tor3h
E 90
Cell dry JL
JL
X
1590000 1600000 1610000 1620000 1630000 1640000 1650000 1660000
Time (s) Figure 17. The behavior of the cell in the region of the boiling point; the cell remains at high temperature for ~ 3 h following the termination of polarization.
1.5 ;TT"ST™*™r^nri™!~iTrTrT*T^^ 1.2 ^
0.9
Q.
0.6
I?! «
0.3
1 2
3 4
5
6 7
8 9 10 1112 13 14 15 16 17 18 19 20 21 Days
Figure 18. The prolonged observation of Heat after Death. T h e lightly shaded bars give the generation of enthalpy following termination of polarization.
605
would reduce the irreproducibility of the phenomenon, which has been observed. This is an aspect, which we have not covered in this report. We believe that excess enthalpy generation takes place in the bulk of the material as mediated by the surface reactions. Such a process would be expected to be highly sensitive to the surface conditions. We note that although it is relatively easy to produce palladium, the metallurgy of this metal is very difficult. Previous work has paid insufficient attention to the effects of the metallurgical variables on the processes observed.
0
2E13
2E13
2E13
2E13
1E14
Helton atoms, normalized to 525 mA and 500 mL Figure 19.
The first study of excess enthalpy generation as a number of 4 He atoms produced.
4. Closure The work presented in the first part of this paper demonstrates that QED is not just a subject to be confined to subatomic Physics, cosmology, etc., but that it pervades modeling in the whole of the Natural Sciences. This is equally true of topics (i), (iii)-(v) also investigated prior to the start of work on "cold fusion," Diagram 1, as well as to topics (vi)-(xii) investigated since the start of that particular research (Diagram 2). We believe that the reluctance to accept such a point of view can be traced back to the belief that both the amplitudes and phases of wave functions can be fixed independently [whereas they are actually linked by an uncertainty principle equation (A.5)]. The question that arises is: will such a view ever be corrected? We note here the severe downturn in present day Science (Fig. 20) which we believe is due to the neo-Roman emphasis on consumption at the expense of production; a consumer society does not need Science but, of course, it will eventually suffer the same fate as did the Roman antecedent.
606
Appendix A: Revolutions in our Understanding of the Natural Sciences We summarize here briefly the multistage conceptual path that has led to "cold fusion" as a possible concept based on rational scientific thinking (not on witchcraft).
Neolithic era Modern era
-100,000 -10,000
-1000 -100 Time/year
Roman Plague era
Neo-Roman empire
Figure 20. (a) The lithographically produced "bustrophedic" configuration of a fine Pd wire. 3 6 (b) An historical perspective of Western Scientific Activity.
Temp (°C)
E(V)
53.20
TempfC) 62.00
52.53
51.86 z=.
51.20
9.207
50.53
i 9.117
49.86
7.890 622011 656451 690891 604791 639231 673671 Time/1000 s
58.44
9.026 2436771 2471331 2505891 2419491 2454051 2488611 Time/1000 s
Figure 21. Polarization of s Pd 90 Ag 10 cathode (0.4 cm diameter, 1.25 cm length) in 1 M OD in D2O; cell current = 0.5 A; calibration input AQ = 0.2504 W. The raw data as a function of time: (a) the early stages; (b) the somewhat later stages showing the completion of the effects of positive feedback.
607
This trip started about one century ago with the two revolutions of our understanding of the natural sciences: quantum physics (QP) and relativity. These two initial revolutions led to a massive change in our understanding of classical physics (CP). The first revolution (QP), arose from the inconsistency between the CP definition of entropy S of a macroscopic state: S = khxT,
(A.l)
where T is the volume of the phase space associated with the macroscopic state and the third principle of thermodynamics, formulated by Walther Nernst, 37 namely that entropy would vanish in the limit of vanishing temperature T. This inconsistency arises from the fact that the phase of space of the classical system in the limit T —> 0 shrinks to a simple point (all momenta are zero and the coordinates are constrained by the minimization of the potential energy). The volume of the phase space in the limit T —> 0 therefore becomes zero and, unfortunately |ln0| = oo.
(A.2)
We note that this "catastrophe" is usually misrepresented in textbooks where this "failure" is attributed to an "ultraviolet catastrophe" implying a failure of (A.l) at short length scales. This misunderstanding was based on the first physical system studied, black body radiation, where spectral distribution, according to the Wien's law, is a function of the ratio v/T (v is the frequency of radiation, v = cA). In consequence, the limit T —> 0 could be mimicked by the limit v —> oo, namely A —> 0. In point of fact that "failure" is to be attributed to low temperatures rather than short length scales. However, the misinterpretation has persisted leading, eventually, to an attribution of deviations from "classical behavior" to subatomic physics only. In fact CP is flawed by the inconsistency (A.2), at all length scales. The way out of the dilemma posed by Eqs. (A.l) and (A.2) developed from the solution given by Max Planck to the problem of black body radiation. He proposed that the microscopic states corresponding to a given macroscopic state should no longer be points in the phase space, but small regions whose volume is controlled by an universal constant, the celebrated Planck constant h. We thus are able to introduce a natural system of units in the phase space where the volume of each elementary region is just 1. We then obtain In 1 = 0
(A.3)
as required by the Third Law of Thermodynamics. This has proved to be the cornerstone of QP. We address the simplest case of a physical system made up of just one particle in one dimension. In this case, the phase space is a plane, where each microscopic state corresponds to a region where sides Sp and 5q obey the celebrated Heisenberg uncertainty principle. SpSq > h.
(A.4)
Equation (A.4) is often presented as indicating the presence of a limit to our knowledge, an inability of the observer to "know" the "real" p and q. In fact the "real"
608
p and q do not exist; p and q are intrinsically fluctuating quantities, otherwise entropy (it is irrelevant whether observed or not) would diverge and involve all of us (observed or not) into the "ultracold" catastrophe. In this way a new fundamental variable must add to the old-fashioned position, time, momentum and energy: the phase of the oscillations describing the quantum fluctuations. Let us address now an important consequence of the relativistic revolution coupled with QP. This consequence emerges from the mutual interchangeablity of mass and energy and does not affect kinematics: it therefore applies to the everyday world. Consider a single electron. This could be conceived either as an extended or as a point-like object; in the former case it would be torn apart by the inner repulsive forces, in the latter case the energy of its associated electric field would be infinite. In both cases the sheer existence of a free, isolated, electron causes difficulties, which are resolved by relativity. A point-like "bare" electron converts the diverging energy of its fields into infinitely many positron-electron pairs within a radius ro (the so-called "electron radius") such that e2
2
— = 2mc 2 ,
(A.5)
where ro is the distance from the "bare" electron where the first positron-electron pair can be formed. The "bare" electron attracts the "dressing" positrons and repels the electrons. The "dressed" electron, which is the physically observable electron, is the example of the "bare" electron, whose charge must be assumed to be infinite and close to the infinitely many surrounding positrons within the radius ro- The physically observable charge is the difference of the two infinities that, according to the mathematical structure of QED, is a finite number; QED is a renormalizable theory. This brilliant solution to the problem of the existence and stability of the electron, given in 1954 by Gell-Mann and Low,38 implies that a free independent electron cannot exist. There must be infinity of other electrons elsewhere in the world; the elementary object is not a single electron, but the full ensemble of electrons, the "electron field," whose quanta are the single electrons. The electron field and, in general the "matter field" - should be, of course, a quantum field (QF), i.e., a fluctuating field. We have now arrived at the third station in this journey of the definition of matter. We have to ask: are the quantum fluctuations of these fields tuneable? "This question has been posed firstly by Nemst in 1916, when he assumed that extended objects arising from the interaction of many components should be characterized by the phase locking of the Quantum Fluctuations of the single components. 39 This point of view has been obscured for many decades by the prevailing paradigm of Bohr that confined QP in the remote subatomic underworld far from daily life. However, the possibility that the elementary components could be linked together into macroscopic pieces of matter by the tuning of their Quantum Fluctuations in
609
phase agreement with a long range interaction field, such as the electromagnetic field, has been considered again in t h e last decades by Robert Dicke, 4 0 Hepp and Lieb, 4 1 and finally by Giuliano P r e p a r a t a . 4 2 We note t h a t a macroscopic physical system, whose states arise from the phase tuning of components, would be characterized by a macroscopic phase 0.However, in Q F T , a Heisenberg-like uncertainty principle holds concerning the uncertainty 6N of the number N of q u a n t a of the field and the phase uncertainty 5(j>: 8N6(f> > h,
(A.6)
which has two interesting limits: (i) N is defined, i.e., SN = 0 so t h a t (p is indefinite. This is the underlying representation adopted by the "hard sciences." (ii) Sep = 0 and TV is indefinite. This is the "coherent state" in Q F T . We must ask how is it then possible to build a coherent state in condensed m a t t e r physics starting from a definite number of atoms a n d / o r molecules? This is obviously impossible if one assumes a single eigen state of N. However, it becomes possible when components are allowed to oscillate between two different states; N is well defined on the superposition of the two states but the occupation number is uncertain for each additional state involved in the oscillation, which then leads to a well-defined relative phase. This is just the solution to the problem of the onset of coherence in many physical systems, as shown in the recent literature. Coherence is therefore the way in which a huge number of elementary components co-operate. Following this p a t h it becomes possible to understand the assembly of larger and larger energies towards well-defined goals. Note t h a t the phase agreement of some millions of small children enables these t o overwhelm R a m b o . This is t h e arcane of Cold Fusion and this is why Cold Fusion is such a nightmare for the fans of R a m b o . References 1. G. Preparata, QED Coherence in Matter, ISBN 9810 222 491 QC 173. 454. P74 (World Scientific Publishing Co. Ltd., Singapore, 1995). 2. M. Fleischmann, L. J. Li, and L. M. Peter, Electrochimica. Acta 34, 475 (1989). 3. M. Fleischmann, S. Pons, and J. L. Daschbach, in M. I. Montenegro, M. A. Queiros, and J. L. Daschbach (eds.), Microelectrodes: Theory and Applications, NATO ASI Series 197 (Kluwer Academic Publishers, ISBN 0-7923-1229-5, 1991, p. 393). 4. J. P. Sousa, Ph. D. Thesis, University of Utah, 1991. 5. M. Y. Abyaneh, M. Fleischmann, E. D. Giudice, and G. Vitiello, The Search for the Effects of Quantum Electrodynamics in the Natural Sciences; the Example of Nucleation and Crystal Growth, to be published. 6. M. Y. Abyaneh, M. Fleischmann, E. D. Giudice, and G. Vitiello, The Investigation of Nucleation using Microelectrodes; I, the Ensemble Averages of the Times of Birth of the First Nucleus, to be published. 7. M. Y. Abyaneh, M. Fleischmann, E. D. Giudice, and G. Vitiello, The Investigation of Nucleation using Microelectrodes: II, the Second Moment of the Times of Birth of the First Nucleus, to be published.
610 8. M. Fleischmann, Searching for the consequences of many-body effects in condensed phase systems, in Proceedings of the 9th International Conference on Cold Fusion, ISBN 7-3 02-0648 9-X, X. Z. Li (ed.) (Tsinghua University Press, Beijing, 2002, p. 141). 9. M. Fleischmann, Searching for the biophysics of an elementary system, in Brain and Being, ISBN 90-272-51940; 1-58811-550 x QP411. B74. G. G. Globus, K. H. Pribram, and G. Vitiello (eds.) (John Benjamins Publishing Company, Amsterdam/Philadelphia, Vol. 58, 2004). 10. M. Fleischmann, Background to cold fusion: the genesis of a concept, in Proceedings of the 10th International Conference on Cold Fusion, P. Hagelstein (ed.). 11. M. Volmer, Kinetik der Phasenbildung (Steinkopff, Leipzig, 1939). 12. J. Zeldovich, J. Exp. Theor. Phys. 12, 525 (1942) (in Russian). 13. J. Frenkel, Kinetik Theory of Liquids (Oxford University Press, London, 1946). 14. M. Fleischmann and M. Liler, Trans. Faraday Soc. 54, 1370 (1958). 15. P. W. Bridgman, The Physics of High Pressure (International Textbooks of Exact Science, London, 1947). 16. A. Coehn, Z.Elektrochem. 35, 676 (1929). 17. A. Coehn and W. Specht, Z. Fiir Physik 62, 1 (1930). 18. C. Bartolomeo, M. Fleischmann, G. Larramona, S. Pons, J. Roulette, H. Sugiura, and G. Preparata, Trans. Fusion Technol. 26, 23 (1994). 19. G. Alefeld and J. Volkl, Hydrogen in Metals I, ISBN 3-540-08883-0; 0-387-08883-0 (Springer Verlag, Berlin, Heidelberg, New York, 1978). 20. M. C. Oliphant, P. Harteck, and L. Rutherford, Nature 113, 413 (1934). 21. P. I. Dee, Nature 113, 564 (1934). 22. P. I. Dee, Proc. R.Soc. 148A, 623 (1935). 23. Y. E. Kim, Trans. Fusion Technol. 26, 519 (1994). 24. M. Fleischmann, S. Pons, M. L. Roux, and J. Roulette, Trans. Fusion Technol. 26, 323 (1994). 25. M. Fleischmann, Thermal and Nuclear Aspects of the Pd/Di O System, Vol. 2, SPAWAR System Centre Report TR-1862, 2002. 26. O. Levenspiel, Chemical Reaction Engineering, 3rd edn. (John Wiley, 1999). 27. M. Fleischmann, in Proceedings of the 5th International Conference on Cold Fusion, Monte Carlo, Monaco, April, 1995, p. 140. 28. Technova, Internal Report, August, 1994. 29. M. Fleischmann, in Proceedings of the 7th International Conference on Cold Fusion, Vancouver, Canada, April, 1998, p. 119. 30. S. Pons and M. Fleischmann, Heat after death, in Proceedings of the 4th International Conference on Cold Fusion, Vol. 2, 1993, p. 8.1; M. Fleischmann and S. Pons, Phys. Lett. A176, 118 (1993). 31. G. Mengoli, M. Bernadini, C. Manduchi, and G. Zannoni, J. Electroanal. Chem. 444, 55 (1998). 32. M. H. Miles and B. Bush, Frontiers of cold fusion, H. Ikegami (ed.). in Third International Conference on Cold Fusion, October 21-25, Nagoya, Japan (Universal Academy, Press, Inc., Tokyo, Japan, p. 113); B. F. Bush, J. J. Lagowski, M. H. Miles, and G. S. Ostrom, J. Electroanal. Chem. 304, 271 (1991). 33. C.-C. Chien, D. Hodko, Z. Minevski, and J. O. Bockris, J.Electroanal. Chem. 338, 189 (1992). 34. Y. Iwamura, T. Itoh, and M. Sakano, in Conference Proceedings of the Italian Physical Society, ISBN 88-7794-256-8, 70, 141 (2000); Y. Iwamura, T. Itoh, M. Sakano, and Sakai, in Proceedings of the 9th International Conference on Cold Fusion, ISBN 7302-06489-X, X. Z. Li (ed.) (Tsinghua University Press, Beijing, 2002, p. 141).
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35. E. D. Giudice, A. D. Ninno, M. Fleischmann, A. Fratolillo, and G. Mengoli, in Proceedings of the 9th International Conference on Cold Fusion, ISBN 7-302-06489-X, X. Z. Li (ed.) (Tsinghua University Press, Beijing, 2002, p. 141) (see also literature quoted therein). 36. A. D. Ninno, A. Frattolillo, A. Rizzo, E. D. Giudice, and G. Preparata, RT 2002 41/Fus, ISSN-0393-3016. 37. W. Nernst, The New Heat Theorem (Dover, New York, 1969). 38. W. Nernst, Verh, Deutsch, Physik. Gesellschaft 18, 83 (1916). 39. M. Gell-Mann and F. Low, Phys. Rev. 95, 1300 (1954). 40. R. Dicke, Phys. Rev. 9 3 , 99 (1954). 41. K. Hepp and E. Lieb, Ann. Phys. 7, 360 (1973). 42. G. Preparata, An Introduction to a Realistic Quantum Physics (World Scientific, Singapore, 2002).
THEORETICAL MODEL OF T H E P R O B A B I L I T Y OF F U S I O N B E T W E E N D E U T E R O N S W I T H I N D E F O R M E D LATTICES W I T H MICROCRACKS AT ROOM T E M P E R A T U R E
FRISONE FULVIO Department
of Physics,
University of Catania, Via Santa Sofia 64, 95125 Catania, E-mail: [email protected]
Italy
In this work, we wish to demonstrate that a reaction path as the following, dislocations, deformations due to thermodynamic stress and, finally, microcrack occurrence, can enhance the process of fusion of the deuterons introduced into the lattice by deuterium loading [F. Frisone, Can variations in temperature influence deuteron interaction within crystalline lattices? Nuovo Cimento D, 18, 1279 (1996)]. In fact, calculating the rate of deuteron-plasmon-deuteron fusion within a microcrack, showed, together with an enhancement of the tunneling effect, an increase of at least 2-3 orders of magnitude compared to the probability of fusion on the no deformed lattice. In fact, strong electric fields can take place in the microcrack and the deuterons are accelerated to the energy which are enough for the D-D tunnelling [M. Rabinowitz, High temperature superconductivity and cold fusion, Mod. Phys. Lett. B, 4, 233 (1990); J. Price Hirt and J. Lothe, Theory of Dislocation (McGraw Hill); Z. Phys., 457, 156: (I960)]. These phenomena open the way to the theoretical hypothesis that a kind of chain reaction, catalyzed by the microcracks produced in the structure as a result of deuterium loading, can favour the process of deuteron-plasmon fusion (N. W. Ashcroft and N. D. Mermin (Eds.), Solid State Physics, Chapter 25 (Saunders College, Philadelphia, 1972), pp.492-509).
1. Introduction In a previous paper 1 , we studied the influence of the temperature on the phenomenon of deuteron fusion within unperturbed crystalline lattices with CFC or HCP structures, hypothesizing that a kind of chain reaction, catalyzed by the microcracks which form following ionic dislocations induced by structural deformations as a result of variations in the thermodynamic conditions or other factors, can increase the rate of fusion. As a result of the numerical calculation performed for different metals, varying the temperature, the total energy and the concentration of impurities, it was possible to conclude that the probability of fusion was in effect substantially enhanced by increasing these parameters. In this paper, we wish analyze the role of impurities on dislocation formation and then on microcrack occurrence. In fact within microcrack local electrical field take place able to accelerate the deuterons along the Coulomb barrier. It is important observe that the microcrack formation is a non-linear phenomenon. It can be depend 612
613
on impurities percentage, ratio loading, and other thermodynamic conditions. So from a point of experimental view we can expect that the microcrack formation is a very random effect. However, and this is a very crucial point, the d-d fusion enhancement within microcrack (due to electrical local field) is a very linear effect. 2. Lattice Screening Role After the Fleischmann and Pons experiments had been published, it soon became clear the main role of palladium lattice as catalysing. Many people supposed that in the lattice the Coulomb potential is screened. To illustrate this topic, we report the argument of Horowitz.4 The electrons in a metal should become a Fermi gas and the hydrogen nuclei interacting via screened Coulomb potential. The effective potential between two nuclei V(r), which includes the effects of electron screening is given, in a simple Thomas-Fermi model, by 2
V(r) = -e e x p - -r T
L
,
(1)
A-
of course A is the screening length and depends on density. But for r
e2
85 eV.
(4)
It means that the deuterons can reach the intermolecular distance of 0.165 A. In this case by means of Eq. (1) and using A = 1022 s" 1 , he obtains A = 10~ 22 s _ 1 . We conclude this section observing that within a lattice in according to the quantum mechanics principles the fusion probability is observable.
614
3. A n Effective Potential Proposed From these results appears clear that within lattice the d-d reactions takes place in a D2-molecule whose inter-nuclear distance is reduced by screening effect. More exactly by means of works reported in reference, 3-13 we can say that within a lattice: (1) the screening effect is able to increase the fusion rate, (2) a compound potential as which used by Siclen and Jones 5 is also able to reproduce the d-d interaction. For this reason we tried to find a d-d effective potential such that for distance smaller than p gives about the Coulomb potential while, for the distance bigger than psg Morse-like potential. In Ref. 10 to fit a such "Coulomb-Morse linked" potential we have proposed the following effective potential: V(r)=k-(vM(r)-~), r \
(5) r )
where Vu(r)
= D' [ e - 2 ^ - ^ - 2e"T ( r - r ° ) ] .
(6)
Here A, D', 7s and r'0 are parameters to determinate by means of fitting. The potential screening VQ value has been taken from Preparata's model (average: 85 eV) and it means that pg 26.9/Vo is about 0.165 A. Then, regarding the other main values (i.e., equilibrium distance ro and disassociation energy D) we have used the many-body theory approach. In fact, as pointed out in Ref. 10, the deuterons interaction with the collectives plasmon excitations of the palladium produces a strong attractive potential. This attractive force is due to exchange of plasmons (in the ref. the authors consider only two plasmon excitations at 7.5 and 26.5 eV) between two deuteron-lines as reported in Fig. 1:
Figure 1.
Feymann expansion used.
615
Taking into account the role of coupling between deuteron and plasmons in Ref. 6 is evaluated a like-Morse potential where p is about 0.2 A, D about 50 eV and ro about 1 A. Table 1. fitting. P ro D A r'o D' 7
= =
= = =
0.8
Parameters
0.165 A 0.35 A 50 eV 0.0001 0.99 1.49 1.04
1
1.2
Bohr radius
Figure 2.
Effective potential.
Using the potential we obtain a fusion rate for E = 0 of about 10" -20 used A = 1022 s" 1 ).
we
4. Deformation in Cubic Lattices In this section, we wish to establish whether, and within what limits, the rate of fusion within a microcrack in a generic cubic lattice subjected to deuterium loading can be conditioned or influenced, not only by extensive lattice defects and
616
other characteristics and thermodynamic conditions, but also by any "deformations" produced in the crystalline lattice by variations in the temperature which finally can take place as microcrack. In fact we wish to study the internal perturbations, which can take place in the lattice following D2 loading and the consequent modifications in the properties of the metal. The loading does not, in fact, simply provide an increase in the percentage of deuterium present, with a resulting disequilibrium of the "d" band; rather this type of procedure also determines, according to our hypothesis, lattice deformations followed by dislocations which cause microcracks in the structure. If this effectively occurs, it is not difficult to hypothesize that the energy produced by the microexplosions within the microcracks present, could favor the creation of new fractures, which in turn would, by the same mechanism, capture other deuterons, and so on. On the other hand, the formation of microcracks in palladium electrodes produced by the energy released during long periods of electrolysis13 has already been observed experimentally for some time but has until now been considered only a consequence of nuclear fusion. Our hypothesis is rather that this phenomenon could favor the process, enhancing the probability of fusion of the deuterons absorbed by the metal lattice. The interaction between the impurities present and the dislocations produced in the metal during deformation, therefore, could significantly modify the electrical properties of the material. Some particular reactions could then take place, which incorporate the impurities in the nucleus of the dislocations, 3 as a result of the different arrangement of the atoms with respect to that of the unperturbed lattice. An adequate theoretical description of the loading can therefore be obtained, in our opinion, only by treating it as a perturbation independent of time. We must also consider the fact that, under conditions far from those of saturation, the rate of fusion, within the metal depends on the number of deuterium nuclei absorbed in unit time, which could also depend on the deformation of the lattice. It is necessary therefore to study both phenomena. We can say that qualitatively the lattice deformation 'I'gepends on many factors, as concentration impurities J, density of the mobile dislocation r, radius of dislocation curvature R, etc. * = ¥ ( J , r,R,...).
(7)
Ay same way J, r, R, etc. are correlated: R = R(r, J, ...).
(8)
It means that the lattice loaded is a very complex system and then it exhibit a non-linear behavior. For simplicity we can now consider a cubic lattice structure subjected to deformations and calculate the probability of fusion within a microcrack, T, on varying the temperature.
617
Indicating the volume of a single cell by df2, the deformation of the entire lattice is given by:
H//M^-(-£K>)4
9(
»
where r\ is a parameter which depends on the lattice and electronic structure of the metal under consideration. In this study we have concentrated on the cubic structure of the lattice, in the specific case of palladium, because it has an easily observable geometry and more exactly we have indicated by p the density of the mobile dislocation8 within the lattice at non-constant lattice temperature, so that the thermodynamic stress of the deuterium nuclei for unit volume must be taken into consideration. Further, L2 indicates the area between the lines of separation between two adjacent dislocations, produced during a deformation of the lattice 9 with non-constant temperature, R is the curvature which the dislocation assumes during deformation, a is proportional to the thermal increment and represents the effect of the sudden variations in temperature to which the lattice is subjected, as a result of which the deformations form, v is the frequency of vibration of the deuterons in the metal, which we consider "negligible" here (and which will be considered at higher temperatures in future), b2 is the stress line which dampens the transformation of the crystalline lattice for small stress variations within the lattice,9UQ = 2£/j — Dbd(a — o"i)eo is the activation energy which is always less than a couple of jogs. In the latter expression, a — G\ represents the stress applied at the small dislocations. With a good approximation, we can calculate that lib ^ 2 ^ where 0, has the dimensions of a wavelength, while /J, is an elastic constant which depends on the characteristics of the lattice; SQ = ep — (3tm , where /3 depends on the temperature causing the "deformations"; TO is a variable which depends on the lattice and, in this case, is equal to 1/3; 2Uj ~ fcTcln(X/e) is obtained from the comparison of two curves with velocity of deformation e, Tc is the "critical temperature" for the formation of the microcracks and lies within the temperature range 9 of 200-300 K for cubic metals, X ~ 105 in the CGS system, d indicates the distance between the dislocations which have not suffered internal splitting, 6can be associated with the interatomic distance and D depends on the movement time of the dislocations, x i s the deuterium load which we can associate with a perturbation independent of time, within the lattice subjected to thermodynamic variations, and per unit of surface area. Finally, £(r) is the number of dislocations. We want to emphasize the deformation dependence on k. In fact, it is very easy to demonstrate that exist a deuterium loading percentage (which at the same time
618
depends on other thermodynamic conditions!) Xo f° r that happens
,H
{///„' (j!£sg*"»(-15>)to)*<}2«—
do)
where Piatticeis the lattice pitch: in this case the microcrack take place. Now we propose some approximate calculations in which the lattice deformation and the microcrack depth are correlated. The depth of the microcrack LD (T) , a function of the lattice temperature, is given by: 11 LD(T) =
^W[(W-^V2'
(11)
the quantity ( L ( ff^j ) 5r is the change in elastic and potential energies of the external mechanisms per unit of lattice length, due above all to the variations in the thermodynamic conditions caused by thermal exchange with the external system; r is the distance between the center of the dislocation and the center of mass of the lattice, 6r is a small variation. The quantity: V
7T(l-I/d)J<7r
'
represents the length of a microcrack in a generic cubic lattice in conditions of quasi-equilibrium (the typical value5 is I ~ 700 A), Nb is the number of lattice ions, of mass (i, involved in a super-dislocation (this number generally depends on the extension of the core). If the energy of the dislocation is limited by a cut-off R, within the metal there is a lattice configuration which is only slightly modified and whose particularities could depend on the external energy. vA is the frequency of deformation: 2Wk
(
2Fk\
Expression (7) represents the independence of the internal stress from the external conditions, a valid hypothesis in this approximation: a2 is the position of equilibrium of the distribution core, separated along a "split" in the crystalline lattice of generic symmetry; 2Wk, approximately, is the energy of the barrier in different states of near equilibrium of the nuclei within the lattice, which includes the stress in conditions of non-equilibrium, kT is the thermal energy to which the metal is subjected; 2Fk is a parameter which depends on the lattice; Dk represents the point of fusion with energy kT. Further, the factor aT in (7), is the stress factor in quasi-equilibrium: a r
~
2 T T ( 1 - « / ) £ > (r 2 ) J
'
K )
where v is the frequency of the lattice vibrations induced by the dislocations, D the distance between dislocations and b is the three-dimensional Burgers vector.7 From this model the microcrack formation appears around 300 K and the width fracture is 1-10 nm.
619
5. Electrical Field in a Microcrack The microcrack occurrence takes place as a fracture of lattice-cell, it means 7 that a surface S given from a square with a side length of crystal lattice constant (3.5 A). More exactly we can define a charge density as Q
(15)
We can estimate erc = 2.32 c/m 2 , Then we are able to compute the electrical field E and the potential V: E =
Or
(16)
£o
V = Ed.
(17)
In this way E = 2.96 x 10 11 V/m, so for d = 1 to 10 nm we have V = 2.96 x 102 to 2.96 x 10 3 V. It means that within a microcrack the deuterons acquire a energy between 2.96 x 102 and 2.96 x 103 eV. This mechanism is able to reduce the distance ro (see Fig. 3).
Figure 3.
Effective potential and microcracks energy contribution.
From (17), with the tunneling probability calculated adopting the Morse potential, a numerical simulation program employing the "WKB" method was used to determine the probability of fusion, normalized to the number of events per minute.
620
It was found that: P ~ 10^ 25 (without microcracks contribution), T w 10~ 14 (with microcracks contribution, i.e., V = 2.96 x 103 eV). It is clear that in this case, the probability of fusion within a microcrack is some 10,000 times greater than that calculated on the surface.
6. Conclusions The principal objective of the present study was to demonstrate if and how the deformation of the crystalline lattice and the formation of a microcrack could influence the process of fusion at room temperature. More precisely, we calculated numerically the probability of fusion within a microcrack, comparing it with that calculated on the surface to evidence a possible enhancement effect. The result of this study is that, in effect, the presence of the microcrack not only increases the probability of fusion by at least 2-3 orders of magnitude with respect to the case of the undeformed lattice, but also reduces the height and thickness of the Coulomb barrier. Further, perhaps for the first time, the theoretical analysis of the cold fusion process gives high values for the probability of fusion between deuterons, within a microcrack, at room temperature and with impure metals. Further, tunneling in the presence of deuterium loading was analyzed, observing that, from the theoretical point of view, the phenomenon can be treated as an internal perturbation of the lattice. As shown in Fig. 3, it was found that in the presence of loading, the tunneling appears enhanced due to the reduction, in both height and thickness, of the barrier "X" (Ref. 1). The loading seems therefore to be an important factor conditioning the phenomenon of fusion. The presence of this effect, if confirmed by further investigation, would open the way to new theoretical scenarios in which phenomena ignored until now, such as the potential energy of the barrier and others of quantum mechanics, could determine a broader understanding of the mechanisms at the base of cold fusion. One of these mechanisms essentially "consists" of a kind of chain reaction between deuterons and plasmons, catalyzed by the deformations and microcracks which arise in the structure as a result of variations in the thermodynamic conditions and other causes, such as deuterium loading. This was hypothesized in the present paper and constitutes one of the principal motives of its inspiration. Further study in this direction, and for other lattice structures, are in progress and the results obtained will be published in a future paper. It is however possible to confirm that the initial results obtained so far validate the hypothesis presented here.
621
References 1. F. Frisone, Can variations in temperature influence deuteron interaction within crystalline lattices? Nuovo Cimento D, 18, 1279 (1996). 2. M. Rabinowitz, High temperature superconductivity and cold fusion, Mod. Phys. Lett. B, 4, 233 (1990). 3. J. Price Hirt and J. Lothe, Theory of Dislocation (McGraw Hill); Z. Phys., 457, 156: (1960). 4. N. W. Ashcroft and N. D. Mermin (Eds.), Solid State Physics, Chapter 25 (Saunders College, Philadelphia, 1972), pp.492-509. 5. M. Yu. Gutkin and I. A. Ovid'Ko, Disclinations, amorphization and microcrack generation at grain boundary junctions in polycrystalline solids, Philosophical Magazine A, 70 (4), 561-575 (1994). 6. F. Frisone "Deuteron interaction within a microcrack in a lattice at room temperature" date accepted for publication: 13/6/00, Fusion Tecnol. 7. R. E. Hummel (Ed.), Understanding Materials Science, Chapter 3 (Springer, 1997), pp. 50-56. 8. F. R. N. Nabarro, Proc. Roy. Soc. A 209, 219; Adv. Phys. 271, 1 (1952). 9. J. Friedel, Dislocations, Chapter V, 116-458 (1960). 10. K. Sumino, In point and extended defects in semiconductors, Nato Asi ser. B, 202 (Plenum Publ. Corp., 1988), pp. 77-83. 11. J. Price Hirt and J. Lothe, Theory of dislocation (McGraw Hill, 1968), p. 463, Eqs. (14-46). 12. M. Fleishmann and S. Pons, Electrochemically induced nuclear fusion of deuterium, J. Electroanal. Chem. 261, 301-316 (1989); Erratum, 263, 187 (1989). 13. H. Kyeong An, et al., Analysis of deformed palladium cathodes resulting from heavy water electrolysis. Fusion Technol. 27, 408-415 (1995).
EFFECTIVE I N T E R A C T I O N P O T E N T I A L IN T H E D E U T E R I U M P L A S M A A N D MULTIPLE R E S O N A N C E SCATTERING
T. TOIMELA Vaasa Polytechnic, Wolffintie 30, 65200 Vaasa, Finland www.puv.fi; E-mail: [email protected] The effective interaction potential for charged particles is calculated in the deuterium plasma formed in the surface region of the palladium cathode in the electrolysis of heavy water. It is shown that the Coulomb potential is overscreened producing, at certain distances, an attractive potential between deuterium nuclei pairs and also between the deuterium nuclei and the surface atoms. This behavior of the effective potential in the deuterium plasma can be regarded as a counterpart of the Friedel oscillations of the electron gas at zero temperature. Because of this attractive potential, there are bound states for the deuteron pairs as well as for the surface atoms and deuterons. In these bound states the equilibrium distance between the nuclei is of the order 0.15-0.2 A depending on the number density of deuterons. The fusion rate is calculated for the bounded deuteron pairs and it is found to be of the order A m 1 0 - 2 2 1/s per deuteron pair for the highest deuteron densities. Furthermore, it is shown that larger fusion rates are possible for the deuterons bound to the surface atoms. This may arise by a process, where the trapped deuterons share the released energy collectively via a proposed Multiple Resonance Scattering (MRS) mechanism. It is then found that the 4 He-channel is the overwhelmingly dominant fusion channel. Moreover, the appearance of the transmutation processes in this MRS procedure is briefly discussed.
1. Introduction The experimental results concerning condensed matter nuclear science, starting from the first announcement of cold fusion,1 are very extraordinary. The idea that there could be nuclear processes caused by the condensed matter environment is astonishing. Furthermore, the experimental results showing that practically no radiation is obtained and that the branching ratios are not the usual ones obtained in the collision experiments of deuterons are even more astonishing features. Including the claims that there are also occurring transmutation processes of heavier nuclei, which should be even more unprobable reactions, it is not a surprise that this area of research has been mostly ignored by the main physics community. However, the aim of this article is to show that those extraordinary features may be explained without any new unknown physical theories, just with reasonable assumptions and correct treatment of the well-established quantum many-body theory. We assume that the deuterium ions reaching the cathode will form (together 622
623
with the electrons around) the deuterium plasma in the surface region of palladium (or other metal used as the cathode). The effective interaction in this plasma and its consequences will be examined in this work. This article is organized as follows: In the next chapter, the effective potential in the deuterium plasma is calculated. It is shown that the deuteron pairs will acquire an attractive potential, which sustain bound states. The fusion rate in these pairs will be calculated and a low-level neutron emission is shown to arise. The details of the calculations of that chapter will be published elsewhere.2 In Section 3, the deuterons trapped by the surface atoms are considered. A multiple resonance scattering mechanism is proposed, which is shown to lead to predictions that are consistent with the main experimental results in the condensed matter nuclear science. In the last section, an outlook for further studies will be given. 2. Effective Potential Following the standard electron gas calculations in solids,3 the Hamiltonian in the plasma composed of deuterons and electrons can be written as the sum of six terms: H = Hei + H d + H e l _ d + H b + H e l _ b + H d _ b ,
(1)
where Hei (H d ) is the Hamiltonian for the electrons (deuterons) respectively (containing the kinetic energy term plus the Coulomb interaction). H g i ^ contains the Coulomb interaction between deuterons and electrons. Hb is the interaction energy between the background surface atoms H e i_| D and H ^ ^ are the interaction energies between the surface atoms and electrons and deuterons, respectively. Assuming uniform distribution for the surface atoms, the three last energies are just pure numbers and can be ignored here. Beyond these trivial contributions the quantity containing the physically interesting interaction, is given by the effective interaction, obtained in the ring-diagram approximation (random phase approximation). TT -
Cfo(h;,q)
UeB
( ) l-n0(W,q)[70(^q)' where u and q are the angular frequency and the wave vector, respectively. The Coulomb interaction in the momentum space, t/o(w,q) is given by
Oo(u>,q) = - ^72, :
(3)
corresponding to the usual Coulomb potential in coordinate space:
U
^ = jk~r-
(4)
(The standard Si-units are used here.) In Eq. (2), n 0 (aj,q) is the polarization insertion calculated at the first loop level. In the following we shall consider only the static limit of the interaction (u —> 0). In the deuterium plasma both the deuteron and the electron fields have to be regarded dynamical variables (unlike the lattice atoms in the electron gas calculations of metal). Hence, the polarization
624
insertion has two terms, corresponding to both the electron and the deuteron loops. These can be written as 3
n 0 (o, (/ ) = n[)e)(oIg) + n[1d)(o,q) d3P n £ + q -~4 (2TT)3
f d3p n* + q --
n
B
(5)
J ( 2 7 r ) 3 £ p + q -~EP
£ P + q --Ep
where np1 (iip) is the Fermi (Bose) distribution for electron (deuteron) loop, respectively. Ep is the energy corresponding to the momentum ftp. It can be approximated to be the kinetic energy of a free particle. Note that the RPA approximation with the free particle energy spectrum used here is the same that has been extensively used in the standard electron gas calculations 3 producing (at least) a qualitative agreement with experiments. Consider the first term (the electron loop) in Eq. (5). The electron gas in metal is highly degenerate at the room temperature and consequently a reasonable approximation is to assume the electron states to be filled up to the Fermi energy and to be empty above it. The outcome is then the well-known Thomas-Fermi screening, which, however, has too long screening length to play any role in the fusion processes.4 Hence, we concentrate on the deuteron loop, the second term in Eq. (5). (We can assume alternatively that the electrons form a uniform average background.) If the temperature is high enough («300 K) and the deuterium plasma is not too dense, the Bose distribution can be replaced by the classical Maxwell distribution. The polarization insertion (corresponding to the deuteron loop) can then be written oo
n[)d)(0,(/) = - 3 e ^ f c T ^z ?
TT qnfi J o
fdxxe-x2ln
(6)
where b is given by b(q) = hq/V8mkT. The chemical potential /i of the deuterons can be related to their number density, n. If we assume [consistently with the energy approximation used in Eq. (5)] that the deuterons form an ideal classical gas, the number density of deuterons is
— (if)
3/2
(7)
Using this result we can rewrite Eq. (6) as 2
T(d),
47rafi.cn
K\o,q) = — — / ^ 4nahcn kT
1 . _„r=r- dxxe In v^F6 o
(8)
where a is the fine structure constant. The limits of the integral 1(b) can be easily found:3
625
7(0) = 1 and
1 j(b)«-L
=
Am kT J™-
(g-,00).
(9)
The function (8) should now be inserted into the effective interaction of Eq. (2), which in the coordinate space is p2 { d 3 o UeS(r) = - / ^ \
eiqr %
.
(10)
This effective potential represents the modification of the Coulomb's law by the medium composed of the electrons, the deuterons and the background atoms in the surface region. If the polarization insertion in Eq. (10) is replaced by its low momentum limit, the well-known Debye screening is obtained. The inverse of the screening length squared will be then ^ = - ^ ( 0 , 0 ) = ^
.
(11)
This gives the usual Yukawa-type screening of the Coulomb potential:
U^(r)=ahc^r-.
(12)
The inverse of the screening length go can be calculated provided that the number density of the deuterons is given. The density of the deuterons in the surface region of the palladium must exceed the corresponding density inside the metal (for the deuterons to be able to diffuse into the lattice structure of the metal). How much larger it will be is not known. It has been proposed that in the surface region the deuterium to palladium ratio, D/Pd > 2.0.5 If we take the modest estimate assuming the number density of the deuterons to be just twice the normal number density of bulk palladium (7.0 x 10 28 1/m ), the screening length then becomes 1/<7D = 3.2 x 10 m. Although this length is much smaller than the screening length obtained from the electron loop calculation, 4 it would still be too large to allow any fusion process to occur, if Eq. (12) were a sufficient approximation to the effective potential given by Eq. (10). Classically, the minimum distance of deuterons scattered by each other with thermal energies corresponding to the room temperature (300 K) is about 0.2 A if the Yukawa potential of Eq. (12) is used. The amount of time spent by the deuterons in such distances, however, would be far too short to produce detectable tunneling rates. However, it is evident that the usual approximation, in which the polarization insertion is replaced by its low momentum limit, is not sufficient here. This can be seen from the fact that the expansion parameter b = b(q) in Eq. (8) is of order 3 when q ss qv . Hence Eq. (10) has to be evaluated with greater accuracy by inserting the whole polarization function given by Eq. (8). To do this, numerical calculations have to be performed. The results (obtained by using MathCAD) are
626
shown in Fig. 1, the deuteron density being (1.4 — 2.8) x 1029 1/m (the deuterium to palladium ratio ranging from 2.0 to 4.0). The momentum dependence of the polarization insertion changes the Yukawatype screening potential to one having a minimum. This potential gives an attraction between the positively charged deuterons. The classical equilibrium distance of the deuterons given by this potential is 0.16-0.20 A for the deuteron densities mentioned above. On the other hand the (classical) minimum distance of the deuterons when they are not in a bound state but are scattered by each other with thermal energies varies in this density range from 0.12 to 0.15 A. The potential dip of this effective potential (arising from the influence of the medium to the Coulomb law) is too small to be able to bind electrons. However, by solving (numerically) the Schrodinger equation for more massive deuterons, one finds that these potential dips sustain two (£ = 0) bound states. The binding energy for the ground state varies from 2.5 to 3.7 eV, while for the excited state the binding energy varies from 0.6 to 1.0 eV, at the deuteron density interval quoted above. These energy states may provide a possibility to test experimentally the validity of the idea proposed here by studying the absorption of laser light the wavelength of which corresponds to the difference between the ground and the excited states.
15
""~ r
i
•
i
10
11 * 11
> CD
"<S'U* \ ** I
-6-
''• \ *' \ W
-10 0.1
#**.*JS^^
i
i
i
i
0.15
0.2
0.25
0.3
0.35
rlk Figure 1. The effective interaction potential between deuterons as a function of their mutual distance. The solid, dotted and dashed lines correspond to the deuterium to palladium ratio D / P d = 2.0, 3.0 and 4.0, respectively.
627
The screening potential found here can be considered as a counterpart of the Friedel oscillations in the zero-temperature electron gas. The crucial difference is that the Friedel oscillations do not provide bound states for the electrons, but the effective potential in this deuterium plasma bind the massive deuterons. Similar behavior for the effective interaction has been obtained also by other studies 6 although leading to somewhat larger equilibrium distances. The fusion rate for deuteron pairs in a bound state can be calculated from the value of the relative wave function iprei (ri — r 2 ) of the two deuterons at zero distance (or strictly speaking within the nuclear interaction range, which we will use 3fm). The rate is then given by X = K \Aei(0)\2 .
(13)
The fusion constant K for the 3 He process, D(d,n) He is known to be 1.48 x 10~ 2 2 m 3 /s being equal to the fusion constant for the tritium process D(d,p)T. In the numerical calculation the subroutine "Odesolve" in MathCAD is used to solve the Schrodinger equation to obtain the relative wave function. The fusion rate is then obtained from Eq. (13). Due to the stiffness of the differential equation quite many intermediate steps (of order 10000) are required for accurate results for the wave function. The calculation reveals that when the deuteron pair is in the ground state the fusion rate for D/Pd = 2,3 and 4 are A « 1 0 " 2 6 , 1 0 " 2 4 and 10~ 2 2 1/s, respectively. If light water is used instead of heavy water, similar behavior for the effective potential takes place. (Note that the Maxwell-Boltzmann distribution is also applicable for the protons. Although the electrons are degenerate, the more massive protons are not, at the room temperature and at the densities quoted above.) However, because the low energy limit of the S-function for the reaction P(p,7)D is 23 order of magnitude smaller7 than that of the deuteron reactions D(d,n) He and D(d,p) T, the rate for the proton-proton reaction is far too low to be detectable. Returning to the deuteron fusion, to find the fusion rate per second and per unit surface area, the thickness of the active deuterium plasma in the surface region and also the fraction of the deuterons being in the bound state must be known. If the thickness of the active surface region is about 1000 nm and if one-tenths of the deuterons are bound, 2 the fusion rates for D/Pd = 2, 3 and 4 are, respectively, about 10~ , 10 and 10 reactions per second and per square centimeter. The highest value of these fusion rates arising from the deuteron pairs is in agreement with the low-level neutron emission results reported by Jones et al.,8 but cannot explain the excess heat and excess 4 He claimed in other experiments. The order of magnitude character of our one-loop calculation for the fusion rate should be emphasized. Although the deuteron densities and the thickness of the surface plasma quoted above can be criticized, the sensitivity of the nuclear overlapping and consequently the fusion rate on the equilibrium distance implies that the claimed level of the neutron emission may be easily explained by the exact effective potential.
628
3. Nuclear Reactions in the Deuteron Trap In the previous chapter, we note that the order of magnitude of the fusion rate in the bound deuteron pairs is consistent with the low-level neutron emission obtained experimentally. However, there is a possibility how this effective attraction can cause considerable larger fusion rates. Note that the effective interaction discussed in Section 2 is also valid between the surface atoms and the deuterons. Compared to the case of the deuteron pairs, the polarization insertion is unchanged, while the effective interaction as a whole has to be multiplied by the atom charge number Z. Consequently, the classical equilibrium distance between the surface atom and the deuteron will be the same as for the deuteron pairs. However, the strength of the potential will be Z times the strength of the potential between the deuterons. (If the shielding of the core electrons are taken into account, the nuclear charge Ze should be replaced by an effective charge Zeg(r)e, which will reduce also the strength of the attraction potential. This does not, however, change the picture qualitatively.) The binding energies of the deuterons bound to the surface atoms by this effective interaction are anyway large enough that the bound deuterons are stable against neutralization. (The neutralization can take place by multiparticle interaction. However, the rate for such neutralization processes will be small.) The deuterons bound to the surface atoms of the cathode metal are not necessarily bound to a single surface atom but their wave function may be distributed to an extended potential of several surface atoms. In this way, a group of the surface atoms can form a deuteron trap. As the cathode metal is loaded by deuterium, the number of the deuterons bound by these surface traps will increase. The extension of these surface traps can depend sensitively and in an unknown manner on several factors, like the smoothness of the surface, lattice impurities and defections and even on the chemical composition of the electrolyte. It is possible that, when the deuterium loading (in the surface region) is very low, the traps are formed by only one single surface atom, but when the deuterium loading increases, the embedded deuterons can provide "bridges" joining the attractive potentials of two adjacent surface atoms, leading to more extended traps. As we know neither the dimensions of the traps nor the wave function of the ground state of the deuterons in these traps, we have to proceed at a very general level, in order to extract the main physical consequences of these deuteron traps. Consider the transition from N + 1 trapped deuterons to the final state consisting free deuterons and the fusion product (s). There will be N particles in the final state, if we consider 4He-channel, and N + 1 particles for tritium and 3He-channels. The transition rate is given by the golden rule (*free
H
^trap /
where p is the density of the states given by
/
V \N
p = 6(Et-Ei)(j^)
N
IIdV
( 15 )
629
Note that the conservation of momentum does not require here the existence of a photon in the final state in the 4He-channel, because the momentum is transferred by the other deuterons in the final state. We regard here the initial deuterons as free particles confined in the trap volume VQ. Their momenta are negligible when compared to the momenta of the final state particles. As the Hamiltonian that is responsible for the nuclear reaction, we use the Fermi pseudopotential: 47r?L2 anucl<5(r), (16) m where anuci is the nuclear scattering length. We can assume that the nuclear scattering length for the 4He-channel and for the tritium and 3He-channels are of the same order due to the absence of the extra electric coupling to the photon field in the 4He-channel here. For the elastic interaction between deuterons sharing the released energy we use similar pseudopotential as Eq. (16) the scattering length for those interactions being ae\. The process, where the energy is collectively distributed among all the deuterons in the trap, contains N — 1 elastic interaction between the deuterons (in the tree-diagram level). Hence, the rate will be of form: H =
2
. /A„k„
. x
*_(*£-) KMo,,'^)
2
^ -
1
)
In Eq. (17), the functions G(wj,qi) are the propagators corresponding to the virtual lines (the spin indices have been deleted for simplicity).
G(wi,cu) =
J
. , ,
(18)
where T is the line width corresponding the decay of the virtual deuteron to the lower energy states, uji and qi are the frequency and the wave vector of the virtual lines (depending on the final state wave vectors p in such a way that the frequency and the momentum are conserved at all the verteces in the Feynman diagram). As we shall see below, the dominant contribution to the transition matrix arises from the diagrams of the type, where the energy released is distributed most effectively (so that the energies of the virtual particles split consecutively by interactions with internal state deuterons). That kind of a diagram is shown in Fig. 2. Now, consider a virtual deuteron that interacts with a initial state deuteron so that both of them become free particles at the final state. The conservation of the energy and the momentum determine that the propagator of the virtual particle, Eq. (18), has to be
G(w ft) =
*'
** | ** nl+«f ~ W 2m" 1 " 2m
2m
(19)
2L I "
where p and q are the wave vectors of the two final state deuterons. From Eq. (19), we note that there will be a resonance, if the final state momenta are perpendicular
630
AA
AA
AAAA
AAAA AAAA
AAAA AAAA
Figure 2.
The type of the diagrams having largest contribution to the fusion rate.
to each other. Furthermore, there will be multiple resonances, if the final state momenta are such that after every vertex the momenta of the two (virtual or real) particles are perpendicular to each other. For this multiple resonance scattering to occur, N — 3 components of the final state wave vectors are restricted to be small. Moreover, the conservation of momentum gives three extra constraints. For the diagram shown in Fig. 2, the momenta of the internal and final state particles are shown in Fig. 3 for this multiple resonance situation. Note that in Fig. 3, the two first momenta have to be opposite to each other due to the conservation of momentum.
Figure 3. The momenta of the virtual and final particles in the multiple resonance scattering corresponding to the diagram in Fig. 2.
631
Assume that we integrate over the TV — 3 small components of the wave vectors that are responsible for the resonances in the internal lines. Equation (17) becomes then A=(^^)2|^e1(0)|2(^)2(iV"1)
J
c
(2TT)™ Vo
V
\2^2mi
I Q2 Q*T* r 2 1111
qjT'
where qj are some combinations of the remaining 2N components of the final state wave vectors. Note that we have neglected the small components of the final state wave vectors in the energy delta function before the integration. The reason, why the diagrams of the type shown in Fig. 2 have the largest contribution to the transition rate, is that the wave vector combinations qj in Eq. (20) have the smallest numerical values, if the energy released in the fusion process is distributed most effectively as described above. Noting that the final state wave vectors are of the order pt ss \j2mQ/N /h, the wave vectors qj in Eq. (20) range from ^j2mQ/N/h to \/mQ/h. The product in Eq. (20) can then be approximated (for the type of diagrams shown in Fig. 2): N 3
~
/tav\C- 3 )/ 2
1
Si-"(££)
•
where A is some numerical constant of order unity. In the delta function of Eq. (20) the mass corresponding to the fusion product (s) is not the deuteron mass m. However, at the large N limit we can replace it also with the deuteron mass without making any essential difference. The delta function in Eq. (20) can then be written as 'IE S2^2
\
/t2^2
where p is the length of the 2TV dimensional wave number vector in Eq. (20). Moreover, the 2N dimensional integration volume element can be written as 27V
YldPj =
d™p=2-£^p™-idp [
J=I
2
>
(23)
where the Stirling's approximation: T{x) « xx-1/2e-xV2ir,
(24)
has been used. The transition rate given by Eq. (20) becomes now „7V X
~
A
™
V'rel 0
jViV-3 (27V - l)2iV-2 W
— QN-*(^ael)AN-Ah2N r2JV-2y2/Vm/V-l
(25)
632
where all the numerical factors (independent of N) have been embedded in the factor A'. We define here a constant E*, which has the dimension of energy. 4n2e2a4e]h2"
[
]
(Note that e in Eqs. (25) and (26) is the Neper's number and not the electric charge.) By the energy constant of Eq. (26) the transition rate can be written as
^c^W^^p'2,
(27)
where all the numerical factors are now in the constant C. Moreover, 27V — 1 in Eq. (25) have been replaced by 2N. This transition rate, Eq. (27), is extremely sensitive function of the trap occupation N and the energy released Q. At fixed N the rate is a monotonic and rapidly increasing function of the released energy Q. This shows that practically only the process having the largest possible releasing energy could take place. In the case of a fusion of two deuterons considered here, this is the 4He-channel, directly to the ground state. (For processes involving only two deuterons the tritium and 3He-channels are dominant in the usual way. So the inclusion of the trapped deuterons, besides the deuteron pairs discussed in Section 2, increase somewhat the neutron emission rate. However, for larger values of the trap occupation N, the rates of these two deuteron processes are vanishing small compared to the collective iV-deuteron MRS-rate.) Note that only few per cent change in the released energy (corresponding to the reaction to the first excited state) leads to the transition rate that is several orders of magnitude smaller than the transition rate to the grounds state even for moderate values of the trap occupation N. As the dominant fusion process will be d + d —> 4 He (to the ground state and without any final state photon) there will be no radiation (except possible soft secondary radiation caused by the free deuterons in the final state having kinetic energies typically in keV range). When the trap occupation N increases, the rate given by Eq. (27) increases by two ways. First, there is the rapid change arising from the factor:
fW = ( ^ )
.
(28)
Second, the overlap of the deuteron wave functions |^>rei(0)| increases, when the density of the deuteron gas in the trap increases. If we consider the fusion rate as a function of the trap volume VQ, we note that there will be a "window", where the fusion can take place. If the trap volume is too small (the trap consisting only one or very few surface atoms), the trap cannot maintain such a high deuteron occupation that the factor f(N) could be large enough to produce detectable transition rates in Eq. (27). On the other hand, for very large trap volumes the deuteron gas in the trap remains dilute (so that the nuclear overlapping factor |^>rei(0)| remains
633
small) until the factor f(N) has passed already its maximum value and is decreasing preventing the fusion to occur. However, if the t r a p volume is in the fusion "window", the 4 He-fusion occurs inevitably, when TV become large enough. As a m a t t e r of fact, the fusion rate therefore depends ultimately on the rate by which the occupation increases in these traps. It should be noted t h a t larger released energies are obtained in multi deuteron processes (with two or more deuterons reacting with a heavier nucleus). T h e expression for the rate in these t r a n s m u t a t i o n processes, corresponding to Eq. (27), contains more t h a n one nuclear overlapping factor |i/>rei(0)| . T h e overlapping of a deuteron and a heavier nucleus depends similarly on the deuteron density in the t r a p , as the overlapping of two deuterons, although less sensitively. Similarly, as for the fusion reaction, there are "windows" in the t r a p volume for the different t r a n s m u t a t i o n processes. At larger volumes the t r a n s m u t a t i o n processes are more probable t h a n the fusion process due to the larger releasing energy and the smaller value of the deuteron overlapping. W h a t t r a n s m u t a t i o n reactions can really occur, depends then on the released energy Q, the nuclear charge number Z, the t r a p volume VQ and the scattering lengths. There are large uncertainties in the numerical values corresponding to the t r a p volume and to the elastic scattering length and also to the line width. These uncertainties prevent us from predicting the relative transition r a t e of the transmutation processes to t h a t of the 4 H e -fusion process. Anyway, we can understand by this model t h a t the ratio of the excess heat to the excess 4 H e varies depending on the volumes of the traps. If light water is used instead of the heavy water the surface atoms can similarly t r a p t h e protons. In t h e case of light water, however, there will be no p r o t o n - p r o t o n fusion, because the energy released is too low. Anyway, t r a n s m u t a t i o n processes with large released energy can take place. We can also expect to obtain fusion reactions a n d / o r t r a n s m u t a t i o n processes in other type of experiments (e.g., gas permeation experiments, etc.) provided t h a t deuteron traps, similar as here, emerge. 4. C o n c l u s i o n s a n d O u t l o o k We assumed t h a t in the electrolysis of heavy water the deuterium ions reaching the cathode form (together with the electrons around) a deuterium plasma in the surface region of the host metal. We calculated the effective potential at one loop level with energy spectrum of free particles. W i t h these inputs we found t h a t the deuterons experience an attractive potential, which sustain b o u n d states for deuteron pairs. T h e equilibrium separation of the deuterons in this effective potential is of the order t h a t allow the fusion processes to occur with low but detectable rate for the neutron emission. Furthermore, we assumed t h a t the surface atoms can t r a p the deuterons by this effective potential. T h e fusion processes in these t r a p s were considered
634 assuming t h a t the t r a p p e d deuterons collectively share the released energy becoming free particles. A simplified model with general argument was used to extract the main physical consequences of the processes. It was shown t h a t the rate of the nuclear process increases very rapidly with the releasing energy showing t h a t the 4 He-channel is in practice the only emerging fusion channel. Moreover, we argued t h a t t r a n s m u t a t i o n processes having similarly large releasing energies occur. For further research a more refined model for the deuteron t r a p is required and the ground state in this t r a p has to b e solved. Moreover, t h e numerical uncertainties corresponding t o the iV-particle scattering matrix element has to be reduced in order to obtain accurate predictions of the relative rates for the fusion and transmutation processes. In order to get an estimate for the absolute reaction rates, better knowledge is required on the details of the flow dynamics and the surface structure and their influence to the t r a p formation and to the t r a p occupation rate.
Acknowledgements I would like to t h a n k Carl-Gustav Kallman for valuable discussions and comments.
References 1. M. Fleischmann, S. Pons, and M. Hawkins, J. Electroanal. Chem. 261, 301 (1989). 2. T. Toimela, to appear. 3. A.L. Fetter and J.D. Walecka, Quantum Theory of Many-Particle Systems (McGrawHill, 1971). 4. S. Feng, Solid State Commun. 72, 205 (1989). 5. E.K. Storms, Infinite Energy 1, 7 (1996). 6. K. Czerski, A. Huke, P. Heide, and G. Ruprecht, Europhys. Lett. 68, 363 (2004). 7. W.A. Fowler, G.R. Caughlan, and B.A. Zimmerman, Annu. Rev. Astron. Astrophys. 5, 525 (1967). 8. S.E. Jones, E.P. Palmer, J.B. Czirr, D.L. Decker, G.L. Jensen, J.M. Thome, S.F. Taylor, and J. Rafelski, Nature 388, 73 (1989).
MULTIPLE SCATTERING THEORY A N D CONDENSED MATTER NUCLEAR SCIENCE - "SUPER-ABSORPTION" IN A CRYSTAL LATTICE
X I N G Z. LI, BIN LIU, Q I N G M. W E I , A N D N A O N. C A I Department
of Physics,
Tsinghua
University,
Beijing
100084,
China
SI C H E N , SHU X. Z H E N G , A N D D O N G X. C A O Department
of Engineering
Physics,
Tsinghua
University,
Beijing
100084,
China
A simple one-dimensional model is used to illustrate "super-absorption" in a crystal lattice. The WKB method is applied to calculate the reflection rate and the transmission rate for a single cell. Then matrix algebra is manipulated to give the relation between the single cell and an array of N cells. The selective resonant tunneling in this array of N cells is discussed, and the dependence of the absorption rate on the number of the cells is calculated to show the difference between coherent and non-coherent systems.
1. I n t r o d u c t i o n Super radiation was proposed in 1950s by Dick. 1 Super radiation means t h a t the resultant intensity of N coherent optical sources will be proportional to iV 2 instead of N. One might ask t h a t if light is absorbed by A^ points of an absorber where the light is coherent in phase; then, what would happen? Would the absorption be enhanced or reduced? T h e answer is, "the absorption would be enhanced when certain resonant conditions are satisfied." T h e resonance conditions include not only the frequency of incident waves, which should be in resonance with the absorbing medium, but also the absorption coefficient in the medium, which should match with the attenuation of the wave in propagation. We will discuss this matching in the single cell first; then, we will discuss the matching in a crystal lattice. This enhanced absorption might be called as "super-absorption." 2 ' 3 An experiment has been proposed to detect the effect of this "super-absorption." Experiments have showed the wave nature of the deuteron inside the palladium deuteride (hydride) already. 4 ~ 7 Hence, the Multiple Scattering Theory (MST) is supposed to show the correlation between the anomalous deuterium flux and heat flow. As a first step, a simplified one-dimension model is described to show qualitatively the feature of the M S T . Non-coherent diffusion process is quite different from the coherent wave propagating process. 635
636
2. Selective Resonant Absorption in a Single Cell Figure 1 shows the single cell of a lattice. The wave function of the incident particle might be reflected by a potential barrier (U2), or trapped by a potential well (Ui or U3 = Uzr + iUsi), or tunneling through the double barriers. In the planewave-representation, a 2 x 2 matrix M may be introduced to describe the relation between the amplitudes of these wave functions. Having assumed that the potential energy in the well and barrier varies so smoothly that the WKB method is valid, we may write the M matrix as: 2,3,8
!expHA][2sin(§) M
^iexp[_iA](4^-iiJ)cos(i)
i§exp[i£](402-^)cos(&)
iexp[i£][2Sin(^) -z(4^ + Ii5)cos(i)] (1)
Here, Ji
= J VME
/
Ui)dr,
(2)
2/i(E/2 - E) dr, h2
(3)
1
J2 = J VME - U3)dr,
(4)
/i is the reduced mass, U\, U2, and U3 are the potential in the regions 12, 23, and 34, respectively, E is the energy of the incident particle, r the distance in one-dimensional space, H is the Planck constant divided by 27r. In the plane-wave-representation, the tunneling wave is represented by a column vector as 1 0
(5)
On the left-hand side of the single cell, the wave function is represented by "Afn" M21
M
Hence, for this single cell, the tunneling rate, T\, is defined as
(6)
637
Incident Mn Tunneling 1
Imaginary potential U3 to describe absorption in well
Figure 1. M matrix is used to describe the incident plane wave {M\\), wave (M21). The amplitude of the tunneling wave is fixed as 1.
and the reflecting plane
The reflection rate, R\, is defined as Ri
\M-21 |Afn
(8)
When the imaginary part of the potential vanishes, i.e., C/3i = 0; then, the conservation of the probability requires:
|M n | 2 = l + |M 21 | 2 .
(9)
However, U^i is introduced here to describe the absorption in the region 34. Thus the absorption rate, A\, is defined as A1
=
l
1 + |Af211 :
(10)
| M ]i l l
When the wavelength of the incidental particle changes, the phases of the reflecting wave from the first barrier and the second barrier also change. The superposition of these reflecting waves will determine the amplitude of the wave reflected by this single cell (i.e., M21). It will show a resonant feature. The resonance happens when
«»f£l-0.
(")
In the case of resonance, the perfect tunneling happens and the reflection is zero, i.e., T\ = 1, and R\ = 0. However, if there is any absorption in the well region 34;
638
then, cos ( | ) ^ 0 .
(12)
In other words, the absorption will introduce the reflection (M 2 i ^ 0) even if in the case of resonance. Now one may ask a question: when the module of the imaginary part of the potential, \Usi\, is getting greater and greater, will the absorption rate, R\, get larger or smaller? The answer is: "the absorption rate will be get larger first; then it will get smaller." The physical reason is the interference of two reflecting waves. When |C/3,| is getting greater, the reflecting wave from the second barrier would be much weaker; then, there is no way to make M 2 i = 0. Thus, there will be a competition between the absorption and reflection. When the Uzi = 0, there is no reflection because M21 = 0 in the case of resonance; however, there is no absorption also in this case, because \Mu\ = 1 + |M 2 i| . On the other hand, if Usi —> —00; then, cos(J2/2h) —> 00, and A\ —> 0. Consequently, we may find an intermediate value for U-a which makes A\ maximized. This is a feature of selective resonant absorption. 9 " 14 Not only the energy, E, has to make the real part of J 2 , J 2 r = 2nirh(n = 1, 2, 3,...), but also the absorption capacity, U^i, has to match a specific value. Figure 2 just shows that the absorption rate A± reaches a peak at the value of t/3; between 0 and -00. (6 was assumed to be 10 in Fig. 2). Here, arc sinh
2#2 + _L ) s m h
, / ^ J^lnlVME-U^r.l
v
-
(^ K-Ust) ( E u ^ r ,
(13)
(14)
(15) M2i = - ^ c o s a ,
(16)
QP QP
= 26>2 +
Qm
= 2027T
802
(17)
1 (18)
a = 2 + ',A. (19) We may notice that J\ does not effect the value of tunneling rate or the reflection rate for the single cell. The situation will be quite different when we calculate these rates in the case of multiple cells.
639
Figure 2.
Absorption rate for single cell reaches a peak at selective damping, Usi
3. Selective Resonant Absorption in a Crystal Lattice Figure 3 shows a series of cells, which represent the potential inside a crystal lattice. The reflecting waves from each single cell will affect the total reflection rate, Rpj. = v-^-
RN
The matrix of N cells, M in terms of N and a:
(20)
, may be expressed by the matrix of the single cell, M, N
_
sin(Na)
L
2\
N
(21)
M21,
sin a
_ sm(Na)Mn
- sm[(N - I)a]
(22)
sina a = arc cos arc cos cos
— h
26z
sin —: \2h
— cos — • (23) h V 2fi The wave propagation in the lattice cell region will affect the phase of the reflecting wave. This effect is represented by Ji in the expression of a. When (2n+l)?rS Ji
a = arc cos
202
sin
( n = 1,2,3,...), J2 2h
(24)
(25)
640 Incident ( M \
Tunneling 1
Figure 3. A chain of single cells to represent the potential energy inside a crystal lattice for a charged particle.
The resonance condition for a single cell without absorption is J 2 = mnh
(m = 1, 2, 3,...).
(26)
It gives: a = mir/2. However, if U$i ^ 0; then, (27)
J 2 = nh + iJ2i, a = arc cos it
^ +«log
2<92 + J-
I I -isinh
V + V1 + V'
Jit
~2h •iA,
y = QPx,
(28) (29) (30)
x = sinh
A = arcsinh
202
~2h —xI sinh ( —4802 J V 2ft
(31)
(32)
We may plot the absorption coefficient of N cells, AN, as a function of A in Fig. 4. The curves share the same feature that AN always equals to zero when A = 0; and there is always a peak of AN at certain A p . However, when the number of cells, N, increases, this peak value of AN increases, and the location of this peak, A p approaches 0. The physical reason for this behavior is just the selectivity of the resonance tunneling.9~14 When A = 0, it means U$i = 0 (i.e., there is no absorption at all); hence, AN = 0. However, if the absorption is too strong (A —> oo); then, the reflection from the first cell is inevitable and there is no way to cancel it by any reflection from other cells. As a result, at certain immediate value of A, the total absorption coefficient will reach its maximum value. The higher the number of cell is, the higher the chances that reflection wave will be cancelled. It means that more
641
Figure 4. The peak of absorption rate shifts towards smaller A, and the peak is getting higher for greater N.
waves will enter the array of the cells and undergo the absorption there. As a result the peak value of absorption, AN, increases with N. The peak value appears at the lower absorption, A p , for greater N, because the cancellation of the reflecting wave requires less absorption for more cells.
4. Comparison Between Coherent and Non-Coherent Array of N Cells It is interesting to compare the behavior of coherent cells and the non-coherent cells in order to see the "super-absorption." In Fig. 5 the non-coherent beams are plotted for the consequent reflections and penetrations. The phase of the wave disappears in this figure, because only the module of the wave is concerned. We still use the same reflection rate, Ri, and the transmission rate, T\, for a single cell, but the phase J\ would not appear any where in the expression of RN (non), or TJV (non). The non-coherent reflection rate RN (non), and transmission rate TN(non) for N cells may be expressed by recursion formula in terms of R\ and T\ as follows:
642
N cells
1cell
z>
r
N*rl
= > TN* R,* RN* I,
7"W*«1 ' T w - O
T- N *fl 1 *fl N *fli...r N
Total reflection:
Total tunneling:
TN*m^*RN)
Figure 5.
Flux flow for the case of non-coherent beam.
-RjV+1 =
<-N+l
RN
•Ti JV
TN*R\*TN
(1 -
Ri*RN) Ti
(l-iii*i?Ar)'
(33)
(34)
From Eqs. (33) and (34), it is clear that i?jv+i > RN, and TJV+I < TN- There is no way to make RN = 0, if R\ ^ 0. However, in the case of coherent case, RN may equal to zero even if R\ ^ 0. This is the first distinction between the non-coherent and coherent case. There is another distinction between two cases as follows. For the non-coherent cases, i?i and T\ may be assumed to be same as that for coherent case [Eqs. (15-19); Fig. 6a]; however, i?2 and T2 will be calculated according to Eqs. (33) and (34). In Fig. 6b, we see that (R2 + T2) = 1-A2 forms a minimum also. Nevertheless, this minimum is different from that of the coherent case. We may define an escaping rate as (1-AN); then, this escaping rate would reach its minimum value when the absorption rate, AN, reaches its peak value. In Fig. 7 this minimum escaping rate is plotted as a function the number of the cells. The open circles are for the non-coherent cells [Eqs. (33) and (34)]; and the solid circles are for the coherent cells [Eqs. (20)-(22)]. Those circles may be fitted by two fitting curves. For non-coherent cells: 1 - Ajv(non)
0.5356 JSfO.82 '
(35)
643
0.8 } \ "1 + T1
06 f?2+ T2 "1
0.4 R2
1
1.5 A
Figure 6.
(a) Minimum of (Ri + Ti) and (b) minimum of (R2 + T2).
0.6
1
1
1
1
1
1
1
1—
Fitting curve: 0.5179/A/1-3 for super absorption
-5
0.5
f,
0.5356/AF for non coherent case
+ (D
0.4
to en c Q. CO O
0.3
w 0
o E E c
0.2
03
I-
-©,.
0.1
0.0
j
2
--©--... "~o~-—
1
4
6
8
10
Number of cells (A/) Figure 7.
The minimum of (1 — AN) as a function of number of cells.
644
For coherent cells: 0.5179 ~A^KiJfTM--
1
, x (36)
T h e dependence on N for coherent cells is stronger t h a n t h a t of non-coherent cells. This is the effect of "super-absorption." It is not the dependence of 1/N2, because in this one-dimensional case, N cells in an array are not equal. In the slab model, N cells in each slab are equal; then, the result would be different. I t would be discussed later in another paper.
5. C o n c l u d i n g R e m a r k s Although a special W K B model is used in this illustration, the feature is quite general: (1) T h e definition of resonance here is no longer an energy level only. It should include a matching damping, i.e., the absorption capacity [7^. This resonance condition varies with the number of the cells. However, it always corresponds t o t h e condition of least reflection; i.e., minimizing t h e m a t r i x element (MN)2iThis concept t u r n s out to be very important when we discuss the correlation between anomalous deuterium flux and the heat flow in a D / P d system. (2) T h e wave of deuterons inside the palladium deuteride is quite different from a non-coherent deuteron beam. Their behavior is very different in propagation (reflection, transmission, and absorption). Hence, the coherence of the deuterons inside the crystal lattice is essential in explaining the macroscopic behavior of deuterium flux permeating the P d thin film. (3) There is no way to have any resonant behavior in a non-coherent deuteron beam, because the reflection rate, i?Ar(non), would never be zero.
Acknowledgments This work is supported by T h e Ministry of Science and Technology (Fundamental Division), Natural Science Foundation of China (#10145004 and #10475045) and Tsinghua University [Basic Research Fund (985-1)].
References 1. R.H. Dicke, Coherence in spontaneous radiation processes, Phys. Rev. 93, 99 (1954). 2. X.Z. Li, et al., Super-absorption - the effect of crystal lattice on enhancement of nuclear reaction, in Proceedings of the 2001 Chinese Physical Society Fall Meeting (Shanghai, China, September 20-23, 2001), p. 98 (in Chinese). 3. X.Z. Li, B. Liu, et al., Super-absorption - correlation between deuteriumfluxand excess heat, in Proceedings of the ICCF-9 (Beijing, China, May 19-24, 2002). X.Z. Li (Ed.) (Tsinghua University Press, 2003), p. 202.
645 4. X.Z. Li, et at, Pumping effect - reproducible excess heat in a gas-loading D/Pd system, in Proceedings of the ICCF-9 (Beijing, China, May 19-24, 2002). X.Z. Li (Ed.) (Tsinghua University Press, 2003), p. 197. 5. X.Z. Li, J. Tian, et al., Correlation between abnormal deuterium flux and heat flow in a D / P d system, J. Phys. D: Appl. Phys. 36, 3095-3097(2003). 6. Xing Z. Li, et al., " Progress in gas-loading D/Pd systems: The feasibility of a selfsustaining heat generator," Proceedings of ICCF-10, Sept. 19-24, 2003, Cambridge, USA. 7. X.Z. Li, B. Liu, Q.M. Wei, G.L. Schmidt, and J. Tian, Anomalies correlated with abnormal deuterium flux and heat flow in D(H)/Pd systems, W.E. Collis (Ed.), in Proceedings of the 5 Asti Workshop on Anomalies in Hydrogen/Deuterium Loaded Metals (Asti, Italy, March 19-21, 2004). 8. D. Bohm, Quantum Theory (Prentice-hall Inc., New York, 1954). 9. X.Z. Li, Overcoming of the gamow tunneling insufficiencies by maximizing a dampmatching resonant tunneling, Czech. J. Phys. 49, 985 (1999). 10. X.Z. Li, J. Tian, and M.Y. Mei, Fusion energy without strong nuclear radiation, J. Fusion Energy 18, 51 (1999). 11. X.Z. Li, et al, Maximum value of the resonant tunneling current through the coulomb barrier, Fusion Technol. 36, 324 (1999). 12. X.Z. Li, J. Tian, M.Y. Mei, and C.X. Li, Sub-barrier fusion and selective resonant tunneling, Phys. Rev. C61, 024610 (2000). 13. X.Z. Li, Nuclear physics for nuclear fusion. Fusion Sci. Technol. 4 1 , 63 (2002). 14. X.Z. Li, et al, Study of nuclear physics for nuclear fusion, J. Fusion Energy 19, 163 (2002).
F R A M E W O R K FOR U N D E R S T A N D I N G LENR PROCESSES, U S I N G C O N V E N T I O N A L C O N D E N S E D M A T T E R PHYSICS
S C O T T R. C H U B B Research
Systems
Inc.,
9822 Pebble Weigh Ct., Burke E-mail: [email protected]
VA 22015-3378,
USA
Conventional condensed matter physics provides a unifying framework for understanding low-energy nuclear reactions (LENRs) in solids. In the paper, standard many-body physics techniques are used to illustrate this fact. Specifically, the paper shows that formally the theories by Schwinger, Hagelstein, and Chubb and Chubb (C&C), all can be related to a common set of equations, associated with reaction rate and energy transfer, through a standard many-body physics procedure (i?-matrix theory). In each case, particular forms of coherence are used that implicitly provide a mechanism for understanding how LENRs can proceed without the emission of high-energy particles. In addition, additional ideas, associated with Conventional Condensed Matter physics, are used to extend the earlier ion band state (IBS) model by C&C. The general model clarifies the origin of coherent processes that initiate LENRs, through the onset of ion conduction that can occur through ionic fluctuations in nanoscale crystals. In the case of PdDj,, these fluctuations begin to occur as x —> 1 in sub-lattice structures with characteristic dimensions of 60 nm. The resulting LENRs are triggered by the polarization between injected d's and electrons (immediately above the Fermi energy) that takes place in finite-size PdD crystals. During the prolonged charging of PdDx, the applied, external electric field induces these fluctuations through a form of Zener tunneling that mimics the kind of tunneling, predicted by Zener, that is responsible for possible conduction (referred to as Zener-electric breakdown) in insulators. But because the fluctuations are ionic, and they occur in PdD, nano-scale structures, a more appropriate characterization is Zener-ionic breakdown in nano-crystalline PdD. Using the underlying dynamics, it is possible to relate triggering times that are required for the initiation of the effect, to crystal size and externally applied fields.
1. Introduction An important challenge for theory is to explain why high-energy particles are almost never emitted in LENRs. In fact, through wave-like effects that can occur in condensed matter systems, it is possible for large amounts of momentum to be transferred instantly to distant locations, without requiring that any particular particle (or particles) acquire high velocity. In Refs. 1 and 2, the author provided a context for explaining how this can occur through a combination of structural effects (related to crystalline order) and dynamical changes (resulting from momentum fluxes of charged particles) at the boundaries of ordered regions, and through a phenomenon [Broken Gauge Symmetry (BGS)], in which many particles coherently move, at once. Specifically, in Refs. 1 and 2, the author identified 646
647
a particular Gauge Symmetry (the invariance of the ground state, in bulk regions, which are electronically neutral, with respect to rigid translations that do not alter the separations between charged particles) that is the basis of Mossbauer-like processes, in which a solid, as a whole, can recoil in response to an outside force. The associated BGS refers to the fact that near surfaces and interfaces, where charge can accumulate, a preferential gauge, and zero of momentum, is required for each charged particle. In Ref. 1, the author explicitly identified features associated with the electronic structure of fully loaded palladium (Pd) deuteride (PdD a , x —> 1) that explain how this can occur. In particular, the electronic states in PdD, in the immediate vicinity of the Fermi level, are delocalized and have small overlap with the octahedral site region locations of the D-nuclei (deuterons d's). Because of this fact, in finite, PdD crystals, outside forces are always needed in order to sustain high loading, and slight variations in loading are required to induce long-range coupling, through vibrational modes that have conventionally been thought to involve acoustical phonons. In fact, in the limit of small variations in loading, these vibrations, are not conventional phonons because the associated coupling does not conserve the number of d's that are present in the crystal. Instead, in the extreme low-temperature limit, a more appropriate starting point is the ion band state (IBS) picture 4 in which each d effectively occupies a delocalized state, similar to the delocalized (energy band) states that electrons occupy in ordered solids. In Refs. 2 and 3, the author used a generalization of a well-known procedure (Multiple Scattering Theory) in order to explain how the initial IBS theory 4 is related to a more complete description of the nuclear physics problem and to situations in which disorder is present. In Ref. 1, the author generalized these results to finite size crystals, with real boundaries. In fact, the essential physics of these papers, 1 _ 3 which involves identifying relative time-scales associated with particular transient, resonant processes, is really quite general: it can be re-expressed using standard many-body physics techniques (e.g., conventional .R-matrix theory 5 ). Within this context, it is possible to identify relationships between particular theoretical approaches (Hagelstein's "Unified Phonon-Coupled SU(N) Model/Resonant Group Method," 6 Schwinger's "Nuclear Energy in an Atomic Lattice," coherent phonon model, 7 e.g.) that involve resonant processes and the IBS 1 ' 4 model. In Section 2, the author examines this relationship and the importance of certain features (e.g., boundaries) that can be included within the more general approach 1-3 that are not included in Refs. 6 and 7. The Generalized Multiple Scattering Theory (GMST) can be used to identify particular forms of coherence and to assess their impact (based on reaction rate and overlap with externally applied fields) on potential dynamical processes. In particular, during the overcharging of portions of a sub-lattice of PdD, using GMST, it can be shown that the fastest, most coherent, dynamical reactions do not alter the charge in the interior (bulk-like) regions of the associated structure. This can occur when the momentum from a particular LENR is transferred directly to the
648
center-of-mass of the particles in the sub-lattice, in a manner that mimics the recoil of a solid in response to the absorption of a gamma ray, in the Mossbauer effect. Because the associated process does not alter the relative energies or momenta of any of the charges in the "bulk-like" neutral region, it does not alter the ionic charge appreciably, in these regions. (Here, the bulk region refers to the portion of the sub-lattice, where, on the average, no net charge is allowed to accumulate in each unit cell.) Instead, the process induces variations in the ionic charge at the immediate locations of potential reactions and in surface/interface regions, outside the bulk region. (Technically, since a net accumulation of charge is allowed to take place at the locations of potential reactions, as well as at other locations near surfaces and interfaces, these regions are located outside the "bulk region.") This can occur in a particular limit in which each d occupies the same (lowest energy) IBS, initially, and, effectively, with respect to the remaining (non-IBS) dynamical changes (associated with charge transport from electrons) that result from the presence of an applied electric field, as a function of wave-vector, all of the (lowest energy band) IBSs share a common energy eigenvalue. In this limit, as a function of time, all IBS eigenvalues, effectively, are degenerate and will remain degenerate with respect to order-preserving processes. These processes provide a way for the momentum of any collision or reaction in the entire sub-lattice to be shifted, rigidly, to its center-of-mass in response to externally applied fields. The kinds of order-preserving processes that can allow this to occur are referred to as Umklapp Processes or U-Processes. Beginning from the ground state (GS) of an ordered sub-lattice, involving a finite number of atoms, processes that preserve order can only be initiated, provided the initial and final states differ by specific amounts, and provided the amount of momentum that is imparted does not exceed a particular, maximum value. Because, in the presence of an externally applied field E, the momentum of each charged particle is shifted, as a function of time t, by an amount eEt, the requirement that specific values of momentum are associated with greatest coherence is equivalent to requiring that, at particular times, resonant (Umklapp) processes take place. The additional constraint that the change in energy associated with the process be so low that the particles in the bulk region of the solid remain in their GS, further restricts how energy and momentum can be transferred during the associated processes. The physics of the associated limit essentially is the same physics that describes the onset of conductivity in insulators, through Zener-electric breakdown,8 in which electrons in a filled electron band are subjected to electric fields for such a long time that they effectively tunnel into the first excited state band, where they then, effectively, move (and conduct electricity) through the normal transport processes associated with conventional band theory. Three important differences are: In the PdD situation, (1) the conduction involves ions, not electrons, (2) instead of dealing with a filled band, all d's occupy the same state, but this state, effectively, always has vanishingly small dispersion (so that the ions in the state do not create a
649
current because the energy of the state is not altered by changes in the momentum), and (3) the effect is initiated in nano-crystalline structures of PdD (as opposed to macroscopically large insulators). In Section 3, the author explains the physics of the associated limit, and its implications. This includes a plausible explanation for the frequently observed (but poorly understood) requirement that the onset of an LENR in the PdD system does not occur at the time that high loading is achieved. In particular, a finite incubation (or triggering) time is required that can vary between minutes, hours, days, and (in some cases) even weeks. The triggering time requirement involves crystal size: beginning with 60 nm nano-crystalline structures, LENRs are initiated with triggering times that are on the order of minutes through ionic fluctuations (associated with Zener-ionic breakdown); in micron size crystalline structures, the required triggering times (through Zener-ionic breakdown) are on the order of 10s of hours. 2. Framework for Understanding LENR Based on Many-Body Physics A standard many-body physics technique, i?-matrix theory 5 can be employed to understand the relationship between several theories that have been proposed as explanations of LENRs. In particular, in i?-matrix theory, the effects of a particular interaction are introduced by dividing all of the (possible) many-body configurations into two sets, associated, respectively, with: (1) states that involve physically measurable quantities (involving a restricted set of energies and momenta); (2) the remaining states. Then, by construction, the states from the first set (e.g., the GS and the low-lying excitations of the solid) are assumed to play a direct role in the associated dynamics and are relatively well-known; while states from the second set are assumed to play a secondary role and, as a consequence, are not required to be as well characterized. (In practice, in LENR theories, particular models, based on "plausible" assumptions, have been used to model the states associated with the second set.) The assumption that the states from the first set play a direct role means that a restricted form of interaction can be used to model the relevant dynamics, in which both the initial and final states are restricted to have components associated with this particular set of states. Formally, this constraint can be imposed by projecting both the initial and final states onto a subspace, defined by the first set of states. Thus, if \Qt) is one of the states in the first set, the average value of a particular operator O is assumed, by construction, to be the average of PQOPQ, where PQ is the projection operator, defined by Pq^lQiXQil-
(1)
i
Similarly, if \Pt) is one of the states in the second set, the associated projection operator Pp is defined by Pp^WiPil^l-PQ, i
(2)
650
where implicitly, in a formal sense, it is assumed that the many-body states are complete. In practice, because only a limited amount of information is known about the second set of states associated with Eq. (2), by construction, normalization and energy conservation are not imposed from the outset in particular regions of space, or as a function of time, but are determined dynamically (as in the renormalization procedure, used in quantum field theory). As a consequence, an effective, non-Hermitean, energy-dependent many-body Hamiltonian Hes can be constructed that describes the relevant dynamics associated with the propagation of states within the subspace defined by PQ. In fact, because the momentum/energy cut-off for states that belong in the first or second sets is not unique, the resulting decomposition is not unique. However, neither the loss of uniqueness, or the fact that the resulting Hamiltonian is not Hermitean or energy-independent detracts from its usefulness in assessing the potential importance of coherent effects (in particular) in solids, or, more generally, in the problem of estimating relevant physical quantities. In particular, i?-matrix theory can be used to identify key effects associated with the relevant dynamics in many problems in which a dominant form of interaction can be identified. Consistent with the associated picture, the formal generalization that is used in i?-matrix theory involves allowing the energy, associated with solutions of the manybody Schroedinger equation, to be complex (by allowing the wave function to grow or be dampened through dissipative processes that break time-reversal invariance). In .R-matrix theory, a particularly useful representation is constructed by requiring that the deviations from perfect time-reversal invariance be infinitesimally small. The construction is also useful because when causal relationships are imposed, it provides a way to derive an approximate Hamiltonian by "removing" the degrees of freedom of the true Schroedinger equation that are not involved in the associated process through an "inversion procedure." This is accomplished by constructing an effective inverse of the Schroedinger equation, which is used to eliminate the dependence of the equation on the variables (and the associated range of energies) that are not directly involved in the problem. This becomes possible when the energy is allowed to take on complex values. In particular, in the "inverted" form of the Schroedinger equation, the effects of the implicit perturbations from states that are not physically important (designated by \Pi) in Eq. (2)) on the remaining (physically important) states are inferred through a projection procedure. Formally, this is accomplished through a two step process, in which: (1) an effective inverse, G{Z) = 1/(Z — H), of the many-body Schroedinger equation (defined by if), associated with a complex value of the energy, Z, is constructed (or assumed), based on a knowledge of the relevant dynamics, initially, and (2) the fact that only a restricted set of states (the states associated with Eq. (1)) are important is used to justify eliminating the states that are not included in this set from the relevant dynamics. In particular, if G(Z) is an inverse of the Schroedinger equation, formally, it follows that G{Z){Z ~H) = 1 = (PQ + PP)G(Z)(PQ
+ PP)(Z - H)(PQ + PP).
(3)
651
But then because PQPP = 0, by construction, from Eq. (3), it also follows that Q PQG(z)PQ
PPVFP
PQ(Z - H)PQ - PQVFPP ( ^ 4 f f )
= 1,
(4)
where Vp = V — PQVPQ is the difference between the full, many-body potential (V") and the projection of V onto the subspace, defined by \Q), and PQ(Z — H)Pp = —PQVFPP is the negative of the projection of all of the matrix elements that couple the physically realizable states (\Q)) to the remaining (\P)) states. Equations (2) and (3) define an effective Hamiltonian Heg (through the inverse, Z — i?eff, of the projection of G(z) onto the initial and final states associated with the physically measurable states, \Q)): Z~HeS
= PQ(Z - H)PQ - PQVFPP
( ^ T f f ) PPVFPQ-
(5)
In particular, the effects of the outside perturbations associated with the excited states enter through the additional term, —PQVFPP(1/(Z — H))PPVFPQ. Equations (l)-(5) apply to arbitrary many-body configurations. In problems related to reaction, the relationship between V and the initial state potential V0 has to be specified. Provided the final state that results from some outside interaction and the initial state have the same total energy E, all deviations from the initial state involve states that are orthogonal to it. Then, if the initial state can be modeled, using the set of states \Q), the full potential projected onto this set of states must equal V0 = PQVPQ, and VF = V — VQ = AV is the change in potential that is responsible for the transition to the final state. Because PQPP = PPPQ = 0, PQVFPP = PQAVPP = PQAV(PP+PQ) = PQAV; and similarly, V¥ PQ = AVPQ. As a consequence, it follows from Eq. (4) that Z - HeS = PQ(Z - H)PQ - PQAV
( J ^ ) ^VPQ
= PQ(z-HQ-Av(^-1^AV^PQ,
(6)
where H0 = T + V0 is the initial state, unperturbed Hamiltonian, defined by the kinetic energy T and initial state potential V0. To be consistent with time-dependent perturbation theory, since E is real, Z can differ from E only through the addition of a small positive or negative imaginary component (i.e., Z = E±\8). As a consequence, it is possible to write two effective Hamiltonians, H^s and H~s, which, respectively, describe situations in which coupling through the perturbation AV (to the states associated with Pp) vanishes in the distant past, or future: Hf. = PQ {H. + AV (
E
_'
H ± l 5 )
) A ^ PQ.
(7)
Since it is assumed that the initial state is spanned by the set of states \Q), H^ can be understood to be the projection of the full Hamiltonian H onto a particular set of states, possessing specific boundary conditions and/or that is defined in a
652
particular (restricted) region of space. Because Z is a complex number, particle flux, state normalization and energy need not be conserved. Implicitly, through the second term (associated with G(Z)) in Eq. (7), HeS includes coupling with "forbidden" states (or "regions"), associated with overlap of the physical system with the sub-space defined by Pp, that is not included in the initial ("allowed") sub-space, defined by PQ. Consistent with conventions used in formal scattering theory and the Fermi Golden Rule, the imaginary part of the expectation value of the difference between the Hamiltonians, (Imag{ty\(H+s — H~s)\^)), denned by Eq. (7), is interpreted as defining an effective lifetime r and rate of interaction R = 1/r = l/h Imag(i?(^F — H~s) associated with overlap between the initial states (defined by P Q ) with the "forbidden" states (defined by Pp) which, by construction, have vanishing overlap with the initial states, in the absence of any perturbation. In particular, from Eq. (7), it follows that if ^ 0 is any many-body state that is initialized, in the absence of outside perturbations (so that PQ^0 = *o), the associated values of R and r are given by R=~
1
2TT
= — {M>0\AV6(E -
T
= j E ^ n
H)AV\^>0)
tl £
™ t(C F ))|(* 0 |Ay|vI/ exact (C F ))| 2 ,
(8)
F
where * exact ( C F ) is any many-body state, possessing a particular configuration (denoted by Cp) of particles that solves the Schroedinger equation of the exact Hamiltonian, H, and Eexact (Cp) is its energy. Three important points are: (1) Eq. (8), in principle, is exact, (2) as a consequence, it holds for arbitrary perturbations AV (and not merely when the AV is sufficiently small, which is the case, when the Fermi Golden Rule applies), and (3) it is virtually impossible to evaluate the RS of Eq. (8) without detailed knowledge either of \fexact ( C F ) and/or both \I>exact ( C F ) and AV. Nonetheless, it is possible to make considerable progress, using Eqs. (8)-(17), by making reasonable assumptions about the relevant physics, associated with the more refined LENR theories. In particular, it is possible to show directly from Eq. (8) (as discussed below) how forms of coherence associated with both BGS or phonons can lead to LENRs. In applying Eq. (8) to LENRs, two obvious effects have to be explained: (1) the lack of high-energy particles that are released in any of the final states, and (2) how to "overcome" the Coulomb barrier. But as opposed to situations in conventional nuclear physics where the initial state involves two particles that collide at a particular location, in a solid, the initial many-body state consists of many particles that potentially can interact with each other at many different locations. Similarly, as opposed to the conventional nuclear physics situation in which a small number of particles appear in the final state, in solids, many particles can interact with each other, instantly. For this reason, the idea of overcoming a Coulomb barrier at a particular location, in which a particle tunnels across a region where its kinetic energy becomes forbidden classically, can be replaced by a more general concept, in which many particles interact through one, two, or even many "forbidden" transitions
653
(associated, potentially, with many different possible configurations Cp) in which many particles can interact with each other at many locations. In the idealized limit in which many particles are allowed to respond coherently, e.g., through a particular transition, involving a particular, common characteristic frequency, v, the total energy associated with the response, in principle, can be as large as the product of hv with the total number (iVr) of particles. As a consequence, in the most efficient transitions, intuitively, one expects that characteristic rates R associated with coherent many-body processes, in principle, can become proportional to N?, which means that it can become possible to achieve the kinds of reaction rates (and lifetimes) associated with conventional nuclear reactions, even when the energies associated with the particular transition of an individual particle are quite small. For this reason, Schwinger,7 Hagelstein,6 and Chubb 1 invoked arguments associated either with Eq. (8), or (in Hagelstein's case) to an equivalent formulation, based on an alternative formalism (the Resonant Group Method), involving coupling to a coherent many-body state. Unfortunately, before his death, Schwinger did not complete his model. However, he made approximate calculations of R, by evaluating Eq. (8), directly, based on the assumption that all of the available energy from the nuclear reaction was released coherently by producing a large number of phonons, associated with a particular frequency. Also, as opposed to using wave functions associated with conventional tunneling at a particular location, he dealt with the overlap problem by assuming that the deuterons could be constrained by the lattice to occupy different locations within a common unit cell, where conceivably, they could have appreciable overlap. However, although he based his overlap argument on assumptions that appeared to involve a realistic geometry 9 (in which d's simultaneously occupy the tetrahedral and octahedral sites in a particular unit cell), subsequently, this geometry was shown to be in-appropriate. Also, in Schwinger's treatment, the associated coherence involved coupling through phonons, derived within the harmonic approximation, which, if applicable, only applies at low loading. Subsequently, Hagelstein developed a considerably more sophisticated treatment that also is based on the idea of coherent phonons. As opposed to assuming that in the complete many-body configuration (associated with ^reXact(CF)) the overlap occur between deuterons exclusively in different lattice site locations (which was assumed by Schwinger), or at the same site, Hagelstein considered both situations. He found by including coupling to a phonon spectrum that is dominated by a single, coherent phonon, through the associated "forbidden states," which result when the displacements associated with the phonons are included in the behavior of the deuteron-deuteron separation variable, that appreciable overlap between deuterons only takes place when the two deuterons occupy the same site. (Schwinger undoubtedly would have found a similar result had he not been misled by the incorrect geometry suggested by Sun and Tomanek. 9 ) In his treatment, Hagelstein6 explicitly includes the coordinate dependencies of all of the nucleons in the problem, as well as
654
an effective (Gamow-like) tunneling factor that impedes deuteron-deuteron overlap when two deuterons occupy the same site. He also finds that by applying second (and/or higher) order perturbation theory (which effectively can be inferred to all orders, using Eq. (8)), it is possible (through phonon exchange) to derive appreciable reaction rates, associated with "fast alpha" particle creation (i.e., where the alpha energies exceed lOMeV), by allowing for a pair of deuterons on one site to interact with a second pair, located on a different site, through phonon exchange. In order to obtain appreciable reaction rates for "slow alpha" production, he concludes it is necessary to include additional, nonlinear phonon coupling in the associated, site-other-site, deuteron pair interactions. He also points out a potentially important, implicit form of additional interaction could enhance the non-linear coupling: the fact that because phonons are bosons, effectively, a collection of coherent phonons could stimulate additional, coherent phonons (that possess the same frequency), through stimulated emission processes (analogous to the kinds of processes that are used in Lasers to produce coherent beams of light). Hagelstein speculates that amplification of phonon exchange from such processes could make it possible for many units of angular momentum to be transferred between the coherent phonons and pairs of deuterons through the associated coupling. In fact, as pointed out above and elsewhere,1 in the particular limit, near full-loading, in finite size crystals of PdD, the extreme long wavelength, acoustical phonons that result from small variations in deuterium loading, actually are deuteron IBSs. In a real solid, these variations in loading couple directly to the electric (and ionic) charge in the surface region. Thus, implicitly they provide longrange coupling that is required to be coherent (since deuterons are bosons, on length scales associated with electromagnetic interaction). Because in the limit of small additional loading, the associated "vibrations" lead to small fluctuations in deuteron charge in the immediate vicinity of deuterons (located in the octahedral sites) that have been loaded into the lattice, the associated IBSs, effectively, appear to be the phonons that couple most directly to deuterons in the lattice. But the associated IBSs involve coupling that leads to an effective, external electric field (resulting from build-up and depletion of charge in non-bulk regions). In the context of an idealized form of Eq. (8), involving an initial state consisting of the many-body state associated with the GS of an infinitely periodic, neutral, Harmonic crystal, the effects of coupling to a many-body state that includes IBSs occur through changes in the electrostatic zero of energy of each charged particle (which effectively alters the chemical potentials of the "conventional" phonons and electrons, associated with the periodic solid) and through non-linear (second and higher order) processes. As a consequence, although the coupling to IBSs occurs through variations in charge that "appear" to be acoustical phonons in finite PdD crystals, relative to the initial state associated with the infinite crystal, case, these variations "appear" to be optical phonons. Thus, in the context of Hagelstein's model, a case can be made
655
that the "coherent" phonons that he uses could be IBSs, in certain circumstances. On the other hand, at elevated temperatures, as a result of electron-IBS coupling, and electron-phonon coupling, again through Eq. (8), occupied and/or unoccupied IBSs will induce additional coherent and incoherent phonons, that also could play a role in his model. Regardless of whether or not Hagelstein's model applies, there are more direct forms of coherence, associated with BGS, 1 ' 1 0 and IBSs, that can lead to nuclear interactions, especially, either at lower temperatures, or in smaller (nano-scale) crystals (or both). In particular (as noted above) GMST, in its most general form, is equivalent to i?-matrix theory. To establish this, it is sufficient to: (1) identify \Q) with the ground state, VQS = PQVPQ, and, (2) for computing the time evolution of the overlap of $ G S with an arbitrary (excited state) \f', in the bulk region, formally, to require that V = PpVPp. Thus, it follows, that the difference in potential AV = — (V — V). Then, each matrix element in Eq. (8) can be expressed in terms of the overlap of 'J'QS and VP' with the divergence of the velocity flux v(r), used in Refs. 1 and 2: dt
/ill/ /
1>
"
"
at
= - J d3rV • (*>(r)|*GS> + (*'\VCSm ^ V G S ) = 0, where (*>(r)|* GS > = E / / / 3
d 3 r
i • • -d3rn63(r -
r,)^J
X ( — [*' * V r . * G S " V r , * ' * *GS] - 7 * ' * ^efffo^GS J , and Aeff(r) = (A(r) +A'(r))/2 is the arithmetic mean between the vector potential A'(r) associated with the state \P' and the comparable vector potential A(r), associated with the state * G S - The GMST follows from the observation that Eq. (9) applies, in general terms, for any two states that have the same total energy, globally, but different potential energies. The problem of applying GMST, in its complete form (as in Eq. (9)), is formidable because, in principle, it provides a solution to the general many-body problem. In the limit in which particular symmetries are present, however, GMST can be extremely useful. In particular, as the author has noted previously, 8 ' 11 in order to have minimal overlap with outside processes, in particular regions of space, the flux contributions from J d 3 r V • (*'|i'(r)|vD,Gs) from these regions are required to vanish. Because of this fact, implicit forms of symmetry can evolve that preserve the overlap (or lack of overlap) between many-body configurations. In situations involving finite solids, with real boundaries, an important source of symmetry results from a form of Galilean relativity that exists because of approximate invariance (of the bulk region) with respect to rigid, Galilean transformations.
(9)
656
In the absence of interaction with surface regions and lattice imperfections, the associated symmetry makes it impossible to distinguish the GS from other states that can be derived from the GS by simply shifting the zero of momentum of the solid because such a shift can be accounted for through a trivial gauge transformation (in which a constant is added to Aes(r)). The BGS in finite crystals occurs because charge accumulates in surface/interface regions. In the case of LENRs, BGS can also occur in regions where overlap between charged particles can take place. Appreciable overlap can also take place through BGS, between charged particles in solids, because K/2i\%>' * V r ^ c s - V^.*' * * G s ] and ej / c^' * Aes(rj)ipGS) locally can change suddenly, without the velocity v(r), ever becoming large. Potentially, the most relevant nuclear-scale processes (that occur in situations involving BGS) are initiated when the bulk region, effectively remains in its GS, and momentum is transferred coherently, through rigid translations (associated with UmKlapp processes) that preserve periodic order from locations where overlap between nuclei can take place (and the associated ionic charge from IBSs can accumulate) to regions outside the bulk region. Within this context, initially the "forbidden" regions are the non-bulk regions. Through subsequent transfer of momentum to these regions, heating is triggered. As a consequence, nuclear products (heat and new elements) are expected to appear outside the bulk. In order to describe how these processes couple to IBSs, in situations involving BGS, it is necessary to relate the individual coordinates ( r i , . . . , rjvT) of the various particles in the many-body wave function to the coordinate Rcm associated with the center-of-mass, the separation variables r ^ that describe the difference in the position of each particle from the remaining particles, and the total mass M of the collection of particles. In particular, by definition: _
_
_ _
R
_ JL,i=l,NT
m
iri
nn
s
and, from Eq. (10), it follows that n=
J2
T
W+R™>
r3=rx-r^
j £ 1.
(11)
j=2,7V T
The summation in Eq. (11), in principle, should be carried out over all particles in the many-body system. In fact, the only contributions that are relevant in any reaction occur from particles that have non-vanishing flux, at the boundaries of the bulk region.1 Also, because at the immediate location of a potential nuclear reaction, a change in charge can take place that can alter the charge and raise the energy of the system, technically, the associated location is not part of the GS, bulk system (since a net flux of charge can occur, as a result of the reaction), even when the associated redistribution occurs in a nuclear-scale size volume, surrounding the reaction, where the potential is altered. In any case, potential nuclear reactions can occur whenever the coordinate r^ associated with the center of mass of a single deuteron (d) in the many-body wave function, that possesses a wave-like, IBS form
657
(in the bulk), has overlap either with a second d or with some other nucleus, that possesses a coordinate Tj. This overlap can only occur at locations where r ^ can become sufficiently small that the strong force becomes appreciable (which occurs in the idealized limit in which, on the scale of electromagnetic interaction, r ^ —> 0). The lowest energy forms of LENR, within the context of BGS, involve situations in which the reaction is triggered by potential overlap between an initial state involving p's, t's, or d's in IBS form. In the vicinity of a location where this can occur, as a result of Coulomb repulsion, the potential energy is required to change rapidly. As a consequence, a surface integral contribution occurs in Eq. (9), at each location where r y —> 0, as a result of the flux of particles (and charge) that is introduced as a result of the change in potential at the location of a nuclear reaction. In particular, as in Ref. 1 it follows that we may write: *'\V~V'\*)
= / d 3 r V •(*>(?•) | * ) =
fd2Sh»(^'\v(r)\^) bulk boundary
V [[[d^-Vr dV 2^ HI
r
2 d Sd I[d ^nd.
l
[*' * V r j .* - V r . * ' * $] - ^ - # ' * A e ff(rj)* J • (12) Here (in the first line), we have assumed that V — V vanishes in the bulk region, and we have used Greens theorem to convert the divergence of the velocity (which, in principle, includes all particles that leave or enter the bulk) into a surface integral that extends over the boundary of the bulk (which we have represented through the label beneath the final integral, in the first line, and through the two dimensional integration symbol that appears in the same integral). In the second line of this integral, we have divided this final integral into domains, which we have denoted, using the symbol dj, and through the label S ^ , which refers to the area of the associated domain. In particular, each of these domains is associated with an effective boundary of a location (defined by r^ —> 0) where a nuclear reaction can occur, or to the external boundary of the bulk region, which occurs at the boundary of the region where, on the average, a net accumulation of charge begins to take place in each unit cell. Also, in this integral, the multi-dimensional integral (JXfd3(JVT~1V) extends over the remaining coordinates. It follows from Eqs. (10) and (12) that energy and momentum can be transferred directly from nuclear reactions, in the interior (non-bulk) regions to locations outside the solid. Provided the final and initial state (nuclear) portions of the wave function involve (different) stable, ground state configurations (e.g., when the initial and final states are ground states of different nuclei), when the number (TV) of locations where potential reactions take place is sufficiently large, it is possible to derive an effective velocity flux (through an expansion of the bulk wave function, in terms of the shift in the zero of energy), across the (nuclear region) boundaries in Eq. (12), based on the semi-classical equations of motion. 1
658
In the most coherent situation, no excitation of any state, whatsoever, in the bulk region can take place; while outside the bulk region, momentum can be transferred from the solid as a whole into surface/interface regions (through center-of-mass motion and excitation and the resulting ion-electron interaction), or into the bulk region, from nuclear reactions, in the interior. But since
at locations where rij —> 0, in the surface/interface region effective discontinuities in Vr3- ^ and V r . Vl/'* (wave function cusps) can occur (associated with sudden changes in potential), either through ion-ion or electron-ion overlap. In Eq. (12), these effects can be treated by enclosing each location associated with a cusp with a volume of size VMT- In principle, size VMT can be a small, enclosing sphere, surrounding the singularity, which (in analogy with the situation in multiple-scattering theory) we will refer to as a muffin tin (or MT). Globally, we could pick each MT to be a sphere of nuclear dimension. On the other hand, in the surface and interface regions, where significant electron-ion interaction takes place, d's and/or 4 He nuclei become partially neutralized. In this limit, the lifetime of each d-reactant and/or 4 He-product nucleus in a particular IBS can be reduced dramatically. As a consequence, a more useful representation of the associated perturbation, in analogy with situations in which electrons become important, involves allowing for the possibility that the (residual) singularity (if it exists at all) be allowed to extend over a larger domain (which asymptotically can approach an atomic scale characteristic size). In the associated interaction, coupling to final state many-body states can occur in which 4 He either appears in a localized (ionic or partially ionic) form at MT locations, or delocalized, in a surface IBS form. The most coherent effects occur when a large number of states, in the bulk, that are related to each other, through rigid, Galilean transformations, become approximately degenerate. Previously,1 by requiring that the overlap between states near the GS, with each other, and with the GS, be stable with respect to variations in the zeroes of energy and momentum, the author generalized a number of results associated with conventional energy band theory, as it relates to charged particles in infinitely repeating ordered solids to finite size solids, with real boundaries. By requiring that the net force on the bulk region vanish and that the potential and density decay (in surface regions) sufficiently slowly, the author was able to generalize the semiclassical equations of energy band theory (for infinite lattices) to situations involving finite-size lattices. Essentially, the associated construction (which is a form of BGS) is equivalent to identifying the preferential gauge that minimizes coupling between low-lying states (associated with different wave-vectors) in the bulk with each other and with the GS. In general, because the basis of the BGS is the idea that all of the particles in the bulk can "move" rigidly, in response to some symmetry-breaking perturbation, the associated effect involves a form of coherence in momentum that can be large at particular locations but be distributed, instantly, to many locations.
659
For this reason, through BGS, for example, the velocity operator (in Eq. (9)), which can become discontinuous, can change suddenly, but without high-energy particles ever being emitted. This kind of effect is guaranteed to be possible in LENRs provided the target nucleus either occupies or could occupy an IBS in bulk regions (which requires that it be a proton [p], a triton [t], or a d ) . Alternatively, potential LENRs could be initiated outside the bulk, with an alternative target nucleus, through some alternative effect involving accumulation of charge (e.g., in surface regions), triggered by the bulk, through an Umklapp process. (This kind of reaction could also trigger "fast alpha" production, as well as some of the other phenomena, suggested by Hagelstein.) For illustrative purposes, however, in describing the most coherent form of LENR, we will focus exclusively on the d + d —> 4 He reaction. 3. Triggering Time and Coherence Through Zener-Ionic Breakdown The BGS occurs when, as a result of a continuous symmetry, many energy states, resulting from many energy configurations, become approximately degenerate. In the case of d's in PdD, the greatest degeneracy occurs in an extreme limit in which, effectively, initially, all of the d's have the same energy, for all values of the momentum. In PdDj;, in finite regions, where x —> 1, the presence of an electric field E can induce long-range fluctuations (in x) that induce variations in Emd that cause the degeneracy to be lifted. The resulting form of coupling is strongest when the contribution to the (ionic) current from two d's that occupy IBSs becomes vanishingly small. The associated interaction (which, in its strongest form, can mimic the phenomena of Bloch Oscillations in insulators) can trigger d + d —» 4 He reactions, with minimal coupling to the bulk (and with no high-energy particles), provided the crystal size is sufficiently large, and the initial state d's interact with each other and with the applied .E-field for a sufficiently long period of time. The initiation of d + d —> 4 He LENRs, through the most coherent processes, occurs in a limit that involves the transfer of small amounts of charge from (cusp) regions throughout the interior (where it is highly polarized), to surface/interface regions through a process that initially, effectively, excites d's in lowest energy band (which is effectively dispersionless) to a higher-energy band. The underlying physical effect is analogous to a phenomenon (Zener-electric breakdown 8 in insulators) that was first postulated by Zener (based on an idea by Bloch) that could lead to conduction in insulators. In particular, Bloch suggested that the semi-classical equations describe how the energy and momentum of "quasi-particles" (electrons) change, as a function of time. He observed that in the limit of a one-dimensional periodic lattice, in the absence of collisions, a particular phenomenon (referred to as a Bloch oscillation) might take place. In particular, when the lattice is one-dimensional, it can be represented in terms of integral multiples of a single primitive vector (the lattice spacing o). Then, if the precise wave function associated with the conduction electrons could be written in terms of a superposition of band state energy wave functions, in the long wave-length limit (where the semi-classical equations apply),
660
in the absence of magnetic fields, the associated charge would appear to oscillate (as a function of wave-vector and time) between the boundaries of the first Brillouin zone, with a period r of oscillation defined by the applied electric field E, through the relationship,
eEr =
. a
Zener pointed out 8 that because E can become quite large in insulators and/or semi-conductors, the idealized (semi-classical) limit, associated with a single band, can breakdown, implicitly, through excitations that lead to inter-band transitions. Instead, he pointed out that implicitly these forms of excitations could be treated by allowing for the possibility that the associated charge could tunnel into different (higher energy) bands, where alternative forms of transport (including those associated with the semi-classical theory) could apply. In general, an externally applied i?-field alters the zero of momentum of the bulk region, as a result of polarizing the charged particles in non-bulk regions. The associated polarization is strongest in the surface/interface regions and occurs as a result of accumulation of charge. Typically, in transition metals, screening occurs very rapidly (within 5-10 layers from a surface or interface). Thus, for example, in most situations, an applied voltage of 1V across the entire solid induces an £-field that varies between 0.2 and 0.1 V/A, in the immediate vicinity of surfaces/interfaces. On the other hand, because, in order to sustain high loading, it is always necessary to apply an external field, small fluctuations of charge, associated with deviations from perfect stoichiometry, involve non-local coupling that extends over many unit cells. Relative to the perfectly stoichiometric PdD compound, these fluctuations can be represented (e.g., using i?-matrix theory) through an external perturbation AV that alters the vector potential (and zero of momentum), in the regions (associated with cusps) where d-d overlap can occur. The most coherent forms of reaction occur in the limit in which the current becomes vanishingly small. In particular, in order for the bulk region to remain in its GS, the possible energy (or momentum) release, throughout the bulk region must be less than the characteristic energy or momentum release associated with processes that would excite conventional (optical) phonons (associated with the bulk, in the idealized limit of an infinite PdD lattice). In particular, because the smallest (zero-point) energies associated with optical phonons in PdD are typically < ~ 0.01 eV, this requirement can be used to identify a useful bound for the (dominant) contribution associated with the interior (cusp regions) from the timedependent terms that result from the change in electric field AE = E—E-m^, through the associated induced perturbation to the Hamiltonian (through the change in the vector potential AA = —AEct). In particular, when the associated change in
661
energy/ n o n _ b u l k d 3 £ AEt(^'\J(x)\lti>Gs)
< ~ 0.01 eV, an appropriate bound for J is
[ d*x < * | j ( a ; ) | t f G S ) < ~ ° ^ X . non—bulk
'
(14)
'
On the other hand, because the bulk region is required to remain in its ground state, the shift in the zero of momentum is equivalent to a rigid, Galilean transformation, in which beginning from a state, associated with vanishing IBS current (which occurs when all d's occupy the lowest energy k = 0, IBS), the momenta of all d's that have overlap in the interior cusp regions, are shifted coherently by an amount eAEt. But this is only allowed provided the resulting wave-vector k(t) = AEt/h of the single IBS (associated with all d's in the cusp region) remains in the First Brillouin zone, defined either by the entire bulk region, or by a (Bravais) sub-lattice of the bulk. With increasing time, for a fixed value of AE, in principle, the bulk region can still remain approximately in its GS (in the absence of nuclear reactions), even when k (t) does not remain in the first Brillouin zone. Specifically, a particular discrete set of values of the time t = t(i) exists that define situations where the shift in the wave-vector zero, et{i )AE, identically equals a reciprocal lattice vector. (The vector symbol iis used as a short-hand for the three numbers, ii,Z2, and is {i = (ii, «25 23)} that a r e used to construct the reciprocal lattice.) The possible values of t(i)can be constructed from discrete units of time, Ata (a = 1 and 3), using the primitive vectors bj (j = 1,3) that define the Bravais lattice 12 : t = t(i)=t(ia)
= iaAta,
a = 1,2,3,
Ata = ^r^-—-. eba • AE
(15)
At each of the values of t, in Eq. (15), a resonant, Umklapp process can occur in which, the bulk, or a sub-lattice of the bulk can effectively undergo a rigid, Galilean translation. It also follows that in the most coherent situation, where the shift in zero is coherently added to each d, since the total shift is
*W)) = ^ M ,
(16)
and an Umklapp process also occurs at additional times, defined by t = t ( £ ) = iaA*a f
(17)
At alternative times (where t can never be represented, using Eqs. (15)-(17)) especially in smaller lattices, the associated shifts in momentum zero alter the distributions of charge in the non-bulk regions, which, in turn, alter the value of AE. Provided N is sufficiently small, the associated phenomena can be viewed, effectively, as elastic d-d scattering processes, in which momentum associated with d-d collisions (in cusp regions) in the interior is transferred to the surface/interface regions, without altering the bulk. As N becomes sufficiently large that the total shift
662
in zero of momentum becomes comparable to the amount that would normally be associated with the gamma ray that is released in the conventional d + d —> 4 He + 7 reaction, new forms of collisions can take place (in cusp regions), involving a final state in which a net flux of 4 He is transferred through an IBS current in the interior cusp region, and either through contributions from the terms that involve currents (and vector potentials) or through the dipoles (and E fields), to MT volume cusp regions in the vicinity of the surface and/or interface. Key effects that play a role in triggering are associated with the relevant timescales, and the flux of (positive and negative) charges in the surface/interface region. The initiation of d + d —• 4 He LENRs, through the most coherent processes, which occurs in the limit of small current and long time, involves small amounts of charge that are initially highly polarized (in cusp regions) throughout the interior, followed by a small transfer of charge through a process that initially, effectively, excites d's in a particular band to a higher band. Thus, the triggering process, in the most coherent regime, is analogous to the transition between an insulating and conducting state that is driven by increasing periodic order, as a function of time. An important distinction between this transition and Zener-elcctronic breakdown, however, is that in the situation in fully loaded PdD, the transition involves ions (as opposed to electrons). For this reason, as opposed to Zener-electric breakdown, a more appropriate name for the phenomenon might be Zener-ionic breakdown. In Ref. 1, the author estimated a minimal crystal size (of ^3000 unit cells), associated with the onset of the most coherent process. The characteristic dimension of the associated crystal is ~6 nm. The author based this estimate on the fact that in the absence of any accumulation of charge in the cusp regions, asymptotically, it is possible to equate the change in momentum (defined implicitly by eNAEt(i)/h in Eq. (16)) by the total momentum that the bulk would have in a reference frame that moves with the common velocity that cusp and bulk regions would have in the limit in which all regions move rigidly. Because this estimate fails to include the asymmetry associated with the applied fields, it has no time-scale associated with it, or preferential orientation. Crystal size, orientation (with respect to the fields) and lattice imperfections all are important in triggering the process. In the idealization of a perfect bulk region, surrounded by a uniform surface region, the lowest energy configurations minimize stress and strain along the surface/bulk boundary. This suggests that in such an environment, the induced electric field (from Coulombic repulsion/nuclear reaction in interior, cusp regions) will be oriented in opposition to the applied field. But detailed calculations, based on a microscopic model of the nuclear physics and atomic/ionic/electronic structure, would be required to understand the magnitude and orientation of the induced response. Historically, it has been observed that the time required to trigger d -\ > 4 He varies between several weeks, to several hours, or (e.g., in laser-triggering experiments 13 ) to several minutes. Zener-ionic breakdown provides a potential mechanism for understanding how such a wide variability in triggering time t can occur. In particular, using Eqs. (15)-(17), it is possible to relate crystal size to information about the
663
values of t, and the magnitude of AE. Equation (14) can be used to relate AEt to the magnitude of IBS current. Consistent with the associated picture is the idea that although the nuclear reaction would occur over some nano-scale size region of the lattice, in order to preserve periodic order, charge neutralization in the MT volumes, associated with cusp regions outside the bulk, would extend considerably further beyond the boundary of the nano-scale region, through an effective damping of the associated induced dipoles. Within this context, it is reasonable to assume that the induced charge polarization would involve effective values of AE that are also consistent with values of ttrig ~ 10-10 4 . For illustrative purposes, consider a situation in which the induced potential difference (during the triggering process) is ~ 1 V and that it extends over a cubic structure, possessing a characteristic dimension of 1 cm. In a situation in which the polarization in charge is approximately the same everywhere in the non-bulk, surface and interface region (which includes all of the cubic structure, except for the nano-scale bulk region where the transfer of momentum occurs from the nuclear processs), nuclear reaction effectively induces a value of AE w 10 _ 8 V/A = 1 V/cm. When Afvert = 1.5 x 10 (as in the bound, involving 6nm characteristic crystal dimension, identified in Ref. 1), using Eq. (15) [as in the derivation of Eq. (63)] it follows that At\ii
= Ai2«2 =
^zr- = ttrig = 3.03/xs; a\eAE\
while if A^ert = 1.5 x 100,000 (involving 60nm), i t r i g ~ 840 h. In the first example (-/Vvert = 1.5 X 1 0 , t t r i g ~ 3
fis),
0-01 eV
de_ dk
<~
\eAE\ttrig
„ „„ 12 x , = 3.30 x 1012 A/s,
which is roughly an order of magnitude larger than the characteristic group speed associated with IBS's that have appreciable dispersion (and charge transport). In the second example, (Nvert = 1.5 x 100,000, £trig ~ 840h), the associated value of 9e
< ~ 0.330 A/s dk is more than 12 orders of magnitude smaller than the characteristic value, associated with a lattice that has appreciable IBS current. The transition between IBS currentconducting to IBS-insulating crystalline structures occurs when de_ dk
< ~ 3 . 3 0 x 10 9 A/s.
This applies when the crystal has a characteristic dimension of ~60 nm. Acknowledgment I would like to thank Talbot Chubb, David Nagel, and Mitchell Swartz for providing valuable suggestions about the material in this paper.
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References 1. S.R. Chubb, in Proceedings of the ICCF10 (in press), http://www.lenrcanr.org/acrobat/ChubbSRnutsandbol.pdf. 2. S.R. Chubb, Trans. Am. Nuc. Soc. 88, 618 (2003). 3. S.R. Chubb and T.A. Chubb, in Proceedings of the ICCF8, 385 (2000). http://www.lenr-canr.org/acrobat/ChubbSRtheoretica.pdf. 4. T.A. Chubb and S.R. Chubb, Fusion Technol. 17, 710 (1990); S.R. Chubb and T.A. Chubb, in Proceedings of the AIP Conference 228 (Provo, UT, USA, 1991), p. 691. 5. P.G. Burke and K.A. Berrington, Atomic and Molecular Processes: An R-matrix Approach (IOP Publishing, Bristol, 1993). 6. P. Hagelstein, Unified phonon-coupled SU(N) models for anomalies in metal deuterides, in Proceedings of the ICCF10 (in press). http://www.lenr-canr.org/acrobat/Hagelsteinunifiedpho.pdf. 7. J. Schwinger, in Proceedings of the First Annual Conference on Cold Fusion, 1990, pp. 130-136. 8. C. Zener, Proc. R. Soc. A 145, 523 (1934). 9. Z. Sum and D. Tomanek, Phys. Rev. Lett. 63, 59 (1989). 10. S.R. Chubb and T.A. Chubb, in Proceedings of the ICCF9, 2002, pp. 57-62; http://www.lenr-canr.org/acrobat/ChubbSRrelationsh.pdf; P.W. Anderson, Basic Notions of Condensed Matter Physics, Chapter 1 (Benjamin-Cummings Publ. Co., Menlo Park, CA, USA, 1984), pp. 8-69. 11. S.R. Chubb, Impact of boundary effects involving broken gauge symmetry on LENRs, in Proceedings of the ICCF10 (in press). Also, http://www.lenrcanr.org/acrobat/ChubbSRimpactofbo 12. N.W. Ashcroft and N.D. Mermin, Solid State Physics (Saunders College Publishing, Orlando, FL, USA, 1976), pp. 64-82. 13. D.G. Cravens and D.J. Letts, in Proceedings of the ICCF10 (in press); also, http://www.lenr-canr.org/acrobat/CravensDpracticalt.pdf; D.J. Letts and D.G. Cravens, in Proceedings of the ICCF10 (in press); also, http://www.lenrcanr.org/acrobat/LettsDlaserstimu.pdf.
I. BLOCH IONS
TALBOT A. CHUBB Greenwich Corp., 5023 N. 38th St., Arlington, VA 22207, USA E-mail: [email protected] A Bloch ion has periodic symmetry and is distributed in space in a lattice array form. Its spatial density distribution is neutralized within each unit cell by a metal's electrons. The wave function repeats coherently modulo a Bravais lattice vector. Paired Bloch deuterons partitioned over a sufficiently large number of unit cells become superposed and coherently mixed by coordinate exchange. A Hamiltonian describing paired deuterons 2-Dg l o c h is presented, and its nuclear self-interaction and coupling with the lattice are described.
1. Introduction This paper is the first of a group of three papers that argues the view that LENR processes share a common physics. Conclusions are summarized at the end of Paper III. Wave function coherence plus a partitioning of nuclear charge appear to be a requirement for LENR, including Fleischmann and Pons (F-P) cold fusion. Bloch ion wave functions1 have the required characteristics. The Dg loch ion is compared with the D2 molecule in Fig. 1. The deuterons in the molecule have coordinateexchange symmetry 2 and share a common potential well provided by spin-paired electrons. Drawings compare a D2 molecule trapped in a harmonic well with a 2-Dg loch wave function trapped in multiple potential wells furnished by a metal lattice. The center of the D 2 molecule is distributed as a Gaussian within the harmonic well (not shown). The molecule's double-peaked structure exists in "separation space." It is pictured in Fig. la, and is the site of vibration,rotation excitations. The lattice-conforming structure of the 2-Dg loch wave function exists in "center-of-mass" space, i.e., lattice space and closely resembles that of the Bloch-state electrons in a metal. Both are characterized by phase-coherent partitioning of charge density over multiple potential wells. Their wave function phases are ordered with respect to position, and can only change in concert. The partitioned coherence of Bloch electrons gives the metal its high conductivity. Both types of Bloch particles are described by periodic symmetry that occurs in response to the periodic order of a hosting metal atom lattice. The 2-Dg loch wave function also exists in "separation space." In "separation space" it has important resemblance to the spin-paired 2-electron orbital that neutralizes the He nucleus in the atom ground state. Both paired particles are subject to coordinate exchange symmetry, but differ in that the 2-Djjjj h has a local maximum in each of multiple potential wells, whereas the He atom's spin-paired 665
666
2-electron density has a single maximum in a single potential well. Both are expressed by 2-particle wave functions describing anti-correlated superposed charged particles, instead of side-by-side charged particles kept separate by a Coulomb barrier.
•Like a dimpled metal sheet
(a)
H
Figure 1. (a) Density distribution of D2 molecule in separation space {ri2}. If D2 molecule is bound inside harmonic-well potential cavity, its ground state spatial distribution in physical space {r} is a Gaussian (not shown). The double peak structure shown in (a) exists in {ri2} and is subject to vibration,rotation excitations, (b) Density distribution of D]t. . in physical space {r}. The D g l o c h ion charge is dressed by electron charge contributed by the lattice. The dressing process creates iVwen potential wells. For ATwen > Nweut criticali the 2-Dg l o c h ion charge distribution is the same as that of the single-deuteron D g l o c h charge, since the two deuterons in 2-Dg ] o c h are superposed, and not side-by-side.
2.
Quantum Delocalized Surface States
Three papers concerned with atom surface science provide a background for cold fusion theory: Puska et al.3 titled "Quantum Motion of Chemisorbed Hydrogen on Ni Surfaces," Puska and Nieminen4 titled "Hydrogen Chemisorbed on Nickel Surfaces: A Wave-Mechanical Treatment of Proton Motion," and Astaldi et al.5 titled "Vibrational Spectra of Atomic H and D on Cu(l 10): Evidence for H Quantum Derealization." These papers show that hydrogen nuclei can be prepared in a coherently partitioned form on a metal surface. Such a coherently partitioned nucleus is dressed by metal surface electrons so as to form a neutralized species conforming to a template provided by the underlying metal. The nucleus sees itself as the positively charged part of a coherently partitioned surface atom, coherent in that it has an ordered wave-function phase. These coherently partitioned nuclei were prepared by scattering low energy electrons off ordinary chemisorbed ground state atoms. The partitioned nuclei were formed as excited surface states with 2-dimensional
667
¥(r)
*12)
Figure 2. The 2-Dg| c h wave function is a six degree-of-freedom wave function, which can be written as \P(r,ri2) = V , ( r )ff( r l2) when the interaction between the dressed lattice potential U(r) in physical space {r} and the form of the density distribution in separation space{ri2} can be neglected. In accord with double Bloch symmetry, both i/>(r) a n c ' fl(ri2) are independent Bloch functions, describing a distribution modulo a Bravais lattice vector. \if>(r)\2 is a physical density distribution. |g(ri2)| 2 describes a normalized amplitude modulation function which decreases the amplitude of the 2-body wave function at ri2 = 0 modulo a Bravais lattice vector. |g(ri2)| 2 expresses dd anti-correlation. There is no Coulomb barrier. This superposed-deuteron functional form minimizes system energy when Nweu > iVwe]j critical-
periodic symmetry, and had band-broadened energy levels, i.e., they occupied an ion band state. In contrast, the calculated energy levels for the as-adsorbed ground-state chemisorbed atoms were sharply defined (zero band width), except for H on Ni(l 11), where calculation described a narrow energy band with width - 0.004 eV. 4
3. Phase-Coherent Partitioning and Double Bloch Symmetry Since it is now known that protons and deuterons can be prepared in the form of coherently partitioned surface states, it seems reasonable to consider whether partitioned deuterons might be responsible for cold fusion. A similar configuration would be deuterons in a coherently partitioned interface state, such as might exist within a water-metal interface. It seems reasonable to ask whether some of the chemisorbed deuterium "atoms" at the interface between a polarizable electrolyte-like water and
668
a transition metal like Ni or Pd might exist in a coherently partitioned deuteron form. It would seem that the dressing (electron screening) of such deuterons would be more complete when the non-metal side of an ion's surface charge distribution makes contact with a high dielectric constant medium-like water, as opposed to vacuum. It may be that under some conditions the interface ground state has the partitioned configuration. However, the main question to be answered is: does a pairing of spin-paired coherently partitioned deuterons (deuteron d = D+ ion) result in a lower mutual Coulomb repulsion force between dd partners than would exist for the same pair in a non-partitioned state? Based on a system energy minimization study, 6 this is a distinct possibility, provided that the number of coherent pieces Nweu exceeds a critical number called ATweu, critical- (-^weii is the number of potential wells provided by the lattice. A 3-dimensional fee crystallite having iVceii unit cells has A^wen = Nce\y octahedral sites and JVweii = 2iVcen tetrahedral sites.) The applicability of the energy-minimizing calculation depends on which of two quantum mechanics protocols for constructing a center-of-mass,separation 2-particle wave function applies when one models a coherently partitioned pair subject to coordinate exchange symmetry. The idealized wave function for a coherently partitioned surface particle on a periodic lattice is a Bloch wave, which describes a density distribution within a unit cell, modulo a Bravais lattice vector. There is an ambiguity as to what the proper protocol is for combining two independent Bloch functions in configuration space into a 2-particle wave function in center-of-mass,separation space. If independent Bravais lattice vectors are used in the protocol (as opposed to using the same lattice vector for both ions) the 2-particle repulsion potential decreases with the number of partitions, as designated by iVweii- The resulting symmetry is called "double Bloch symmetry." 4. Double Bloch Symmetry The 2-Dg loch double ion, like the D2 molecule trapped in a harmonic well, has six degrees of freedom. It is best expressed in "center-of-mass,separation" coordinates {r, T12}, where the r dependency describes a density distribution in the lattice and the ri2 dependency describes an internal structure, as shown in Fig. 2. The distinguishability of the two Dg loch deuterons prior to coordinate exchange is formally expressed by starting with independent Bloch functions in configuration coordinates {ri,r2}. If independent Bravais lattice vectors apply, the coordinate transformation to {r, 1-12} results in a double Bloch symmetry, in which both r and ri2 dependencies are independent Bloch functions. At sufficiently large iVweii, the r i2 dependency expresses superposed single-particle wave functions with an anticorrelation behavior, in which the 2-particle wave function has reduced magnitude near n 2 = 0 modulo Ri2y, where Ri2y is a lattice vector in ri2 space. Nwe\\ is the number of potential wells within which each ion is divided, as shown in Fig. 3. As iVwen increases, the degree of anti-correlation, described by cusps, decreases while wave function overlap increases. In the limit of large ATweii, the cusp amplitude —> 0,
669
and there is no anti-correlation. With decreasing iVwen, the amplitude of the cusps increases, as shown in Fig. 3. At Nweu = iVweii, critical, the cusps reduce the wave function amplitude to zero at iVwen points, and double Bloch symmetry no longer applies. The wave function reverts to side-by-side molecule form. However, for all iVwen > Nwent critical spin-zero paired-deuterons with symmetric coordinate exchange symmetry (+ parity) have no Coulomb barrier to a coalescence type of fusion.6
5. Bloch Sensitive Nucleus and Bloch Ion Fusion In accord with double Bloch symmetry, this paper assumes that there is a reduction in the Coulomb potential between a pair of coherently partitioned ions proportional to l/JVWeii. At large JVweii this reduction is sufficient to allow: nucleus-nucleus contact, coordinate exchange symmetry, 2 and nuclear reaction. Coherent partitioning reduces the e 2 /ri2 work required to bring two deuterons into nucleus-nucleus contact. Contact allows nuclear reaction. The immediate nuclear product is a nucleus whose ground state energy decreases with increasing partitioning. Such a nucleus is called a Bloch-sensitive nucleus. Bloch sensitivity couples the nucleus ground state energy level to the occupied area on the lattice surface, as measured by Nwe\\. Fluctuations in occupied area perturb the lattice, do work, and transfer energy from the product nucleus to the metal lattice. They also cause the Bloch-sensitive nucleus to become mobile, expand, and migrate so as to minimize total system energy by becoming partitioned into a maximally large effective number of potential wells, as described in Paper II. Interestingly, this behavior is needed to explain Iwamura's observations of 2-a-addition transmutations involving protruding surface atoms. Also, there is a second cold-fusion related process demanding explanation. Electrolysisassociated MeV particle showers originating in some sort of source suspended in electrolysis off-gases have been repeatedly observed by Oriani using CR-39 particle detectors. Coherently partitioned nuclei provide the essential starting point for understanding these showers, as described in Paper III.
6. Stationary-State Bloch Ion Hamiltonian A first approximation to the stationary-state Hamiltonian Hi describing a spinzero positive-parity 2-deuteron model of the F - P cold fusion process describes the coordinate-exchanged dd pair as a six degrees of freedom double ion in which the dependency on lattice space (physical space) {r} is separable from the dependency on internal space (separation space) { r ^ } . This Hamiltonian includes no explicit coupling between the nuclear configuration and the hosting metal lattice. The
670
Afcell = w cell, critical
Afcell = 3Afceii, critical
A/cell = 10Afcell, critical
Figure 3. Anti-correlation wave function
dressed double-deuteron is treated as a subsystem of the hosting crystallite. f fi2 H i ( r , n 2 ) =* | - ^ V " + (2e)f/iattice(r,iVweli;
{"^
fi2
Afwe
"
V?a+
e2
1
S^K^R^I^'-' '
coherent volume
(1)
/
Here the first bracket is the Schrodinger Hamiltonian for a mass-4, charge-2 ion in the external potential field of a metal lattice. The coordinate-exchanged doubledeuteron is treated as a single particle of mass = 2ma- ^lattice(ri -Wweii) describes a dressed lattice potential in which the double-deuteron is embedded. In this paper, the lattice potential is assumed to be periodic over an interface layer volume one layer thick covering an array area containing iVwen potential wells. Dressing is an implicit coupling between the 2-ion system and the lattice, since there are no potential wells unless the lattice electron charge redistributes itself so as to lower the
671
2-D
Bloch
Coalescence to nuclear dimension
2-D
12-
Bloch
">
4Hl
2+ 'dd Bloch
'12 Figure 4. When cold fusion occurs, the cusp function transitions from a normalized anticorrelation function that preserves the dd spatial separation spread-width at a value matching potential well diameter, modulo a Bravais lattice vector, into a form where separation spread-width equals a nucleus diameter, modulo a Bravais lattice vector. The shrinkage is called coalescence. During energy transfer, the 2-deuteron system can be in a mixed quantum state in which the fraction of time spent in the coalesced form increases until it becomes the metastable final state 4 „2+ FnTe P A subsequent mixed quantum state transition involving fluctuations in Nwe\\ changes d d Bloch 4 nH e„ 2 + into 4 H e R , , , which is the partitioned alpha particle form. d d Bloch
energy of the combined lattice+ion system. The second bracket is the Schrodinger Hamiltonian for two mass-2, charge-1 particles relative to their center of mass. The Hamiltonian calculates kinetic energy using the reduced mass of the two equal-mass deuterons, which is ma/2. The second term within the bracket calculates the dd Coulomb repulsion work in accord with double Bloch symmetry. The interaction potential is calculated for the work done in each unit cell as the coherently partitioned charge fractions are brought together so as to reduce the 1*12 separation. Coherency requires that the work done in each unit cell be summed so as to give the total work involved in reducing |ri21- The summed work = e 2 /(iV we n|ri2|). The nuclear potential term -Bnuc(i"i2), which is negative, reflects the contact nature of the strong interaction. It contributes (negatively) to subsystem energy once the separation |ri21 is reduced to twice the deuteron radius. At this point the Coulomb + nuclear force is attractive for a spin-zero double-deuteron (which has symmetric
672
coordinate-exchange symmetry), 2 and there is no barrier to fusion into a coalesced coordinate-exchanged dd nuclear configuration. A second approximation to the Hamiltonian adds the effect of having a Blochsensitive nucleus final state. The coalesced double deuteron is a Bloch-sensitive nucleus. The work done in bringing two deuterons to nuclear contact depends on the degree of partitioning, as designated by iVWeii- This means that the energy level of the coalesced product nucleus is a function of /Vweii. The second approximation Hamiltonian H2 is H i ( r , r 1 2 ) 9* | - ^ V
2
+ (2e)C/ lattice (r,7V well )|
H2 V TO d
^ 2 2
+
e2
1
Y, AT2 {lr ,H M + ^uc(ri2,iVwen». (2) jr( A^ ell |(ri2+Ri2i)| I coherent volume
*
This Hamiltonian couples the r and r i 2 dependencies. It provides an explicit coupling between the hosting lattice and the double-deuteron nuclear configuration. 7. Intermediary Bloch-Sensitive Nucleus The immediate (direct) coalesced double-deuteron nuclear product does not have the a particle nuclear configuration. The a particle configuration involves the attraction between spin-paired coordinate-exchanged protons and spin-paired coordinate-exchanged neutrons, rather than the attraction between spin-zero coordinate-exchanged deuterons. The F - P fusion reaction can be viewed as a 2-step reaction. The first step starts with a spin-zero double-deuteron 2-D Bloch and ends with a spin-zero coalesced double-deuteron 4 He d J B l o c h " intermediate state. There is no change in coordinate exchange. The second step is a change from the coalesced 4 He 2 J B l o c h " intermediate state to the Bloch alpha configuration 4 He B | o c h , in which the two protons are coupled by coordinate exchange and the two neutrons are coupled by coordinate exchange. The 4 He d J B l o c h designates an intermediary Bloch-sensitive nucleus, while final product 4 He B j o c h is not Bloch sensitive. The last term in H 2 describes an explicit coupling between the intermediary nuclear state and the lattice. The lattice parameter Nwe\] in {r} affects the Gibbs free energy of the nucleus 4 He 2 id " Bloch . Reversibility requires that the structure of the nuclear state in {ri 2 } affects the lattice potential [/lattice (r, Nwe\\) in {r}. The last term in H 2 is the Bloch-sensitive nuclear strong force term 2r d
£nuc(ri2,Nwell(r)) = .Enuc, strong(l-l 2 )-
r 2 / 6 / — d|ri 2 |, J |l"i2|/Vwell |r.c|
where r s c is the screening radius and r j is twice the nuclear radius of the deuteron. The integration limit |r sc | expresses imperfect dressing caused by the mismatch between the deBroglie wavelength of the electron and the deBroglie wavelength of the deuteron. It is a lattice parameter whose value is determined by energy minimization of the combined double-deuteron Bloch function and the many-body lattice
673
system. For the non-ideal case (e.g., imperfect lattice) not all potential wells will have the same weight, so iVWeii should be considered an effective number of potential wells, and not necessarily an integer. The integral is the work required to bring the coherently partitioned nucleus into nucleus-nucleus contact. The subscript "nuc, strong" emphasizes that the weak force plays no role in the cold fusion nuclear interaction. 8. Coupling to the Lattice The coupling mechanism between {r} and {1*12} involves the parameter Nwe\\t which determines the surface area of the double-deuteron subsystem. In other words, iVWeii determines the circumference of the planar double-deuteron nucleus. Without the nucleus-lattice coupling in {r,ri2} the circumferential boundary is determined by electrostatics involving the initial hosting crystallite, which is part of the multi-crystallite hosting metal. When the double-deuteron is in coalesced form (fusion product form), the Gibbs free energy of the hosted Bloch-sensitive nucleus decreases with increasing Nwe\\. This decrease in free energy powers an increase in the area of the locally periodically ordered portion of the metal's surface layer, in a manner that matches the periodicity of the central portion of the periodically ordered sub-region, where the 4 He^J B l o c h was formed. During nucleus expansion, work is done on the multi-crystallite metal lattice, while the combined lattice-nucleus system goes to a lower energy level. Ignoring the possible role of resonance, it seems likely that the dd cold fusion reaction is not a simple single-step transition. During energy transfer to the lattice, the double-deuteron may exist transiently in a mixed quantum state 2Dg loch < -^ 4 He d J Bloch ." The mixed quantum state fluctuates between the initial eigenstate 2-D Bloch and a coalesced virtual state 4 He^J B l o c h . (A virtual state can violate conservation of energy by \AE\ for time At such that |A.E|A£ ~ h.) Fluctuations in effective Nwe\\ scatter lattice electrons or generate phonons at the subsystem boundary, which is measured as the locus of classical turning points. Energy transfers result in the metastable state designated 4 He^J B l o c h . Completion of the fusion reaction requires a second step. The second reaction step transitions 4 He^J B l o c h into the Bloch form of the partitioned alpha ground state 4HeB"j~och (4He|"]och = «Bioch )• This second step is also not a single-step transition. It involves a second mixed quantum state 4 He^J B l o c h <-> 4 He B | o c h , which fluctuates between the Bloch coalesced double deuteron and the Bloch alpha configuration. Again, fluctuations in effective A^weii scatter lattice electrons or generate phonons at the "ATwen" boundary. Since the Bloch alpha product is not directly formed by forcing two deuterons together, the 4 He B | o c h (=aBioch) is not a Bloch-sensitive nucleus. Its energy level is independent of the Coulomb work carried out in the initial forced coalescence of the spin-zero dd pair. As a result, the ground state energy level of 4 He B | o c h is the same as that of the ordinary doubly ionized helium ion 4 He 2 + . Hence 4HeB"j^ch is not Bloch-sensitive.
674
Summarizing the above picture, and remembering that d = D + = 2 D + , the F - P reaction is 2D£ioch - 4 H e ^ + B l o c h -
4
He|| o c h = aB1och,
(3)
where reversibility is converted to irreversibility by energy transfers to the metal lattice at the dd subsystem boundary. The symbol «-> signifies fluctuations occurring while in a mixed quantum state, which can be treated as a virtual state. The 4 He d J B i o c h state is a Bloch-sensitive state, whereas the initial and final states are ordinary stationary states of Schrodinger quantum mechanics. 9. Reaction Rate Calculation Let us now consider the F - P reaction rate problem. The reaction rate physics that makes F-P fusion possible recognizes that nuclear force is a contact force. The reaction rate calculation is based on the Fermi Golden Rule for calculating time-dependent perturbation of a stationary state configuration. Wave function overlap is required for fusion to occur. The reacting deuterons must share some common volume of space, and the initial state wave function must also share a common volume of space with the final state wave function. The condition that normally prevents this from happening is a zone of exclusion, caused by inadequate electron screening. The inadequate screening prevents deuteron(l) from contacting deuteron(2). This zone of exclusion vanishes if the charge repulsion between the two deuterons is sufficiently reduced. This reduction occurs if one or both of the deuterons is coherently partitioned into a sufficiently large number of pieces. The second overlap requirement, namely, the sharing of space between the initial and final states, introduces a very small number into the reaction rate calculation. This small number is about 10 - 1 5 . It is the volume ratio between the volume of the product nucleus and the volume of the pre-coalesced 2-deuteron system. This small overlap occurs in {ri2J. The overlap in {r} is unity, due to coordinate exchange, which in the large iVweii configuration considered, causes the two Bloch deuterons to "sit on top of each other." The reaction takes place at Nweu locations in {i"i2}, and at the continuum of points which contribute deuteron density in {r}. The small volume ratio in { r ^ } is what keeps the nuclear reaction rate small and what makes the F - P fusion process intrinsically relatively safe. The Fermi Golden Rule equation includes a summation over final states. As applied to the nuclear reaction step, there could be a single final nucleus state. However, a modeling of Oriani's observations of anomalous cold-fusion related MeV-energy particle showers suggests that there could be a large density of nucleus final states, describing a range of vibrationally excited nuclear excitations. 7,8 Additional Bloch-phonon hyperfine states may exist, as discussed in Paper III. The reaction rate calculations apply to spin-zero double-deuteron pairings, and to deuterons in both 2-dimensional and 3-dimensional symmetry Bloch configurations. The feedstock reactive component is best thought of in terms of a multiply occupied ion-band state, i.e., as a many-body Bloch system in which individual D+
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quasiparticles are simultaneously partnered with all the other D + quasiparticles in a reactive subsystem. 1 The spin-zero pairings are 1/3 of the total pairings. 2 (There is another 1/3 of total pairings that has symmetric coordinate-exchange symmetry and non-zero spin, and a final 1/3 which has anti-symmetric coordinate exchange symmetry, so that amplitude —> 0 as ri2 —> 0.) In this picture the reaction rate per subsystem for large and small subsystems is the same at equal Bloch-deuteron concentration Dg l o c h /Pd. The subsystem reaction rate varies with concentration as (Dg l o c h /Pd) 2 . In F - P cold fusion most of the deuterons in PdD^ are non-Bloch deuterons and are not part of the reactive subsystem. Because small and large subsystems have equal reaction rate at the same Dg l o c h /Pd as long as Nweu 3> iVWeii, critical, this picture leads to the recommendation that "small crystals are better." Crude calculations assuming 3-dimensional periodic symmetry, such as might exist in PdDa, at large loading where x ~ 1, indicate that the reaction rate can provide cold fusion power in the observed range. 10. Role of Resonance Li has pointed out that resonance (no change in system energy) can play a major role in cold fusion reactions. 9 The existence of Bloch-sensitive nuclei, whose energy level varies with the degree of partitioning as measured by iVweii, makes the occurrence of resonance a likely phenomenon in cases where a non-partitioned reaction product would be moderately endothermic. This situation seems to apply to the fusion of Bloch alpha-particles, as addressed in Paper III. An increase in JVwen makes the reaction increasingly exothermic. If the endothermicity of the non-partitioned reaction is not too high, at some value of Nwe\\ the heat of reaction passes through zero. Since lattice imperfections affect the effective Nweu, and since the effective iVweii need not be integer, a relatively precise matching of the resonance condition seems possible, in part due to the many internal nuclear vibration,rotation excited states 8 that may be present. Li's resonance picture was developed to explain tunelling through a Coulomb barrier for deuterons in a side-by-side molecule-like geometry. In this paper, we are discussing the coherently partitioned Bloch configuration where deuterons are superposed and there is no Coulomb barrier. A coherently partitioned configuration is required for the existence of Bloch-sensitive nuclei. When there is no Coulomb barrier, the resonance can be broad and is better thought of as a Feshbach resonance. In a Feshbach resonance a transition occurs between equal-energy states with different configurations, such as occurs when an atom Bose condensate switches into a molecule-like Bose condensate form.10 The occurrence of nuclear resonance would mean that an initial nuclear reaction could occur without need for "instantaneous" energy transfer to the lattice. During resonant nuclear fusion transitions, an energy transfer process acting on a nonnuclear slower time scale could make the initial interaction irreversible. As a result, potential impediments to fusion due to a difference in the time scales of the nuclear part of the reaction relative to that of an electromagnetically coupled energy transfer
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step are avoided. In accord with the 2-step process applied to the deuteron fusion case, slower sequential electromagnetic-time-scale energy transfer fluctuations of a mixed q u a n t u m state can transition the deuteron subsystem into the partitioned metastable form 4 H e ^ B l o c h . T h e energy transfer process partially stabilizes the intermediary 4 H e ^ J B i o c h Bloch-sensitive nucleus. Similar energy transfer fluctuations can transition 4 H e d J B i o c h into 4 H e B | o c h at the electromagnetic rate. These slower transfers of energy, which involve mixed q u a n t u m states, occur in response t o fluctuations in iVweii, completing the transition from 4 H e d J B i o c h " t o 4 H e | 4 o c h .
11. Alternative Picture B a s e d on Feshbach R e s o n a n c e There is an alternative modeling of the role of Feshbach resonance in F - P cold fusion. T h e energy level of the intermediate fusion state 4 He dd ~ B l o c h is subject to large predissociation broadening, because of t h e near identity of its structure with t h a t of the "un-coalesced" (dissociated) state 2 - D B l o c h . If the life time of the 4 He dd ~ B i oc h state is 10~ 2 2 s, the broadening extends the wings of the resonance peak so as to include the energy levels of b o t h the un-coalesced initial state 2 - D B l o c h and the coalesced final state 4 He B j^ ) d l state, even though these states are separated by 24 MeV. Predissociation broadening of a nuclear energy level has proved important in modeling Oriani showers, as discussed in P a p e r III. Fluctuations in the energy level of the intermediate state 4 He dd ~ B i oc h means fluctuations in the double-deuteron's value of -Nweii) which means fluctuations in the circumference b o u n d a r y of the 2-deuteron subsystem, which means fluctuations are imposed on the hosting lattice. T h e fluctuations span a large range of time scales. T h e slower fluctuations (possibly as groups of fast fluctuations) can be expected t o scatter electrons or generate phonons at the circumferential boundary, resulting in energy transfer. T h e situation is the reverse of t h a t encountered in the Oriani shower problem, where Brownian-motion type energy transfers play a key role. As the energy transfer process proceeds, the resonance peak moves toward t h e energy level of 4 H e B | o c h . Since t h e process is enabled by a Feshbach resonance, the change in structure from spin-paired deuteron to alpha configuration is allowed.
References 1. T.A. Chubb and S.R. Chubb, Cold fusion as an interaction between ion band states, Fusion Technol. 20, 93 (1991). 2. L.I. Schiff, Quantum Mechanics (McGraw-Hill Book Co., New York, 1955). Note particularly discussions on applicability of coordinate-exchange-symmetry and on spinsymmetry as applicable to paired spin=l particles, pp. 307, 225-226, 231-232, and nearby pages. 3. M.J. Puska, J.R.M. Nieminen, M. Manninen, B. Chakraborty, S. Holloway, and J.K. Norskov, Quantum motion of chemisorbed hydrogen on Ni surfaces, Phys. Rev. Lett. 51, 1081-1084 (1983). 4. M.J. Puska, and R.M. Nieminen, Hydrogen chemisorbed on nickel surfaces: a wave mechanical treatment of proton motion, Surface Sci. 157, 413-435 (1985). 5. C. Astaldi, A. Bianco, S. Modesti, and E. Tosatti, Vibration spectra of atomic H and
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6.
7.
8. 9.
10.
D on C u ( l l O ) : evidence of H quantum derealization, Phys. Rev. Lett. 68, 90-93 (1992). T.A. Chubb, and S.R. Chubb, Radiationless cold fusion: why small 'crystals' are better, Nceu requirement, and energy transfer to lattice, Proc. ICCF6, Vol. 2, Editor, M. Okamoto (New Energy Development Organization, Tokyo, 1996). p. 417. R.A. Oriani, and J.C. Fisher, Energetic charged particles in the gas phase produced by electrolysis, in Proceedings of the ICCF10, in press (2005); R.A. Oriani and J.C. Fisher, Energetic particle shower in the vapor from electrolysis, in IGCF11 Abstracts (www.iscmns.org/Abstracts, (2004). K. Heyde, Basic Ideas and Concepts in Nuclear Physics, (Institute of Physics Publishing, Bristol and Philadelphia, 1994) pp. 299-323. X.Z. Li, M.Y. Mei, J. Tian, D.X. Cao, and C.X. Li, Coherence in cold and hot fusion, in Proceedings of the ICCF8 Conference, Vol. 70. Editor, F. Scaramuzzi (SIF, Bologna, 2000), p. 357; X.Z. Li, J. Tian, M.Y. Mei, and C.X. Li, Sub-barrier fusion and selective resonant tunneling, Phys. Rev. C 6 1 , 024610 (2000); X.Z. Li, Nuclear physics for nuclear fusion, Fusion Sci. Technol. 4 1 , 83 (2002); X.Z. Li, B. Liu, S. Chen, M.W. Wei, and H. Hora, Fusion cross sections for inertial fusion energy, in Laser Particle Beams, Vol. 22:4 (Cambridge University Press, UK, 2004), p. 469. W. Zhang, C.P. Search, H. Pu, P. Meystre, and E.M. Wright, Feshbach-resonanceinduced atomic filamentation and quantum pair correlation in atom-laser-beam propogation, Phys. Rev. Lett. 90, 140401 (2003).
II. I N H I B I T E D D I F F U S I O N D R I V E N SURFACE TRANSMUTATIONS
T A L B O T A. C H U B B Greenwich
Corp.,
5023 N. 38th St., Arlington, E-mail: [email protected]
VA 22207,
USA
This paper is the second of a set of three papers dealing with the role of coherent partitioning as a common element in Low Energy Nuclear Reactions (LENR), by which is meant cold-fusion related processes. This paper discusses the first step in a sequence of four steps that seem to be necessary to explain Iwamura 2-a-addition surface transmutations. Three concepts are examined: salt—metal interface states, sequential tunneling that transitions D+ ions from localized interstitial to Bloch form, and the general applicability of 2-dimensional vs. 3-dimensional symmetry hosting networks.
1. Introduction Iwamura et al. 1 have developed an LENR process that converts surface Cs atoms into surface Pr atoms using deuterium permeation through a specially structured, largely metal assembly. The assembly consists of a Pd substrate on which are deposited four layers of 2-nm CaO overcoated with 8-nm Pd, plus one CaO layer overcoated with a 40-nm Pd inflow layer. The Iwamura assembly is used as a permeable barrier between a D2-pressurized volume and a vacuum volume. 2. Envisioned Process The author speculatively models the process as follows. At a CaO-Pd interface, a diffusing deuteron is converted into a coherently partitioned, nuclearly reactive Bloch form Dg l o c h . 2 Multiple Bloch deuterons organize themselves into a manybody Bloch-ion subsystem. Independent subsystems form on different CaO crystallites as shown in Fig.l. In these subsystems Bloch deuterons fuse, creating Bloch helium ions 4Heg"|"0(:.h. In a second step two 4Heg~]~och fuse, creating a product nucleus 8 Be B | o c h , which is stabilized by being coherently partitioned. The 8Beg"]"och is energized by increases in coherent partitioning in a process that uses nuclear energy to mobilize the Be ion. The 8 Be B | o c h nucleus spreads out beyond the hosting CaO-metal interface, spreading along accessible Pd-crystallite boundaries, including the interfaces between metal and gas, and metal and vacuum. A Cs atom protruding above the mean surface of the Pd metal is overlapped and infiltrated by the 8 Be 4 j| och . The Cs nucleus combines with and absorbs the 8 Be 4 J | och nucleus, and becomes a Pr atom. Both the formation of Bloch helium and the transmutation of surface Cs into Pr are exothermic processes. 678
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3. Primary Challenge The core question is: Why does Bloch deuterium form within the CaO-metal interfaces? My guess is that within the interface layer the Bloch deuterium configuration has lower free energy than such discrete particles as D + , D~, or adsorbed free-radical D atoms. This is generally not the case at the metal-gas and metal-vacuum interfaces, where electron-neutralized surface D + ions must be in excited states to be of Bloch configuration.3 Bulk CaO is a face centered NaCl lattice with a large Gibbs free energy of —898kJ/mol. One might imagine that a CaO crystal, with its alternating positive ion, negative ion structure, when interfaced with deuterided Pd could host a fraction of a Dg loch ion adjacent to each interface 0 2 ~ ion and a fraction of a Dg l o c h ion adjacent to each interface Ca 2 + ion. Each fractionally distributed Bloch deuteron and its fractionally distributed neutralizing electron charge would be in Bloch-function configuration. In Fig. 2, the CaO lattice determines the Bloch periodicity, while the interface boundary electrons of the more plastic metal adjust to ensure unit cell neutrality. The result is a partitioned D + ion with a local maximum in density within each of a large number of non-self-trapping potential wells.4 The essential step that transitions localized D + into a delocalized Bloch configuration presumably occurs within these CaO-Pd interface layers, as discussed later. Bloch deuteron pairs
Pd substrate
CaO
Pd overcoat
Figure 1. Multi-crystallite modeling of Iwamura reactor plate, showing contacts between Pd substrate, sputtered CaO deposition layer, and sputtered Pd metal overcoat. The CaO is shown as a discontinuous set of ionic nano-crystals.
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then convert into wavelike 4 Heg| och , which participate in Step 2 of the Iwamura process.
Salt-metal-interface Bloch deuterium CaO
Figure 2. Fine scale view of nano-portion of interface between ionic crystallite CaO and transition metal Pd, as fabricated for the Iwamura reactor. Arrow points to the location of the hypothesized D Bloch deuteron. The B+{ och ' o n ' s a n u c l e u s with 2-dimensional symmetry matching the template provided by the CaO crystallite, and is neutralized (dressed) by the metal's electron Fermi sea.
4.
Impact on Cold Fusion
The Iwamura et al. a-addition transmutation discoveries are the first of two new discoveries that clarify the role of coherent partitioning and Bloch-sensitivity in LENR processes. The Iwamura program started as a Mitsubishi Heavy Industries research study exploring anomalous Fleischmann-Pons (F-P) emissions. Mitsubishi support allowed the science team to evolve their program into use of permeation as a means of avoiding electrolysis contamination worries. The Iwamura protocol is a non-electrolytic deuterium-palladium process by which surface Cs atoms have been repeatedly transmuted into surface Pr atoms. The Iwamura team has identified a new class of transmutations. The archetype is 133 Cs + 2a ^ 1 4 1 P r , which is a type of
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"a-addition transmutation." In the Iwamura process deuterium is forced to diffuse through Pd metal by exposing the front surface of the previously described special Pd plate reactor to D2 gas at 1 atm pressure at 70° C, while the gas from the back side of the plate is pumped away using a vacuum pump. The transmutations do not take place without the use of a complex plate reactor. The specified design describes a Pd foil support plate of 0.1mm thickness, on which are sputter-deposited a set of diffusion-inhibiting layers. Inside the plate there are five sputter-deposited 2-nm layers of CaO salt, separated from each other by sputter-deposited 8-nm layers of Pd metal, and topped with a 40-nm layer of sputter-deposited Pd. A sub-monolayer coating of Cs atoms is deposited on the top surface. The transmutation of Cs into Pr occurs during week-long permeation runs. Cs and Pr surface concentrations are measured by X-ray photoelectron spectroscopy (XPS) before and after permeation, and twice during imposed run interruptions. The salt layers, likely in the form of small CaO crystals, partially block the deuterium atoms as they work their way through the Pd plate. Transmutation is not observed if H-permeation is substituted for D-permeation, or if the CaO layers are not included in the plate structure. The Iwamura process differs from F - P methods in that it avoids electrolysis. The F - P process uses overvoltage electrolysis to create a PdD^ interstitial deuteride with x = D/Pd > 0.85. To achieve x > 0.85 by equilibrium chemistry requires D 2 pressures > several kbar. 5 On the other hand, both processes release nuclear energy from exothermic nuclear reactions, and transfer the released nuclear energy in a manner that heats a hosting metal lattice. Step 1 in the Iwamura process takes place at less than standard deuterium chemical potential. The Iwamura process imposes challenges to cold fusion modelers. To model the Iwamura process one must explain: (1) why nuclear energy release occurs at relatively low D2 chemical potential, (2) how a process made possible by interior CaO crystals can effect transmutation on a distant metal surface, (3) how the transmutation of a high Z nucleus can occur, and (4) why the transmutation involves addition of two alphas instead of one. This paper is concerned mainly with Challenge 1. Challenges 2-4 are addressed in Paper III.
5. Low D g | o c h Concentration Problem Let us consider Iwamura's success in achieving nuclear effects at relatively low Dg l o c h /Pd ratio. As described above, it is suggested that the periodic structure provided by the CaO salt crystallites helps create a one layer thick interface volume unusually suitable for hosting coherently partitioned Bloch deuterons. CaO is an ionic salt like NaCl, and has a large negative Gibbs free energy, which suggests that its ordered form is not easily altered. In this speculation, the CaO forms the template for wave-like deuterium, and the metal's electrons forms the negative charge cloud that converts a positive ion into the neutral "atom" form.
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6. Initial Step in Coherent Partitioning A relatively simple process can be envisioned by which the Iwamura plate reactor creates coherently partitioned deuterons. An incident D 2 gas molecule strikes the Pd top surface and dissociates into two adsorbed D atoms. Each adsorbed D atom enters the Pd top surface by tunneling into an interior self-trapping octahedral site within the fee lattice. The permeating deuteron then diffuses through the top sputtered Pd layer in response to an internal deuteron concentration gradient. Some of the deuterons encounter a CaO crystallite during the diffusion process. After hopping into one of the potential wells provided by the CaO-metal interface volume, it tunnels through a low potential barrier to an adjacent potential well within the interface's 2-dimensionally ordered periodic subsystem. Because of the low potential barrier between potential wells of the 2-dimensional symmetry interface sub-region, and because of the non-self-trapping character 4 of the trapping sites, this tunneling splits the wave function into two coherent parts, as described in Merzbacher's treatment of a particle in a "double-oscillator" potential. 6 The Merzbacher solution of the 2-potential well problem describes a single particle which is split between 2-potential wells. The split-particle wave function has the same wave function phase-coherency that characterizes a single particle bound inside a single potential well. Thus, the transition between single well geometry and double well geometry preserves wave-function phase order. Applied to the Iwamura geometry, it transiently creates a double-maximum coherent deuteron configuration. Further tunnelings further coherently delocalize the wave function, completing a transition from a double-maximum wave function into a coherently partitioned 7Vwen-maximum Bloch form.
7. Cautions It is probably a mistake to assume that cold fusion processes are always associated with 2-dimensional symmetry Bloch deuterons. The heat release associated with Iwamura transmutations is in the low mW range, whereas a number of F - P related studies have resulted in heat release in the multiple Watt range. The Iwamura Cs studies do not include calorimetric measurement of heat; hence it is unknown to what extent additional cold fusion heat release occurs concurrently with transmutation heat generation. For F - P studies involving bulk Pd, it is the consensus view that measurable excess heat is normally produced in PdD^ with x > 0.85. At x > 0.7, it becomes thermodynamically possible to begin to have some small fraction of the interstitial deuteron population occupying 3-dimensional-symmetry bulk-Pd tetrahedral sites. 7 Some modelers suggest that tetrahedral site occupation by a fraction of the interstitial deuterons present in the bulk is required for F - P heat generation. It is important to consider the work of Arata and Zhang (A-Z). A-Z have studied excess heat generation occurring in deuterided Pd in the form of fine
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powders, such as Pd-black. 8 This powder has a nm-scale structure, as evidenced by a broadening of its X-ray Bragg reflection peaks. A-Z have suggested that the powder may include domains having atom cluster order, as described by Fujita.9 They have also suggested that high surface mobility is involved, and have used the term "spillover deuterium" to describe this property. "Spillover deuterium" is a term used in catalyst literature to describe anomalously high hydrogen activity. Recently A-Z have explored use of powders produced by oxidizing amorphous Pd-Zr alloys.10 These powders are very effective absorbers of deuterium gas. If all the absorbed gas is absorbed in the Pd fraction, which is not oxidized, the D/Pd ratio approaches 3, i.e., the PdD^ —* PdD3. In a recent paper 11 not yet published in English, Arata has suggested that the structures produced by deuteriding these powders have fee structures in which the octahedral sites are occupied by more than one deuteron. These expanded structures are presumably made possible by the large area/volume ratio of the powder, which reduces expansion stress relative to that of bulk metal. In his view, the potential well volumes surrounding the two tetrahedral sites and the incrementally available volume associated with a fully occupied octahedral site are about the same. He says that the tetrahedral sites can be transiently occupied. By the same argument the available volume for an incremental occupation of a fully occupied octahedral site can also be transiently occupied. In this view, the presence of these three transiently occupyable volumes in each unit cell forms an interconnecting network that runs through the metal atom cluster. It would constitute a 3-dimensional symmetry network of low barrier potential wells. In such a network the "Merzbacher" coherent partitioning process could occur in the same manner as occurs within Iwamura's 2-dimensional symmetry CaO-Pd interface volume. Diffusing deuteron "visitors" would be converted into coherent Bloch form. It is also important to note that an ordering of wave function phases should be able to occur without sequential tunneling in sufficiently low temperature Pd which has sufficient lattice array order. In the low temperature limit T —> 0, spontaneous ordering should occur in fully loaded palladium PdD. In PdDi + ^, the (5-deuteron fraction should exist in a coherently partitioned Bloch form so as to avoid the free energy cost of breaking lattice symmetry. 12 The F - P cold fusion could then take place in a mode that does not break lattice symmetry in a Mossbauertype momentum-preserving process. Reaction energy goes into the recoil energy of the coherently partitioned Bloch product 4 He|j" och and the recoiling crystallite. This type of fusion does not require the irreversibility step associated with electron scattering. For example, a recoiling host occurs during the Mossbauer energy release from an iron-containing lattice in a process that balances the momentum of a released gamma ray. The de-excited Fe atom recoils as part of the recoiling lattice crystallite. The spontaneous ordering would be an example of the ordering that occurs in many-body lattice systems. 13 However, the author's present view is that it is unlikely that spontaneous ordering is occurring in the above-room-temperature environment that characterizes the Iwamura process.
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References 1. Y. Iwamura, M. Sakano and T. Itoh, Elemental analysis of Pd complexes: effects of D2 gas permeation, Jpn. J. Appl. Phys. 4 1 , 4642 (2002). 2. T.A. Chubb, The dd cold fusion-transmutation connection, Proc. ICCF10, (2004); T.A. Chubb, Bloch ions, This Proceedings. 3. M.J. Puska, and R.M. Nieminen, Hydrogen chemisorbed on nickel surfaces: a wavemechanical treatment of proton motion, Surf. Sci. 157, 413 (1985); See Fig. 13. 4. T.A. Chubb, LENR: superfiuids, self-trapping and non-self-trapping states, Proc. ICCF10, (2004) in Press. 5. J. Baranowski, Metal hydrogen systems at high hydrogen pressure, Hydrogen in Metals II, ed. Alefield and Volkl (Springer-Verlag , Berlin, 1978), p. 157; Fig. 4.5 shows pressure for H/Pd. Pressures for D / P d are higher. Taken from lecture by S. CrouchBaker. 6. E. Merzbacher, Quantum Mechanics (Wiley, New York, 1964). pp. 64-77. 7. R.A. Oriani, The physical and metallurgical aspects of hydrogen in metals, Trans. Fusion Technol. 47, ICCF4, 235 (1994). See p. 239. Y. Arata, and Y.-C. Zhang, A new energy caused by 'spillover deuterium', Proc. Jpn. Acad. 70B, 106 (1994). H. Fujita, Studies on atom clusters by ultra-high voltage electron microscopy, Mater. Trans., JIM 35, 563-575 (1994). 10. Y. Arata, and Y.-C. Zhang, Development of compact nuclear reactor using solid pycnodeuterium as nuclear fuel, Proc. ICCF10, (2004) in Press. 11. Y. Arata, The formation of 'solid deuteriums' solidified inside crystal lattice and intense solid state nuclear fusion, translation to be published in 21st CenturyScience (2005) 12. T.A. Chubb, and S.R. Chubb, Cold fusion as an interaction between ion band states, Fusion Technol. 30, 93 (1991). 13. S.R. Chubb, and T.A. Chubb, Relationship between microscopic and macroscopic interactions in low energy nuclear reactions, Proc. ICCF9, Edited by Xing Z. Li (Tsinghua University Press, Beijing, 2003), p. 57.
III. BLOCH NUCLIDES, I W A M U R A T R A N S M U T A T I O N S , A N D ORIANI SHOWERS
T A L B O T A. C H U B B Greenwich
Corp.,
5023 N. 38th St., Arlington, E-mail: [email protected]
VA 22207,
USA
The Iwamura et al. 2-a addition transmutations 1 and the Oriani—Fisher energetic particle showers 2 demand an explanation. They both depend on the same physics as responsible for cold fusion, namely the phase-coherent partitioning of deuteron charge when the deuteron assumes a Bloch-like form and becomes distributed among a large number Nweu of potential wells. As a result, the work required to bring the two "nuclei" into contact is reduced by l/iV we n- In cold fusion 2 spin-zero paired deuterons fuse as per 2
- D B l o c h - 4 H e B ! o c h + 23-8MeV.
In the Iwamura process 2 4HeB~T , fuse as per H e
M B T o c h ^ B e B l o c h + E-*nuc,
in a Bloch-sensitive reaction where reaction energy Enuc is a function of iVweii. Deuteron cold fusion is not Bloch sensitive because the reaction changes the coordinate exchange symmetry pairing. A Bloch-sensitive fusion product is mobilized to seek a larger number of hosting wells. This causes 8 B e B j o c h to migrate to a surface where Cs+ ions protruding above the surface are overlapped. They add the 8 B e B j o c h product in an exothermic reaction. In an Oriani process the 8 B e B | c h detaches from its hosting surface, dissolves, forms clusters, and gets suspended in off-gases as a flake nucleus with 2-dimensional periodic symmetry. Its geometry and internal nuclear excitation spectrum cause a normally forbidden energy transfer from gas to flake, until the increasingly energized 8 B e B j o c h fissions into a pair of MeV alpha particles.
1. Iwamura Transmutations We first model the Iwamura transmutation process. In the Iwamura transmutation process deuterium permeates a plate reactor containing five internal CaO diffusioninhibiting layers. The process results in a slow transmutation of a surface layer of Cs atoms into Pr atoms by a 2-a addition reaction The process involves four steps. Step 1 is a fusion of 2 D + into 4 He 2 + . It is followed by three steps: the fusion of two 4 He 2 + into 8 Be 4 + , the migration of the 8 B e 4 + to the plate's surface, and the absorption of the 8 B e 4 + by a surface-deposited Cs atom. The deuterons, 4 He 2 + , and 8 Be 4 + are all in Bloch form. The starting reaction is a 2-dimensional symmetry version of the Fleischmann-Pons (F-P) Bloch-function cold fusion reaction. The final-state product of F - P fusion is 4 He 2 + in a coherently partitioned Blochwave form. 4 He 2 + is an alpha particle and has zero spin. If coherently partitioned 685
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He 2 + is created from coherently partitioned D + , it seems reasonable to assume that partitioned 8 B e 4 + can be created from partitioned 4 He 2 + . The 8 BeB| och product is a Bloch-sensitive nucleus, since no change in coordinate exchange symmetry and no spin change accompanies its creation. The 2-a-fusion reaction requires that the partitioned 8 Be nucleus be stable. Non-partitioned 8 Be is unstable by about 0.09 MeV. 3 It is unstable because the work of bringing two 4 He nuclei together is greater that the energy release accompanying the merger of the two 4 He 2 + by a difference of 0.09 MeV. The charge repulsion work is about 1.5 MeV, which means that the nuclear energy made available by merging the two 4 He nuclei is about 1.4 MeV. However, double Bloch symmetry means that the charge repulsion work is reduced by having the 4 He 2 + partitioned. Therefore, at large Nwe\\ the partitioned nuclear product should be stable. Since Bloch 8 B e 4 + is Bloch-sensitive, a decrease in free energy drives an expansion and migration, which delivers it to the metal surface. In contrast, the F - P fusion product 4 He 2 3 | och is not Bloch-sensitive, hence remains within the interface subsystem where it was created. Transmutation occurs when the expanding 8 Beg| och overflows an above-surface Cs + ion in its path. In a suitably deposited sub-monolayer a Cs atom loses its valence electron to the Pd metal and resides as an above-surface ion. The expanding 8 Be B | o c h overlaps the Cs nucleus, encountering a deep nuclear potential well. Because of partitioning, there is only a small amount of positive charge within a single charge-density maximum of the 8Beg"j^ch, namely where a single maximum overlaps a non-partitioned Cs nucleus. The Coulomb repulsion between the Cs nucleus and the small amount of charge in a single maximum is insufficient to destroy the coherency of the 8 B e 4 + Bloch state at large Nweu. Minimization of system energy is the reason that overlap occurs. The 8Beg"Joch and the localized 133 Cs nucleus form a composite state, i.e., Bloch 8 B e + localized 133 Cs. After a first scattering interaction with the lattice at the 8 Be 4 j| och boundary, a mixed quantum state describes the composite state. The iVweii fluctuation process transfers the exothermic reaction energy to the lattice, producing a 1 4 1 Pr stationary state nucleus. Spin considerations seem to suggest that the product state should be a spin 7/2 state, whereas the 1 4 1 Pr ground state nucleus is spin 5/2. It may be that the product state is 1 4 1 Pr spin 7/2, which is metastable by 145 keV. 133
2. Oriani Showers We now model the Oriani showers. Oriani showers are characterized by the observation of MeV-energy decay particles recorded as tracks in CR-39 plastic. The showers are an occasional and anomalous result of F - P electrolysis. There have been repeated observations by Oriani of the MeV-energy particle showers. They demand explanation. The showers are a more challenging problem than the crude modeling of F - P cold fusion and the Iwamura transmutations. Like the Iwamura process, the phenomenon depends on coherent partitioning. But while the fusion and transmutation processes require only a clarification of the protocol used to mathematically describe the wave function of a coordinate-exchanged 2-body Bloch
687
system at large iVweii (double Bloch symmetry), modeling of the Oriani showers explores new physics in the interaction between a coherently partitioned nucleus and a Maxwellian gas. The modeling questions the applicability of the Second Law of Thermodynamics in an unusual sequential scattering process that preserves micro-reversibility. The Oriani observations are illustrated in the following quotes. Oriani and Fisher write, "Approximately 40,000 energetic charged particles were recorded in a pair of plastic detector chips suspended in vapor above an active electrolysis cell... Analysis of track orientations indicates that the shower originated in a compact source in the vapor between the chips... duration is estimated to have been a few seconds. Analysis of etch pit cone angles and sizes indicates that the tracks were produced by 2MeV alpha particles." Concerning other studies they wrote, "The detected particles carried energies in the range of a few MeV, indicating that they must have arisen in nuclear reactions. Evidence for such reactions was found in deuterium gas behind a palladium cathode that served as part of the cell enclosure, in air behind similarly disposed palladium and nickel cathodes, in air beyond the glass well of the electrolysis cell, and in oxygen gas above the anode when the anode and cathode were placed in separate arms of a U-tube cell." Regarding an earlier experiment they wrote, "We focus attention on one experiment with four detector chips suspended above the H2O solution of Li2S04 with Pd as cathode material. Two of these chips developed track densities considerably above levels in the range of controls, but the other two showed enormous numbers of tracks on the sides facing each other and much smaller numbers of tracks on their rear sides." It is difficult to explain the shower observations without building on the modeling of the Iwamura transmutations. The key ingredient is the Bloch-sensitive nucleus with 2-dimensional Bloch symmetry. In the case of Oriani's D2O experiments the Bloch-sensitive nucleus seems most likely to be the same partitioned 8 Be nucleus responsible for Iwamura's alpha-addition transmutations, i.e., 8BeB"J^ch. Each Bloch nucleus is in the form of a flake 1-nucleus thick and extending over maybe a 10-fim2 area. Electrolysis off-gas leaving the metal separates the flakes from the metal surface that had served as a template for their formation. Since water is a polarizable liquid, the flakes dissolve in the water and do not immediately transfer out of their Bloch form, with its multiple charge-density-maxima configuration. Groups of flakes can get tangled up, forming clusters. A dissolved cluster can get embedded in a gas stream evolving from either cathode or anode electrode. This set of behaviors seems required to create nuclearly unstable gas-borne clusters, as required to explain Oriani's shower observations. Interestingly, Oriani also observes MeV showers in light water electrolysis studies. In this case, my view is that the Bloch-sensitive nucleus is likely Bloch 2 He 2 + , which is the coherently partitioned form of the normally unstable spin-paired double proton. Like the 8 Be nucleus, the 2 He nucleus of impact nuclear physics is unstable. However, both 8Beg"|"och and 2 He 2 3 | och are Bloch-sensitive nuclei. In both 8 Be B ] o c h and 2 He 2 J | och , coherent partitioning reduces the Coulomb work needed to
688
bring the precursor nuclides into contact. Therefore, it is probable that 2 Heg| och , like 8 Beg| o c h , is stable at large iVweii3. Energizing Flake Nuclei None of the above explains why a cluster of Oriani flakes decays into a shower of MeV particles. The challenge is that it seems difficult to see how Bloch nucleus flakes can be energized by the cold fusion process. It seems especially difficult for the light water case, since no exothermic proton fusion process has been identified. A different energizing process seems required. Consider the case where the nuclear product is two ~ 3 MeV a-particles produced by fission of a 8 Be B J och flake. A Bloch nucleus in the form of a flake starts out as a stable, well-ordered ground-state quantum system. At large Afwell, it could be in a low energy nucleus state, stable by as much as 1 MeV. Consider the internal structure of 8 B e 4 + . The energy level chart for 8 B e 4 + is shown in Heyde 3 to contain 2 relatively low lying spin-zero states, first, the previously mentioned state that is endothermic relative to zero-velocity free alpha particles by 0.09 MeV, and second, a spin-zero state endothermic by about 6 MeV (see Fig. 1). The 6-MeV state is shown as being broadened to a width of 0.8 MeV by pre-dissociation into two alphas. This means that the flake has a very short life, of the order of 1 0 - 2 0 s, in accord with Planck uncertainty. It means that the state can be transiently occupied at reduced energy as a virtual state, in violation of conservation of energy. To explain the Oriani particles one is forced to consider a non-standard type of energy transfer from a Maxwellian gas to a flake nucleus. One must envision the flake acting as a Maxwell demon, presumably because of the relatively wide spacing between internal energy levels and because of the flake's formal 2-dimensional symmetry structure. Single atoms are considered mostly to collide elastically with the flake, as if bouncing off a rigid wall. They have too little energy to excite the nucleus. Higher energy collisions are viewed as being able to transfer energy to and from the nucleus, exciting the nucleus to higher or lower energy states. On the balance, the transitions go to higher energy levels, since a higher density of levels exists at higher energy. The internal energy of the nucleus gradually rises. Since only the higher energy collisions can contribute energy to the flake, the flake acts as a Maxwell demon, energizing the flake in apparent violation of the Second Law of Thermodynamics, but not in violation of excitation,de-excitation micro-reversibility. It can be argued that none of the molecule-flake impacts have enough energy to excite any of the nuclear transitions indicated in Heyde. However, theory suggests that expansion of a nucleus to lattice dimensions adds a hyperfine,ultrafine structure to the flake's set of energy levels, that goes beyond the Heyde treatment, while still preventing the flake from being responsive to low energy molecule collisions, as described below. Theory 4 models a Bloch nucleus as an independent periodic subsystem in physical space. It supports an independent set of body vibrations, with accompanying quantized excitations, i.e., phonons. There are 2 Nwe\\ in-plane Bloch phonon modes for a flake nucleus, plus iVWeii out-of-plane degrees of freedom, which
689
11.4-
Bloch phonon hyperfine levels
10, •
2o.-dimer model spin and isospin model quadrupole shape pre-dissociation broadening
vibration-rotation spectrum state density increases with E
-f.
if
u
2.94pp + pp + nn + nn model seniority pairing model spin-paired protons, spin-paired neutrons tetrahedral symmetry, octupole shape • 0+ 4
He + 4 He 8
-0.092 Be, A^veii = 1
Li-Feshbach resonance 0.00- r 8
Be,Mwell = 8264
Figure 1. Energy level diagram of 8 Be from Heyde, 3 and extended by interpretation and Bloch modeling. The downward shifted diagram on the right shows only the Bloch spin-zero ground states at 0.00 and 6. MeV. The downward shifting is caused by the coherent partitioning of a Bloch-sensitive nucleus. The 6 MeV state is pre-dissociation broadened, and is interpreted as an 2a-dimer spin-isospin model with quadrupole symmetry (p302). The 0.00-MeV state is interpreted as a pp + pp + nn + nn seniority-pairing model (p322) with octupole symmetry(p302). An energy level excitation structure is sketched as horizontal lines on both unshifted and shifted charts. It represents vibration,rotation excitations of the quadrupole and octupole configurations (p316). Both Bloch configurations likely have additional hyperfine, ultrafine excitation structures due to Bloch phonon degrees of freedom, shown as vertical strips. The single-well nucleus ground state is endothermic with respect to two free alpha particles by 0.092 MeV (p54). Synthesis of 8 B e t The downward shifting of the energy diagram caused by coherent partitioning brings the level representing two free 4 He 2 + into resonance with an excited vibration level of pp + pp + nn + nn BeB"J^ch. Lattice fluctuations move a virtual 2a-dimer 8 B e B ] o c l l on and off a narrow width Li-Feshbach resonance between the free alphas state and the pp + pp + nn + nn nucleus. Subsequent metal-phonon stimulated de-excitation events, and/or electron scatterings due to fluctuations in Nweu, transfer nuclear energy to the lattice. Fission of 8 B e 4 + . Oriani's D2O electrolysis leads to 8 B e B j , nuclei with 2-dimensional periodic symmetry. These nuclei resemble flakes, and are entrained in electrolysis off-gasses. Higher energy collision events with gas molecules cause excitations and de-excitations of the Bloch nucleus. Because the density of hyperfine, ultrafine states increases with increasing E, the excitation energy rises until it reaches ~ 6 MeV, at which level 8BeB"[^ h transitions to the single well 2a-dimer configuration 8 B e 4 + , which fissions into two ~ 3 M e V alphas. The alphas strike Oriani's CR-39 detector plates after losing energy in the gas.
690
greatly increases the number of nucleus excitation levels. These many additional levels support a hyperfine,ultrafine spectrum, facilitating energy transfer between gas and nucleus. If the Maxwell demon process operates, the flake nucleus rises in energy until it gets to a high enough energy that it can transition to the pre-dissociated 6 MeV state. The Bloch wave function collapses to single maximum form, and fissions, producing a pair of ~3-MeV alphas, each of which loses energy to the gas before hitting a CR-39 plate. If a 2 H e | + c h flake is energized by the same type process, energetic protons would be the Oriani-observed fission product. Proton tracks can be difficult to distinguish from alpha tracks of a different energy. Showers are the result of flake fissions within a cluster. A first fission energizes its companions, leading to a sequence of flake decays. 4. Li—Feshbach Resonance, 8 B e Synthesis, and 8 B e Fission X. Z. Li has shown that deuterons can tunnel through a Coulomb barrier to nuclear dimension if they are in energy resonance with a nuclear state for a sufficiently long time. Implicit is the presence of a very narrow resonance (width -ClOOeV), i.e., a resonance not broadened by too strong coupling to dissipation modes. 5 The dissipation can be characterized by an imaginary term in the nuclear potential. In the Bloch-ion scenario, fusion of side-by-side ions plays no role. With superposed ions, there is no Coulomb barrier. Instead the 2-body wave function has an anticorrelation factor. Nonetheless, Li's sharp resonance picture provides a useful way of envisioning the interaction between two free-space alpha particles and a coherently partitioned 8 Be nucleus. Li-Feshbach resonance and 8 Be Bloch sensitivity are applied to 8 Be synthesis and fission in Fig. 1. 5. Hyperfine, Ultrafine States and Phonon-Stimulated Transitions Consider the fusion of 2 4 He|"| och as occurs in Iwamura et al., step 2. The initial non-coalesced 2-4Heg~Joch state is modeled as a coordinate-exchanged double oiBioch i n a n anti-correlated superposed configuration (not side-by-side molecular configuration). In its coalesced form it is 8 Beg| o c h , but its nuclear structure is not the lowest energy form. This coalesced form is designated 2a-dimer. The first fusion step is a Li-Feshbach resonant transition from the coalesced 2a-dimer form to an excited state of the more stable octupole pp + pp + nn + nn configuration. Both configurations are unstable in single-well form relative to a 2-free alpha state. Being Bloch-insensitive, the free alpha state has the same energy as the initial noncoalesced 2 4Heg"|"och, and is assigned energy = —0.092 MeV. The single-well pp + pp + nn + nn nucleus is endothermic by 0.092 MeV relative to 2-free alphas. At large Nwei\ the pp + pp + nn + nn ground state is exothermic, whereas the 2a-dimer ground state, though lowered in energy, remains endothermic. The transition occurs at nuclear time scale because the two free alpha levels are Li-Feshbach resonant with an excited state of the pp + pp + nn + nn configuration, and transition occurs without energy transfer to the metal. This energy resonance is made
691
possible by Bloch sensitivity, which causes the downward shift in energy levels. The resonance is shown near the bottom of Fig. 1 at energy = —0.092 MeV The resonance would likely not occur without an assumed hyperfine,ultrafine energy-level structure present in the nucleus excitation structure, as described below. The excited pp + pp + nn + nn nucleus is metastable because of symmetry mismatches between the pp + pp + nn + nn nucleus and both the 2a-dimer and 2-free alpha configurations. The transition remains reversible, however, until energy is transferred to the metal lattice. The assumed hyperfine, ultrafine excitation structure is caused by the Bloch configuration of the nucleus as embedded in the lattice. Chubb 4 has pointed out that deuterons in a band state "can 'move' in response to externally applied electromagnetic fields... and can 'bond'... to a host in unusual ways... These bonding features can induce vibrations (previously identified as phonons)..." This identification of ion band state occupations with lattice modes suggests that the coherent partitioning of an interstitial nucleus into a Bloch nucleus is accompanied by creation of an additional 3 ATweii degrees of freedom. These new degrees of freedom support phonon modes which split each vibration,rotation excitation into 3 Nwe\\ excitation levels, which we call Bloch nucleus phonon modes. The separation between hyperfine levels includes very small energy differences, as occurs with acoustic phonons. Phonon oscillations orthogonal to the symmetry plane of a flake nucleus, also out-of-plane structure distortions, likely involve small energy differences. Furthermore, free floating flakes likely have out-of-plane vibration modes associated with each of the 2 iVweii Bloch in-plane iondensity maxima. The out-of-plane vibrations apply to each of the in-plane phonon modes, creating a set of ultrafine levels on top of the hyperfine excitation system. But with attached flakes and embedded Bloch nuclei the out-of-plane vibrations remain phonons. At the lower frequencies nucleus acoustic modes would be coupled to metal-lattice acoustic phonon modes. At the higher frequencies nucleus acoustic and optical phonons likely transfer energy to lattice phonons only under resonance conditions. The splitting of vibration,rotation levels into hyperfine levels with ultrafine substructure is represented by the black strips in Fig. 1. 6. F - P Fusion In Fig. 2, the above concepts are applied to F - P deuteron fusion, where there are two nucleus configurations of product 4HeB~J~och, designated dd-dimer and nn + pp. The Bloch nucleus exists as a subsystem embedded in the metal lattice. It has its own phonon spectrum which describes lattice degrees of freedom not present in the non-partitioned nucleus. Experimental evidence for such a subsystem has been reported by Chernov et al.6 With respect to F - P fusion, each of the phonon modes of the two Bloch nucleus configurations is an independent 4 He B | o c h quantum state. The hyperfine, ultrafine splitting of the nucleus vibration,rotation levels is assumed to bring the difference between adjacent excitation energy levels into resonance with metal-lattice phonons. It may be that energy transfer from an excited state Bloch nucleus to the metal lattice is aided by phonon-stimulated nucleus de-excitation.
692 3433-
.pp + n + n .pp + nn
28. 2726-
.p+p+n+n p + p + nn . D+ + D+
24Bloch phonon hyperfine levels
initial dd-dirrjer
pp + nn models ovalshape vibration-excited levels
:'?X dd-diameter ovalshape vibration-excited levels •0+
W+
4 H e 2+ Bloch
y
-0+ N
well = 8264
A/ we i| = 1
Figure 2. F - P cold fusion model. The 4 He 2 + nucleus occurs in two or more configurations. The red ladders show vibration,rotation energy levels for a d + d nucleus configuration, designated pn + pn. The green ladders show excitation levels for a pp + nn configuration. A Feshbach resonance converts 2-Dg l o c h (D+ + D+) to pn + pn at an excited level 24MeV above aeioch- A second resonance converts a pn + pn configuration to a pp + nn configuration. A sequence of resonances between metal lattice phonons and nucleus-phonon hyperfine excitation steps transfers energy from 4 H e B j o c h nucleus to metal in a de-excitation cascade. Both pn + pn and pp + nn configurations are expected to be Bloch sensitive. A third configuration change (not shown), presumably involving an isotopic spin interaction, may be needed to transition the nucleus to a final ctBioch ground state configuration.
A metal phonon in resonance with a dd-dimer or pp + nn hyperfine transition then stimulates a de-excitation transition in the nucleus, with the metal phonon mode receiving energy in the process. If the metal phonon mode involved is sufficiently de-coupled from the electron lattice, phonon lasering might be possible. The acoustic spikes observed by Chernov et al. might support this view. In any case, the non-thermal augmented phonon population would subsequently exchange energy with the lattice, heating the metal. Repeated phonon-mode transitions lower the energy of the Bloch nucleus to that of its non-partitioned ground state. A normal single-well helium ion is "created" at the boundary of the coherence volume. In this view a sequence of phonon transitions is what heats the metal.
693
References 1. Y. Iwamura, M. Sakano and T. Itoh, Elemental analysis of Pd complexes: effects of D2 gas permeation, Jpn. J. Appl. Phys. 4 1 , 4642 (2002). 2. R.A. Oriani and J.C. Fisher, Energetic charge particles produced in the gas phase by electrolysis, Proc. ICCF10, to appear (2004). 3. K. Heyde, Basic Ideas and Concepts in Nuclear Physics (Institute of Physics Publishing, Bristol and Philadelphia, 1994). pp. 54, 299-323. 4. S.R. Chubb, Nuts and bolts of ion band state theory, in Proceedings of the ICCF10 (World Scientific, 2005), in press, p. 3 ofwww.lenrcanr.org/acrobat/ChubbSR -nutsandbol.pdf. 5. X.Z. Li, M.Y. Mei, J. Tian, D.X. Cao and C.X. Li, Coherence in cold and hot fusion, ICCF8, Conference Proceedings. Vol. 70, Editor, F. Scaramuzzi (SIF, Bologna, 2000) p. 357; X.Z. Li, Fusion Sci. Technol. 4 1 , 83 (2002); X.Z. Li, B. Liu, S. Chen, M.W. Wei and H. Hora, Laser and Particle Beams Vol. 22:4 (Cambridge University Press, UK, 2004) p. 469. 6. LP. Chernov, Y.P. Cherndantzev, A.M. Lider and G.V. Garanin, Excess heat released upon hydrogen isotopes electrolytical saturation into metals covered by porous film, in Proceedings of the 8th Russian Conference on Cold Nuclear Transmutation of Chemical Elements, 2001, p. 133.
THEORETICAL S T U D Y OF N U C L E A R R E A C T I O N S I N D U C E D B Y BOSE-EINSTEIN CONDENSATION IN Pd
KEN-ICHI TSUCHIYA AND HIRAKU OKUMURA Department
of Chemical Science and Engineering, Tokyo National College of 1220-2 Kunugida, Hachioji, Tokyo 193-0997, Japan E-mail: tsuchiyaQtokyo-ct.ac.jp
Technology,
The purpose of this study is to give a theoretical explanation for the mechanism of cold fusion. In the beginning, a Bose—Einstein condensation (BEC) in solid is considered and introduced into our theory because deuterons are highly condensed at defects in some metals. Using the Kim-Zubarev theory, the wave function, the DD fusion rate of condensed deuterons in crystalline solid and critical temperature T c of BEC are obtained. Furthermore, by solving the equations of thermal conduction, the temperature around the reaction center as a function of position and time is obtained. The calculated results show that temperature falls lower than Tc and leads to the initial temperature earlier than the inverse of the reaction rate. This means that continuous reactions do not produce any explosions.
1. Introduction Over the past few years, several theoretical studies have been made on the condensed states of deuterons in metal. For example, deuteron cluster fusion was pointed out by Takahashi. 1 In our previous work, we also pointed out nuclear reactions are induced by condensed deuterons in Pd. 2 If many deuterons are accumulated in metal and the local density of the deuterons at lattice defects becomes high enough, BEC may form and induce nuclear reactions when T < Tc. In this work, nuclear reactions in Pd induced by BEC are estimated theoretically. The Kim-Zubarev theory 3 ' 4 is applied to calculate the condensed states of deuterons in Pd. The thermal conduction is estimated using Fourier analysis. 2. Application of Kim—Zubarev Method to the Phenomenon in Solid Quantum states of deuteron clusters trapped at a void in Pd are calculated by applying Kim-Zubarev theory. 3 ' 4 We start to show an outline of Kim-Zubarev method. They assumed the potential for the ion trap device as an isotropic harmonic potential. Then the Hamiltonian of the system including N charged particle in the ion trap is
2 m ^
'
2
^ i=l
i—1
694
-^rj-r,i<j
J
695
where m is the rest mass of the particle and r* is the position of an ion. They used ELTB method, which is based on the variational principle. The ground state of this many-body problem is written as
*(ri,r 2 ,...,r^)^ (3 t ( _ P 1)/2 ,
(2)
where new quantity p is defined as 1/2
(3) =1
The wave function in Eq. (2) satisfies n' d\^P+rr^ 2m dp2 2m p2
+
q^
)=E(Kp)t
(4)
where p and q are defined as _ (3JV-l)(3JV-3) p _
;
g
_
2JVr(gf) /o,w_^\ 3V27rr ( s ^ ) —
(5)
•
It is easy to see that the third term in Eq. (4) corresponds to the second term in Eq. (1). The first and second terms correspond to the first term in Eq. (1). The fourth term in Eq. (4) corresponds to the third term in Eq. (1). The exact proofs of them are given in Kim-Zubarev paper. 3 For example, the fourth term in Eq. (4) is derived by transforming the summation of two body potentials Y,i<jVij into p space. This is done by using
D / d R / d O u .*j
where integrals for R and tt mean integral over all space for gravity center of TV-body and integrals for 3(N— l)-angle, respectively. This is reduced to V(p)=
N(N - 1)T (^-) f^P / ( . 'J \ 2 > / drr2v(r)(l-^)
r2 \ ( 3Ar - 5 )/ 2 •
(7)
The fourth term in Eq. (4) is derived by substituting v(r) = e2/r into Eq. (7). Generally, these differential equations for harmonic oscillators are rewritten by using non-dimensional quantities x = yj^p and e = 2E/hu>. As a result, Eq. (4) is rewritten as d
da;2
' z2 + 4x2 + -W)=£<Xz). x*
x
(8)
In this equation qt are given by qf = 2aq^/mc2/hui, where a = e 2 /he is the fine structure constant. Here, we show the application of Kim-Zubarev method to the
696
phenomenon in solid. The Hamiltonian of a system including N deuterons in fee Pd lattice is written as rr _
^ V " V72 | V "
Ze2
exp(-K\Rj
- r f |)
e2 exp(-fc| r i -
^
rj -|)
where Rj is the Bravais lattice vector of the host lattice and Z is the effective charge of a host ion. In Eqs. (4) and (8) of Kim-Zubarev theory, harmonic term is the electromagnetically induced attractive potential in the ion trap device. For the case of the problems in crystalline solids, this term corresponds to the repulsive interaction between positively charged host ions and positively charged impurity deuterons. The second term of Eq. (9) has a same role with the harmonic term in Eqs. (4) and (8). The second and third terms of Eq. (9) should be transformed into p space. If we define new function u as
^) = E Z e 2 e " ^ r " .
do)
the transformation of the second term in Eq. (9) into p space is written as E/dR/dfiU(ri) U
^ =
'
JdR/d^
(n>
'
where r» means the position of a deuteron. Almost all the parts of the multiple integrations are cancelled between the numerator and the denominator in Eq. (11) and it is reduced to U(p) = w
N- ^
M l
v r(^) -* '
1
fP
I / —
/
drrz
27rr(f)r(3(N-i)\p3-/o
„2 \ (3iV-5)/2
1 - -^
I(r),
p2J
\
w
'
(12) K
'
where the function I(r) for rj Rj is defined as J
I(r)= I du suit) / aj —~-—• (13) Expanding the function l(r) into the power of Kr and substituting it into Eq. (12), Jo Jo Kr *-f U(p) is rewritten as oo
U(p) = ^mto2 J2 AN,mP2m'2 + U0,
(14)
m=2
where the constant term UQ can be omitted by selecting the origin of the energy at UQ. In this equation, the frequency UJ is defined as 1 2 -mw = 2
Ze2K2^e~KR> > —-—, 3! ^ Rj ' ;—
3
J
(15) y '
where Rj is the norm of the Bravais lattice vector R j . The structure of the host lattice is introduced thorough this equation. For example, the value of ui for perfect lattice is larger than that for the lattice including vacancies because vacant points
697
are omitted from the lattice summation in Eq. (15). The coefficients Ajv,mform > 2 are defined as if 2 m - 4 (3iV)!! (16) Nm m ' ~ 2 -2( T O -l)!(3iV + 2 m - 4 ) ! ! ' If we cut the summation in Eq. (14) at m = 2, then U(p) = mw2p2/2 is obtained. This means that U{p) in rough approximation is consistent with the third term in Eq. (1) of Kim-Zubarev theory. The transformation of the third term in Eq. (4) into p space is done by substituting v(r) = e 2 exp(-£x)/r into Eq. (7). The result is not similar to the fourth term in Eq. (4) because of the existence of the screening factor. In p space, effects of screening are described by the screening function for Thomas-Fermi potential, which is written as TT/2
/TF(P) = 3 ( J V - 1 )
f d0sm6cos3N-40exp(-kV2psin6). o
(17)
For the case of Coulomb potential with k = 0, we obtain /TF{P) = 1 which is consistent with fourth term in Eq. (4) of Kim-Zubarev theory. For the case of screened Coulomb potential with k ^ 0, we obtain Vk(p) = Vo(p) JTF(P)- Therefore, if we transform Eq. (9) into x space, it is written as
' ^^ + ^ + z /TF (\l^X) } ^ = * ) ' ^ where M is the cut-off of the summation for m. For the case of M = 2 and k = 0, it is completely consistent with Eq. (8) of Kim-Zubarev theory. In practice, M should be selected to keep required accuracy. Hence anharmonic terms are included in Eq. (18). The coefficient A'N m in Eq. (18) is defined as A'n,m = {h/muj)m~ ^4jv,m- Non-linear screened DD interactions are also tried instead of Thomas-Fermi interaction in Eq. (17). 5 ' 6 The octahedral void, which is defined in Fig. 1, is adopted as an ion trap in fee Pd. The calculated results are plotted in Figs. 2 and 3. 3. Nuclear Reaction Rate and Critical Temperature of BEC The ground state wave function ^ for N identical charged Bose nuclei gives the nuclear reaction rate as 2£i<,-(*|ImV£|tt) * = M*|tt) •
(19)
where imaginary part of Fermi pseudopotential V? [3] is written as JmV^-^Sin-rj).
(20)
The short-range interactions of nuclear forces between two Bose nuclei are introduced by using 5 function.3 This rate can be calculated by using numerical solution
698
Figure 1. The structure of VacO in fee lattice. The black and gray circles mean occupied and unoccupied lattice points, respectively. These defects construct octahedral void, which is called VacO in this paper.
of Eq. (18), because <j> gives * . It is written as AN{N - l ) r ( ^ ) ( ^ f ) 3 / 2 J dx2(x)/x3 R
27r3/2r
(21)
(3(iVpl))
where constant A is given by Bohr radius r B = h2/me2 and the S factor of the nuclear reaction between two nuclei as A = ISr-sl^h. If the ELTB solution is obtained, the critical temperature Tc of BEC is estimated by well-known formula, which is written as 2/3
Tr = ^ - ^ 2nmkB
[-^r I VC(|)
,
(22)
Total
,lvF(x)[--
"---.
••y?
qi?x
pl>?
10
20
30
40
x
Figure 2. The ELTB solution for the system including five deuterons in VacO in fee Pd. T h o m a s Fermi screening potential is used as the d-d interaction. The non-dimensional quantity x is defined as x = y/muj/h p, where w = 0.86 X 10 1 4 s _ 1 . The screening constant is defined as k = l/(2iJ c [ < j), where R^d (=0.74 A) is the d-d separation of D2 molecule. The solid line means the ELTB solution. The dashed lines mean each potential in Eq. (18) normalized by |e| = 1326.
699 2r
I I I
IvMl 2
::::
2
i plx
(\
A
1 1
V
~- .
1 --<
\- - H , . \ , - - - "
5 \
v
y%
•- . ' .
*
.
Total 20
' y'.-''' -1 -
Qf/x
"---'
Figure 3. The ELTB solution for the system including five deuterons in VacO in fee Pd. Nonlinear screening potential is used as the d—d interaction. The nondimensional quantity x is defined as x = ^/muj/h p, where ui = 0.86 x 1 0 1 4 s - 1 . The solid line means the ELTB solution, The dashed lines mean each potential in Eq. (18) normalized by |e| = |—409|.
where n is the number density of Bose particles and ((z) is the Riemann's zeta function. This temperature gives probability of the ground-state occupation. It is written as / j , x 2/3
n = l-
(-)
for T < Tc.
(23)
If we account the ground state occupation for T < Tc, the fusion rate is given by -RJ1 When T > Tc, no nuclear reactions have happened because fl = 0. Table 1. Nuclear reaction rate R ( 1 0 7 s - 1 ) and critical temperatureTc (K) for the case of N trapped deuterons in VacO in Pd. Thomas—Fermi screening N
Tc
R
3 4 5 6 7
56 66 76 86 95
2.1 3.5 5.0 6.7 8.6
Non-linear screening R 257 329 403 480 558
33.8 66.4 108.6 160.2 221.3
4. Thermal Conduction If nuclear reactions happen in solids, heat generated from the reaction center is diffused. In this study, thermal conduction from the center of a DD reaction in Pd is estimated. It is described by 3T -g^=kV2T, (24)
700
where T and t mean temperature and time, respectively. In this equation, the constant k is defined as
k = §-p,
(25)
where K, C, and p are the mean thermal conductivity, specific heat, and density of the solid, respectively. The origin of the temperature is selected as the equivalent value. The initial condition used for solving Eq. (24) is described as following. When t = 0, temperature is uniformly TQ inside of d x d x d cubic including the center of a DD reaction and uniformly zero outside of the cubic. The constant d is given by d = (volume of the defect) 1 / 3 . The initial temperature is obtained by
To
= cio'
(26)
where E and MQ mean energy generated from a DD reaction and number of moles in the d x d x d cubic, respectively. The boundary condition used for solving Eq. (24) is described as following. Assuming periodic L x L x L cubic, the solution expanded into the Fourier series can be obtained. The value of L is given by
where w means vacancy formation energy. The constants used for this calculation are shown in Table 2. The calculated results are plotted in Fig. 4a and b. Table 2.
The constants used for the calculations.
Name of the constant K; thermal conductivity C; specific heat pg; density E; energy generated from a DD reaction w\ vacancy formation energy L; parameter for periodicity
Value 75.5 ( J / s m K ) 25 ( J / m o l K ) 12.0 (g/cm 3 ) = 12.0 X 10 6 /166.4 (mol/m 3 ) 23.8 (MeV) = 23.8 X 10 6 x 1.60 x 1 0 " 1 9 (J) 1 (eV) 9 . 7 x l 0 5 (A)
5. Results and Discussions Results for the critical temperature and the reaction rate are shown in Table 1. For the case of Thomas-Fermi DD interaction, T c 's are lower than the room temperature. For the case of non-linear screened DD interactions, they are higher than room temperature. This means that DD reactions in Pd in room temperature are possible. Seeing Fig. 4a and b, we can see the rapid temperature relaxation from the initial state. Within 10 _ 1 0 s, the temperature outside of the d X d x d cubic is reduced to the initial value. The reaction rate shown in Table 1 for N = 5 with non-linear
701
0.0 \° Figure 4. (a) Thermal conduction from the center of the a DD reaction. Distance from a reaction center is normalized by d. The origin of the temperature is selected as the equivalent value, (b) The same surface view with Fig. 4(a) from another direction.
screening is 1 0 9 s - 1 . This means that temperature reduces lower than Tc and lead to the initial value earlier than the inverse of the reaction rate. This means that a continuous reaction will not produce thermal explosions. If the number of deuteron clusters is very large, recovery from the initial temperature is not so rapid. However, if the temperature is higher than Tc, probability of the ground state occupation fl becomes zero. And the reaction will not continue. From what has been discussed above, we can conclude that continuous but cold 1)1) reactions arc possible in I'd in room leinporaturc.
702
Acknowledgements T h e authors wish to t h a n k Dr. discussions.
Y. Iwamura and Dr.
M. Fukuhara for helpful
References 1. A. Takahashi, Mechanism of deuteron cluster fusion by EQPET model, in Proceedings of the ICCF10 (Boston, MA, USA, 2003), http://www.lenrcanr.org/Collections/ICCF10.htm 2. K. Tsuchiya, Quantum states of deuterons in Pd, Int. J. Hydrogen Energy 29, 1513 (2004). 3. Y.E. Kim and A.L. Zubarev, Nuclear fusion for bose nuclei confined in ion trap, Fusion Technol. 37, 151 (2000). 4. Y.E. Kim and A.L. Zubalev, Equivalent linear two-body method for many-body problems, J. Phys. B: Atomic, Mol. Opt. Phys. 33, 3905 (2000). 5. H. Hohenberg and W. Kohn, Inhomogeneous electron gas, Phys. Rev. 136, B864 (1964). 6. W. Kohn and L.J. Sham, Self-consistent equations including exchange and correlation effects, Phys. Rev. 140, A1133 (1965).
P R O P O S A L FOR N E W E X P E R I M E N T A L TESTS OF T H E BOSE EINSTEIN C O N D E N S A T I O N M E C H A N I S M FOR LOW-ENERGY N U C L E A R R E A C T I O N A N D T R A N S M U T A T I O N PROCESSES IN D E U T E R I U M LOADED MICRO- A N D N A N O - S C A L E CAVITIES
Y E O N G E. K I M , DAVID S. K O L T I C K , R O N A L D G. R E I F E N B E R G E R , A N D A L E X A N D E R L. Z U B A R E V Department of Physics, Purdue West Lafayette, IN 47907,
University USA
Most of experimental results of low-energy nuclear reaction (LENR) reported so far cannot be reproduced on demand. There have been persistent experimental results indicating that the LENR and transmutation processes in condensed matters (LENRTPCM) are surface phenomena rather than bulk phenomena. Recently proposed Bose-Einstein condensation (BEC) mechanism may provide a suitable theoretical description of the surface phenomena. New experiments are proposed and described for testing the BEC mechanism for LENR and transmutation processes in micro- and nano-scale traps. (1) We propose the use of micro- or nanoporous conducting materials as a cathode in electrolysis experiments with heavy water with or without Li in order to stabilize the active surface spots and to enhance the effect for the purpose of improving the reproducibility of excess heat generation and nuclear emission. (2) We propose new experimental tests of the BEC mechanism by measuring the pressure and temperature dependence of LENR events using deuterium gas and these deuterated metals with or without Li. If the LENRTPCM are surface phenomena, the proposed use of micro-/nano-scale porous materials is expected to enhance and scale up the LENRTPCM effects by many order of magnitude, and thus may lead to better reproductivity and theoretical understanding of the phenomena.
1. Introduction There have been many reports of experimental evidences for low-energy nuclear reaction (LENR) processes in condensed matters as documented in a recent review document submitted for a DOE review1 and as reported in the Proceedings of the ICCF-10.2 However, most of experimental results cannot be reproduced on demand. This difficulty appears to be mainly due to (1) the complexities of the experimental set-ups involving many materials (including impurities), (2) numerous variation of experimental input parameters, and (3) the reported results are small effects. This situation has prevented us from development of a coherent theoretical understanding or working theoretical model of the phenomenon which can be used to guide us in carrying out new experimental tests to sort out essential parameters and controls needed to achieve reproducibility on demand (ROD). In this paper, we propose such 703
704
experimental tests based on a theoretical model of the Bose-Einstein condensation (BEC) mechanism. 2. Experimental Status: Surface versus Bulk There have been persistent discussions of whether LENR processes in condensed matters are surface phenomena (SP) occurring in the surface regions or bulk phenomenon (BP) in the bulk of the deuterated metals. 3 " 7 There are now many experimental results supporting the surface phenomena scenario as documented by Storms. 6 The enhancement of excess power using laser stimulations that have been observed in electrolysis experiments 7 suggests that the process is due to surface phenomena. The most recent experimental evidence supporting the SP scenario comes from experiments performed by Szpak et al.8'9 in which a Ni wire mesh cathode is immersed in an electrolyte consisting of the heavy water, LiO, and PdCl2. Excess heat was observed without bulk metals in three experiments. If the LENR and transmutation processes in condensed matters turn out to be a surface phenomena, the BEC mechanism may provide a suitable theoretical frame work to explain the phenomena. Furthermore, the use of micro-/nano-scale porous materials is expected to enhance the phenomena by many order of magnitude, thus providing better ROD and theoretical understanding of the phenomena. 3. Predictions of the B E C Mechanism Theoretical studies of the BEC mechanism have been carried out using an approximate solution to the many-body Schroedinger equation for a system of N identical charged, integer-spin nuclei ("Bose" nuclei) confined in ion traps. 10 ~ 13 The groundstate solution is used to obtain theoretical formulae for estimating the probabilities and rates of nuclear fusion for N identical Bose nuclei confined in an ion trap or an atomic cluster. One of the main predictions is that the Coulomb interaction between two charged bosons may be suppressed for the large N case and hence the conventional Gamow factor may be absent. The theory has been used to analyze LENR experiments involving both atomic clusters (Pd black powders 14 ) and acoustic cavitations. 15 Recently, the one-specie LENR theory of the BEC mechanism 10-13 used for reactions such as (D + D) has been generalized to the two-species case and applied to (D + Li) reactions. 16 In this section, we summarize the results and predictions of two-species BEC mechanism for LENR and the transmutation processes.16
3.1. Effective
Temperature
Dependence
The only unknown parameter of the theory is the probability of the BEC groundstate occupation, fl. Since f2 is expected to increase as the effective temperature of the BEC decreases, the nuclear reaction rates for the BEC mechanism are expected to increase at lower temperatures.
705
3.2. Selection
Rules
There are two selection rules found from the theory for the BEC mechanism when applied to LENR and the transmutation process. (1) Nuclear spin selection rule and (2) nuclear mass-charge selection rule. (1) The nuclear spin selection rule. The nuclear spins of both species must be integer. This rule is obvious for the BEC mechanism. (2) The nuclear mass-charge selection rule. This approximate selection rule is given by the following relation: Z1 __ rrn _ Zx + N\ Z2 m2 Z2+ iV2' where Ni is the number of neutrons in the Bose nucleus for the specie i. We note that the above relation is satisfied, for example, for two species with Zi = N. 3.3. Fusion
Rates
For the two species case, the short-range nuclear interaction is approximated by a Fermi pseudo-potential 10 and takes the generalized form:
where the nuclear reaction rate constants A^ are given by (no sum over i and j implied) Aij
2
~
TTh
2
with re = h /2^,ijZiZje and u%j = rriimj/(rrii + rrij). Sij is the S'-factor for nuclear fusion between two nuclei of specie i and j . The nucleus-nucleus fusion rate is determined from the trapped ground state wave function \I/ as
i<j 2
Ni
N2
i=\
j=l
i<j
and in the mean-field approximation, we have Rn = AnNinf /2, R\2 = A\2Nin^, and R22 = A22N2nf/2, where nf = ATj/(4/3)7ri?f. Ni is the total number of specie i, and Ri is the radius of the trap for specie i.
706
If the probabilities of the mean-field ground state occupation, 10 fli, are taken into account, the trap fusion rates are given by R^ = f2ii?n,.R| 2 = ^2-^221 and R\2 — QzRi2- We expect that O3 w-y/^1^23.4. Application
to (D + Li)
Reactions
For the reaction 6 Li(d,a) 4 He (Q = 22.37Mev) and the reaction, 7 Li(d,n)2 4 He (Q = 15.12Mev), the ^-factors are 18.8Mev-barn 17 ' 18 and 30Mev-barn, 19 respectively (see Tables 1 and 2). Using these values the corresponding nuclear reaction rate constants are found to be Ad&u « 5.8 x 10~ 15 cm 3 /s and A d 7 Li « 8.97 x 10~ 15 cm 3 /s which are about 50 times larger than the d-d nuclear reaction rate constant A d d ~ 1.5 x 1 0 - 1 6 c m 3 / s . Table 1. (D -f 6 Li) reactions with positive Q-values and extrapolated 5-factors at E = 0. Reaction
Q- value (MeV)
S (MeV-barn)
6
22.37 0.59 1.80 2.56 3.38 5.03 22.27
18.8, 17 16.9, 18 18.7 : No data No data No data No data No data No data
Li(d,a) 4 He Li(d,t) s Li 6 Li(d,an) 3 He 6 Li(d,ap) 3 H 6 Li(d,n) 7 Be 6 Li(d,p) 7 Li 6 Li(d,7) 8 Be 6
Table 2. (D + 7 Li) reactions with positive Q-values and extrapolated S-factors at E = 0. Reaction 7
4
Li(d,n)2 He Li(d,a) 5 He 7 Li(d,n) 8 Be 7
Q-value (MeV)
S (MeV-barn)
15.12 14.23 15.03
30 ± 6 1 9 No data No data
We expect that the nuclear reaction rate constants for 6 Li( 6 Li, 5 Li) 7 Li (Q = 1.86 Mev) and 6 Li( 6 Li,a)2 4 He (Q = 20.897Mev) are much smaller than A d 6 Li . If the (D + 7 Li) reaction rate is controlled by the BEC mechanism then it is expected to be suppressed relative to the (D + 6 Li) reaction rate due to selection rule (1). This is consistent with the Arata-Zhang experiments 22-25 which report a depletion of 6 Li, 2 0 ' 2 1 inferred from the increased 7 Li/ 6 Li abundance ratio found from observations of particulate Pd exposed to deuterium gas. 2 2 - 2 5 The excess heat and 4 He observed in electrolysis experiments 22-25 may be due to the reaction 6 Li(d,a) 4 He in addition to other reactions leading to final states without 4 He (see Tables 1 and 2). This would be an alternative scenario to the (D + D) reaction scenario which has been proposed by many other authors. 1
707
4. Proposed Experiments Recent advances in nanotechnology have produced a variety of novel materials that exhibit well-defined features with nanometer-scale dimensions. We propose a number of experiments well suited to utilize for the micro- or nano-scale cavities in porous vycor glass, 26 aerogel,27 nanogel (aerogel bead of a few mm diameter), 28 and ordered nanoporous thin films.29 Porous vycor glass, aerogel, and nanogel have interconnecting cavities or pores with average pore diameter of ~10nm. After saturating these materials with deuterium gas, heavy water, or other deuterated materials, and stimulating them with lasers, electromagnetic fields, or acoustic waves or other energy sources, these special materials may readily illustrate LENR phenomena. The experimental signatures (nuclear emissions, fast neutrons, etc.) in these porous materials 2 6 - 2 9 as well as in electrically conducting carbon aerogels30 and "pocofoam"31 may enhance LENR and allow them to be studied as a function of pressure and temperature. For ordered nanoporous thin films,29 substantial effort is currently directed at developing better control of their composition and structure. Unlike many materials that have broad pore size distributions and poorly defined pores, the ordered nanoporous films now being investigated currently have pores of well-defined size, geometry, connectivity, and orientation. Pore diameter is precisely controlled and tuned to range from 2 nm to over 30 nm using a variety of synthesis chemistries that employ solution phase self-assembly.32 Because of this precise control of the pore diameter, ordered nanoporous thin films are ideal materials to study the pore size dependence for our new proposed experiments to illustrate LENR. Additional flexibility is possible because nanoporous thin films can be synthesized by dip coating and spin coating to yield nanoporous insulating silica,33 wide band gap semiconducting titania, tin oxide,34 and carbon 35 structures. We propose to use micro- or nano-pourous materials in the following types of experiments:
(1) (2) (3) (4) (5)
electrolysis experiements of Fleischman-Pons, 1 ' 2 ' 6 ' 8 ' 2 5 , 3 7 - 4 0 gas experiments, 14 - 22 ' 23 ' 24 ' 41 nuclear emission experiments, 42 ' 43 transient acoustic cavitation experiments, 44 deutreon beam experiments. 45 ' 46
The micro- or nano-porous materials that will be studied include: vycor glasses,26 aerogels,27 nanogels, 28 ordered nanoporous thin films,29 carbon arerogels,30 and pocofoams.31 In all of the proposed experiments the possibility of (D + Li) reactions in addition to (D + D) reactions should be investigated by using 6 Li and 7 Li separately in experiments, as tests of the predictions for the BEC mechanism described in Section 3.
708
5. S u m m a r y a n d C o n c l u s i o n s In most of the experiments reporting L E N R and transmution processes in condensed matters, low counting rates and lack of reproductability on demand are obstacles preventing the extraction of essential parameters and controls required for unequivical proof of L E N R phenomena. These difficulties in t u r n prevent a complete theoretical understanding of these processes. There are now many experimental indications t h a t these processes are surface p h e n o m e n a . 6 - 9 T h e recently proposed B E C m e c h a n i s m 1 0 - 1 4 may provide a suitable theoretical description of t h e surface phenomena. In order t o test the predictions of the B E C mechanism described in Section 3, we propose to use micro- or nano-porous m a t e r i a l s 2 6 - 3 1 in electrolysis e x p e r i m e n t s , 1 ' 2 ' 6 ' 8 ' 2 5 ' 3 7 - 4 0 gas e x p e r i m e n t s , 1 4 ' 2 2 - 2 4 ' 4 1 and nuclear emission experiments, 4 2 ' 4 3 transient acoustic cavitation experiments, 4 4 and deuteron beam experiments. 4 5 ' 4 6 T h e use of micro- or nano-porous materials in these experiments is expected to enhance the observed effect by many order of magnitude if the observed processes are surface phenomena. Because these materials have active surfaces substatically larger t h a n other materials when comparing their surface area of a bulk volume. This enhancement will help us t o overcome lack of reproducibility on demand and to develop a better theoretical understanding of the process.
References 1. P.L. Hagelstein, M.C. McKubre, D.J. Nagel, T.A. Chubb, and R.J. Hekman, New physical effects in metal deuterides, submitted to DOE for a review, July 2004, and references therin. This report was posted December 1, 2004 at the DOE website: http://www.sc.doe.gov 2. See experimental papers in the Proceedings of the 10 International Conference on Cold Fusion (ICCF-10) (Cambridge, MA, USA, 2003). 3. Y.E. Kim, Nuclear physics interpretation of cold fusion and optimal designs for gas/solid-state device, in Proceedings of the # Worlld Hydrogen Energy Conference, (Honolulu, HA, USA, 1990). 4. Y.E. Kim, Surface reaction mechanism and lepton screening for cold fusin with electrolysis, in Proceedings of the 1st Annual Conference on Cold Fusion (Salt Lake City, UT, USA, 1990). 5. Y.E. Kim, Surface reaction theory of cold and warm fusion, Anomalous nuclear effects in deuterium/solid systems, in AIP Conference Proceedings 228 (American Institute of Physics, NY, Provo, UT, 1990). 6. E. Storms, What conditions are required to initiate the LENR effect? in Proceedings of the ICCF-10 (Cambridge, MA, USA, 2003); E. Storms, Why cold fusion has been so hard to explain and duplicate, in The APS Conference, 3-7 March 2003 (Austin, TX, USA). 7. D. Letts and D. Cravens, Laser stimulation of deuterated palladium: past and present, in Proceedings of the ICCF-10 (Cambridge, MA, USA, 2003). 8. S. Szpak, P.A. Mosier-Boss, J. Dea, and F. Gordon, Polarized D + / P d - D 2 0 system: hot spots and 'mini-explosions', in Proceedings of the ICCF-10 (Cambridge, MA, USA, 2003). 9. S. Szpak, P.A. Mosier-Boss, M.H. Miles, and M. Fleischmann, Thermal behavior of
709
10. 11. 12. 13. 14. 15. 16.
17. 18. 19. 20. 21. 22. 23. 24. 25. 26. 27. 28. 29.
30. 31. 32.
33.
34. 35. 36.
polarized P d / D electrodes prepared by co-deposition, Thermochim. Acta 410, 101 (2004). Y.E. Kim and A.L. Zubarev, Fusion Technol. 37, 151 (2000). Y.E. Kim and A.L. Zubarev, Ultra low-energy nuclear fusion of Bose nuclei in nanoscale ion traps, Ital. Phys. Soc. Proc. 70, 375 (2000); Proceedings of the ICCF-8, 2000. Y.E. Kim and A.L. Zubarev, Phys. Rev. A64, 013603 (2001). Y.E. Kim, Prog. Theor. Phys. Suppl., 154, 379 (2004). Y.E. Kim, D.S. Koltick, R. Pringer, J. Myers, and R. Koltick, in Proceedings of the ICCF-10 (Cambridge, MA, USA, 2003). Y.E. Kim, D.S. Koltick, and A.L. Zubarev, in Proceedings of the ICCF-10 (Cambridge, MA, USA, 2003). Y.E. Kim and A.L. Zubarev, Mixture of charged bosons confined in harmonic traps and bose-einstein condensation mechanism for low energy nuclear reactions and transmutaion processess in condensed matters, in Proceedings of the ICCF-11 (Marseille, France, 2004). S. Engstler et al, Z. Phys. A 342, 471 (1992). A. Musumara et al, Phys. Rev. C64, 068801 (2001). J. Yan et al, Nucl. Phys. A 621, 127c (1997). T.O. Passell, in Proceedings of the 9th International Conference on Cold Fusion, 19-24 May 2002, Beijing, pp. 299-304. T.O. Passell, in Proceedings of the 10th International Conference on Cold Fusion (Cambridge, MA, USA, 2003). Y. Arata and Y.C. Zhang, Ital. Phys. Soc. Proc. 70, 11 (2000); Proceedings of the ICCF-8, (Lerici (La Spezia), Italy, 2000) Y. Arata and Y.C. Zhang, Jpn. J. Appl. Phys. 37, L1274 (1998). Y. Arata and Y.C. Zhang, Jpn. J. Appl. Phys. 38, L774 (1999). M. McKubre et al, Ital. Phys. Soc. Proc. 70, 3 (2000) ICCF-8 (Lerici (La Spezia), Italy, 2000). P. Levitz, G. Ehret, S.K. Sinha, and J.M. Drake, J. Chem. Phys. 95, 6151 (1991). J. Fricke and A. Emmerling, J. Sol-Gel Sci. Technol. 13, 299 (1998). http://www.cabot-corp.com. Laika Menon, Nanoarrays synthesized from porous alumina, Dekker Encyclopedia of Nanoscience and Nanotechnology (Marcel Dekker Inc., New York, NY, USA, 2004), pp. 2221-2238. R.W. Pekala, et al, in Y.A. Attia (ed.), Sol Gel Science and Applications (Plenum Press, NY, USA, 1994), p. 369. MRS Bulletin, December 2000, p. 10; http://www.pocofoam.com C.T. Kresge, M.E. Leonowicz, W.J. Roth, J.C. Vartuli, and J.S. Beck, Ordered mesoporous molecular-sieves synthesized by a liquid-crystal template mechanism, Nature 359(6397), 710-712 (1996). D.Y. Zhao, P.D. Yang, D.I. Margolese, B.F. Chmelka, and G.D. Stucky, Synthesis of continuous mesoporous silica thin films with three-dimensional accessible pore structures, Chem. Commun. 22 2499-2500 (1998). V.N. Urade and H.W. Hillhouse, Synthesis of the first thermally stable cubic phase nanoporous tin oxide thin films, Submitted (2004). B.Eggiman, D. Owens, V.N. Urade, M.P. Tate, and H.W. Hillhouse, Synthesis of mesoporous carbon thin films with long-range order. Submitted (2004). G. H. Miley, et al., Quanitative observations of transmutation products occuring in thin-film coated microspheres during electrolysis, in Proceedings of the 6th International Conference on Cold Fusion, Progress in new hydrogen energy (Lake Toya, Hokkaido, Japan, 1996); New Energy and Industrial Technology Development Orga-
710
37. 38.
39. 40. 41. 42. 43. 44.
45. 46.
nization (Tokyo Institute of Technology, Tokyo, Japan); Proceedings of the ICCF-10 (Cambridge, MA, 2003). D. Letts and D. Cravens, in Proceedings of the ICCF-10 (Cambridge, MA, USA, 2003). R.T. Bush and R.D. Eagleton. A Calorimetric study of the Excess heat effect in thin films of palladium, in Proceedings of the Second Annual Conference on Cold Fusion, The Science of Cold Fusion (Como, Italy, 1991): Societa Italiana di Fisica, Bologna, Italy. D.S. Silver, J. Dash, and P.S. Keefe, Surface topology of a palladium cathode after electroylsis in heavy water, Fusion Technol. 24, 423 (1993). L.C. Case, Fusion Technol. 20, 478 (1991); in Proceedings of the ICCF-6 (Vancouver, Canada, 1998). Y. Iwamura et al., Jpn. J Appl. Phys., 41, 4642 (2002); in Proceedings of the ICCF-10 (Cambridge, MA, USA, 2003). S.E. Jones, et al., Charged-particle emissions from metal deuterides, in Proceedings of the ICCF-10 (Cambridge, MA, USA, 2003). S.E. Jones, et al., Neutron emissions from metal deuterides, in Proceedings of the ICCF-10 (Cambridge, MA, USA, 2003). R.S. Stringham, in Proceedings of the IEEE Ultrasonics International Symposioum, Vol. 2 (Sendai, Japan, 1998), p. 1107; in Proceedings of the 7th International Conference on Cold Fusion (ICCF-7) (Vancouver BC Canada, 1990); Proceedings of the IDDF-8, May 21-26 (Villa Marigola, LaSpezia, Italy, 2000); Proceedings of the IDDF9, 323 (2002); Proceedings of the ICCF-10 (2003). J. Kasagi, Prog. Theor. Phys. Suppl. 154, 365 (2004). C. Rolfs, Prog. Theor. Phys. Suppl. 154, 373 (2004).
M I X T U R E S OF C H A R G E D B O S O N S C O N F I N E D IN H A R M O N I C TRAPS A N D BOSE-EINSTEIN CONDENSATION MECHANISM FOR LOW-ENERGY N U C L E A R R E A C T I O N S A N D T R A N S M U T A T I O N PROCESSES IN C O N D E N S E D M A T T E R S
Y E O N G E . K I M A N D A L E X A N D E R L. Z U B A R E V Purdue
Nuclear and Many-Body Theory Group (PNMBTG) Department of Physics, Purdue University West Lafayette, IN 47907, USA
A mixture of two different species of positively charged bosons in harmonic traps is considered in the mean-field approximation. It is shown that depending on the ratio of parameters, the two components may coexist in same regions of space, in spite of the Coulomb repulsion between the two species. Application of this result is discussed for the generalization of the Bose—Einstein condensation mechanism for low-energy nuclear reaction (LENR) and transmutation processes in condensed matters. For the case of deutron—lithium (d + Li) LENR, the result indicates that (d + Li) reactions may dominate over (d + d) reactions in LENR experiments.
1. Introduction In order to understand and explain the anomalous nuclear low-energy reaction phenomena, 1 Bose-Einstein condensation (BEC) of integer-spin nuclei was suggested as a possible mechanism for ultra low-energy nuclear reaction in 1998.2 Recently, theoretical studies of BEC mechanism have been carried out by approximately solving a many-body Schrodinger equation for a system of TV identical charged integer-spin nuclei ("Bose" nuclei) confined in ion traps. 3 ~ 7 The solution is used to obtain theoretical formulae for estimating the probabilities and rates of nuclear fusion for TV identical Bose nuclei confined in an ion trap or an atomic cluster. In this paper, we generalize our previous one specie BEC mechanism to the two-species case in order to apply our formulation to the LENR and transmutation processes in condensed matters. 8 ' 9 2. One Specie Case For the BEC mechanism, the total nuclear d-d fusion rate R^> per unit volume per unit time is given by 3 - 7 R& = nmP^QBa (—) NnB, (1) V 4-7T \fnJ where B is given by B = SAm/Bixahc, nB is a trap/cluster number density (number of traps/clusters per unit volume) as defined as, nB = NB/N,NB is the total 711
712
number of Bose nuclei in traps/clusters per unit volume, and TV is the average number of Bose nuclei in a trap/cluster, nB is an average number of Bose nuclei per trap/cluster, nB = N/{r)3, where (r) is the average size of traps/atomic clusters. A is given by A = 2STB/-KH, where rB = S2/2/xe2, n = m/2, S is the .S'-factor for the nuclear fusion reaction between two deutrons (for D(d,p)T and D(d,n) 3 He reactions, S « 55 keV-barn), and 17 is the probability of the BEC ground-state occupation. In terms of S'-factor, Eq. (1) can be rewritten as RM = nBriK {-]
NnB,
(2)
where K
3^3
1
d>-K2\f^KQ.C
We note a very important fact that R^1' does not depend on the Gamov factor in contrast to the conventional theory for nuclei fusion in free space. This is consistent with conjecture noted by Dirac 10 that each interacting neutral boson behaves as an independent particle in a common average background for the large N case. Furthermore, the reaction rate R^ is proportional to fl which is expected to increase as the operating temperature decreases. The only unknown parameter in Eqs. (1) and (2) is the probability of the BEC ground state occupation, fl. Our predictions imply that nuclear fusion may be achievable at lower temperatures. 3. Two Species Case We consider a mixture of two different species of positive charged bosons, labeled 1 and 2 with iVi and N2 particles, respectively. We denote charges and masses as Z\ > 0, Z2 > 0 and m\, mi-, respectively. We assume that trapping potentials Vi are isotropic and harmonic r2 Vi(f) =77liW 2 y. The mean-field energy functional for the two-component system is given by generalization of the one-component case5 2
E = y > i + Eint,
(3)
i=l
where
e2 f,^,^Zini(x) Emt = ^ dxdy
+ Z2n2{x))(Z1n1(y) x-y
+ Z2n2(y})
713 and m denotes density of species i, n* = \ipi\2, dfni(f)=Ni.
(4)
/ ' In Eq. (3), we have neglected effects of order 1/iVj. T h e minimization of the functional, Eq. (3), with subsidiary conditions, Eq. (4), leads to the following time-independent mean-field equations: " ^ - V 2 ^ ( f O + (Vi + Wi)rl>i(r) = /iiVi(r), zrrii
(5)
where Wi (f) = e2 Jdy[Z2n2(y)
+ Z1Z2n1(ff)n2(v)]/(\r-
j7Mi7)),
(6)
and ^ are the chemical potentials, which are related to the ground-state energy, Eq. (3), by the general thermodynamics identity _ dE We note t h a t t h e mean-field theory, Eq. (5), cannot describe t h e Wignercrystallization regime. 1 1 In the T h o m a s - F e r m i (TF) approximation, in which one neglects the kinetic energy t e r m s in Eq. (5), Eq. (5) reduce t o tH = Vi + Wi.
(7)
Equation (7) holds in t h e region where n* are positive a n d n* = 0 outside this region. We can obtain from these equations t h a t Z2
Z2\ miLO2
I'm2to2
M2 - ^ - MLi = I
Z^
2
2n - — I — : — r
\miuj
Zj
2
and hence we have proved t h a t Eq. (7) has non-trivial solution if and only if
In this case, we have /i2 =
A=^ miLj{Z2 {Z2jZ\)\i\.
= l.
(8)
Equation (7) can be solved analytically t o obtain n ^
=^ 9 ( R
2
- r
2
) ,
(9)
where 0 denotes the unit positive step function, Ri =\l —
hP(Z?N? + Z^NiN^/Ni}1'*,
rriiLOi
and
7c
V &* '
(10)
714
This is done by seeing that potentials Wj, Eq. (6) are solutions of the Poisson equations V2Wx(r)
= -Ane2[Z2ni{r)
+
Z1Z2n2{r)},
V2W2{r) = -47re 2 [Z 2 2 n 2 (f) +
ZxZ2nx{r)\.
Straightforward calculations with m from Eq. (9) yield 3 fli =
-TTliUlfR2,
and
E=^^hP]2/3[(Z2N1+Z1Z2N2 Comparing the radii of clouds i?i and R2, Eq. (10), we see that R\ — R2. Therefore, we have found that depending of the ratio A, Eq. (8), the two components coexist in the same region of space, in spite of the Coulomb repulsion between the two species. This result is obtained in the TF approximation, Eq. (7). If A = 1, and J V i > l , "fc Nj » 1, the TF approximation provides an accurate description of the exact mean-field solution (except a narrow region near a surface). For a general value of A, the mixture becomes unstable against deviations from uniformity. Although the TF approximation is not applicable for this case, we expect that if A PS 1 and Ni ^> 1, 7c iVj 3> 1, the two components may coexist in the same regions of space. 4. Fusion Rates For the two species case, we generalize the one-specie Fermi pseudo-potential 3 as
where the nuclear reaction rate constants Aij are given by
with 7JJ = H2/2fiijZiZje2 and //^ = mimj/(mi + rrij). Sij are the S'-factors for nuclear fusion between two nuclei from species i and j . The nucleus-nucleus fusion rates are determined from the trapped ground state wave function \P as i?
ii
==
2
Nl
-^E(*lImVi,i^-fi)l*)/
R
* = - H E E<*i Imy i F 2(^ - &)i*>/w*>> 11
i=X 3 = 1
715
R22 = - j j E W 1 1 1 1 ^ -J/j)l*>/<*l*>. i<j
and in the mean-field approximation, Eq. (9), we have Rn
= AuNwf/2,
R12 = A12Nin%,
R22 =
A22N2n%/2,
where
nf =
Ni/iA/^Rl
If the probabilities of the mean-field ground state occupation, 3 fij are taken into account, the trap fusion rates are given by Rw = f^i-Rn,
R22 = Q2R22>
R\2 = ^3^i2-
We expect that f^ w^/^i^25. Selection Rules For the BEC mechanism for LENR and transmutation processes, there are two selection rules: (A) nuclear spin selection rule and (B) nuclear mass-charge selection rule. (A) Nuclear spin selection rule: Nuclear spins of both species must be integer. This rule is obvious for the BEC mechanism. (B) Nuclear mass-charge selection rule: If we assume LO\ = UI2, we have from Eq. (8), A — m2Z\jm\Z2 = 1 or Z2
m2 ~ Z2 + N2 '
where Ni is the number of neutrons in the Bose nucleus for the specie i. We note that Eq. (11) is satisfied, for example, for two species with Zi = Ni. 6. Application to (D + Li) Reactions For (d + 6Li) reaction, 6 Li(d,a) 4 He (Q = 22.37 MeV) and for (d + 7Li) reaction, 7 Li(d,n)2 4 He (Q = 15.12MeV), the S-factors are 18.8MeV-barn 12 ' 13 and 30MeVbarn, 14 respectively. Using these values we find that the corresponding nuclear reaction rate constants are A-j6Li « 5.8 x 10~ 15 cm 3 /s and Ad7Li « 8.97 x 10 - 1 5 cm 3 /s which are about 50 times larger than the d-d nuclear reaction rate constant Add x 1.5 x l(T 1 6 cm 3 /s. We expect that nuclear reaction rate constants for reactions 6 Li( 6 Li, 5 Li) 7 Li (Q = 1.86MeV) and 6 Li( 6 Li,a)2 4 He (Q = 20.897MeV) are much smaller than For the BEC mechanism, the (d + 7Li) reaction rate is expected to be suppressed compared with the (d + 6 Li) reaction rate. This is consistent with the observation
716
of depletion of 6 L i 1 5 , 1 6 as inferred from increased 7 L i / 6 L i abundance ratio in A r a t a Zhang's particulate P d exposed to deuterium g a s . 1 7 - 2 0 T h e excess heat and 4 H e observed in electrolysis e x p e r i m e n t s 1 7 - 2 0 may be due 6 to Li(d,o:) 4 He in addition to other reactions leading to t h e final states without 4 He. This would be an alternative scenario to the (d + d) reaction scenario which has been proposed by many. 7. S u m m a r y a n d C o n c l u s i o n s A generalization of the B E C mechanism for one specie L E N R processes in condensed m a t t e r s has been made to the case of a mixture of two different species of positively charged Bose nuclei in harmonic traps. Depending on the ratio of the parameters involved, it is shown t h a t the two components may coexist in same regions of space, in spite of t h e Coulomb repulsion between two species. We have obtained an approximate selection rule involving nuclear masses and charges of two species. For a mixture d and Li species, we expect t h a t the (d + 6 Li) reaction rate may be larger t h a n the (d + d) reaction rate, implying t h a t the (d + 6 Li) reactions may dominate over the (d + d) reactions in L E N R experiments in condensed matters. This is consistent with the recent observation of the 6 Li depletion 1 5 ' 1 6 in particulate P d exposed to deuterium g a s . 1 7 - 2 0 Further L E N R experiments involving 6 Li or 7 Li separately are needed for more conclusive tests of the B E C mechanism with two species.
References 1. See the Proceedings of the 10th International Conference on Cold Fusion (ICCF-10) (Cambridge, MA, USA, 2003). 2. Y.E. Kim and A.L. Zubarev, in Proceedings of the ICCF-7, pp. 186-191 (1998). 3. Y.E. Kim and A.L. Zubarev, Fusion Technol. 37, 151 (2000). 4. Y.E. Kim and A.L. Zubarev, Ital. Phys. Soc. Proc. 70, 375 (2000); in Proceedings of the ICCF-8 (Lerici (La Spezia), Italy, 2000). 5. Y.E. Kim and A.L. Zubarev, Phys. Rev. A 64, 013603 (2001). 6. Y.E. Kim, D.S. Koltick, R. Pringer, J. Myers, and R. Koltick, in Proceedings of the ICCF-10 (Cambridge, MA, USA, 2003). 7. Y.E. Kim, Prog. Theor. Phys. Suppl. 154, 379 (2004). 8. G.H. Miley and P.J. Shrestha, in Proceedings of the ICCF-10 (Cambridge, MA, USA, 2003). 9. Y. Iwamura et al, in Proceedings of the ICCF-10 (Cambridge, MA, USA, 2003). 10. P.A.M. Dirac, The Principles of Quantum Mechanics, 2nd edn., Chapter XI, Section 62, (Clarendon Press, Oxford, 1935). 11. E.P. Wigner, Phys. Rev. 46, 1002 (1934). 12. S. Engstler et al., Z. Phys. A 342, 471 (1992). 13. A. Musumara et al, Phys. Rev. C 64, 068801 (2001). 14. J. Yan et al, Nucl. Phys. A 621, 127c (1997). 15. T.O. Passel, in Proceedings of the 9th International Conference on Cold Fusion, 19-24 May 2002 (Beijing, 2002), pp. 299-304. 16. T.O. Passel, in Proceedings of the 10th International Conference on Cold Fusion Cambridge, MA, USA, 2003.
717 17. Y. Arata and Y.C. Zhang, ltd. Phys. Soc. Proc. 70, 11 (2000); in Proceedings of the ICCF-8 (Lerici (La Spezia), Italy, 2000). 18. Y. Arata and Y.C. Zhang, Jpn. J. Appl. Phys. 37, L1274 (1998). 19. Y. Arata and Y.C. Zhang, Jpn. J. Appl. Phys. 38, L774 (1999). 20. M. McKubre et al, ltd. Phys. Soc. Proc. 70, 3 (2000); in Proceedings of the ICCF-8 (Lerici (La Spezia), Italy, 2000).
ALTERNATIVE I N T E R P R E T A T I O N OF LOW-ENERGY N U C L E A R R E A C T I O N PROCESSES W I T H D E U T E R A T E D METALS B A S E D ON T H E B O S E - E I N S T E I N C O N D E N S A T I O N M E C H A N I S M
Y E O N G E. KIM Department
of Physics,
Purdue
University,
West Lafayette,
IN 47907,
USA
T H O M A S O. P A S S E L L TOP Consulting,
P.O. Box 336, Palo Alto,
CA 94302-0336,
USA
Recently, a generalization of the Bose-Einstein condensation (BEC) mechanism has been made to a ground-state mixture of two different species of positively charged bosons in harmonic traps. The theory has been used to describe (D + Li) reactions in the low energy nuclear reaction (LENR) processes in condensed matter and predicts that the (D + Li) reaction rates can be larger than (D + D) reaction rates by as much as a factor of ~ 5 0 , implying that (D + Li) reactions may be occuring in addition to the (D + D) reactions. A survey of the existing data from LENR experiments is carried out to check the validity of the theoretical prediction. We conclude that there is compelling experimental evidence which support the theoretical prediction. New experimental tests of the theoretical prediction are suggested.
1. Introduction Recently, the Bose-Einstein condensation (BEC) mechanism has been generalized to a ground-state mixture of two different positively charged bosons (such as deuterons and lithium-6 nuclei, or deuterons and palladium nuclei) in harmonic traps. 1 One of the main predictions of the BEC mechanism is that the Coulomb interaction between two charged bosons may be suppresssed for the case of a large number of particles and hence the conventional Gamow factor may be absent. The theory has been used to analyze low-energy nuclear reaction (LENR) experiments involving atomic clusters (Pd black powders) 2 and acoustic cavitation. 3 The generalization to the two species case allows us to propose an alternative theoretical interpretation of LENR processes in deuterated metals to include the two-species reactions with entrance channel (D + X) where X represents a Bose nucleus other than D, in addition to the conventional one-specie (D + D) reaction. Both (D + X) and (D + D) reactions may be occurring in LENR and transmutaion experiments. For application of the BEC mechanism to LENR and transmutation (or cold nucleosynthesis) experiments involving metals, we assume that non-equilibrium fluctuations might make either vacancies or impurities sufficiently mobile so as to allow Bose nuclei to move collectively in localized regions. Another possibility is 718
719
that these non-equilibrium fluctuations might enable the particles to tunnel so as to create localized BEC states. These mechanisms are expected to be more favaorable with micro- and nano-scale atomic clusters, dendrites, and cavities on metal surfaces, and are consistent with recently proposed "crud" scenario.4 The proposed theoretical interpretation is discussed for the results (excess heat and nuclear emission) of LENR experiments with deuterated metals (heavy water electrolysis, deuterium gas, etc.) including triggering requirements such as laser stimulation, 5 and deuteron beam experiments. 6,7 To assess the validity of this proposed theoretical interpretation for the LENR experiments, it is essential to carry out accurate probes of isotope abundance ratios in deuterated metals by neutron activation analysis (NAA), time of flight secondary ion mass spectroscopy (TOFSIMS), and trace-element accelerator mass spectroscopy (TEAMS). 8 ' 9 2. Bose—Einstein Condensation Mechanism Recently, the previously developed theory 1 0 - 1 4 of the BEC mechanism for onespecie LENR such as (D + D) reactions has been generalized to two-species case and applied to (D + Li) reactions. 1 In this section, we summarize the results and predictions of two-species BEC mechanism for LENR and transmutation processes.1 2.1. Selection
Rules
For the BEC mechanism for LENR and transmutation processes, there are two selection rules: (1) nuclear spin selection rule and (2) nuclear mass-charge selection rule. (1) The nuclear spin selection rule: The nuclear spins of both species must be integer. This rule is obvious for the BEC mechanism. (2) The nuclear mass-charge selection rule: This approximate selection rule is given by the following relation: Zi/Z2 = m i / m j « (Zi + Ni)/(Z2
+ iV2),
where Ni is the number of neutrons in the Bose nucleus for the specie i. We note that the above relation is satisfied, for example, for two species with Zi = Ni. 2.2. Fusion
Rates
For the two species case, we approximate the short-range nuclear interaction by a Fermi pseudo-potential 10 and write it in a generalized form as ImV?(r)
=
-Atjh5(r)/2,
where the nuclear reaction rate constants A^ are given by
Mj =
2SiJ4J)/(nh)
720
with r^3 = h2/2/u,ijZiZje2 and /j,^ = mimj/rrii +m,j. Sij are the S-factors for nuclear fusion between two nuclei from species i and j . The nucleus-nucleus fusion rates are determined from the trapped ground state wave function \P as: Rn = - ( 2 / f t ) £ < * \lmV^(xi JVi
- Sj)| * ) / ( * | * > ,
N2
R12 = -(2/»)X;52<* \hnV*& -y3)\ *)/(*|*>, i?22 = _(2/fi) ]T ( ^ l l m ^ ^ - ^ ) ! *>/{*|*>, and in the mean-field approximation, we have Ru = AnNinf/2, R\2 = A^Nin®, and R22 = A22N2n23/2, where nf = iVi/((4/3)7ri?f), where Nt is the total number of specie i and Ri is the radius of the trap for specie i. If the probabilities of the mean-field ground state occupation, 10 fij, are taken into account, the trap fusion rates are given by R\x = Q,\R\\,R\2 = ^2-^22, and R\2 = Q3R12. We expect that f23 « \ / ^ i ^ 2 2.3. Application 6
to (D + Li)
Reactions
4
For Li(d,a) He (Q = 22.37MeV) and 7 Li(d,n)2 4 He (Q = 15.12MeV), the Sfactors are 18.8MeV-barn 15 ' 16 and 30MeV-barn 17 , respectively, as shown in Table 1. Using these values we find that the corresponding nuclear reaction rate constants are Ai6Li ~ 5.8 x 10~ 1 5 cm 3 /s and A d 7 Li « 8.97 x 10~ 1 5 cm 3 /s, which are about 50 times larger than the d-d nuclear reaction rate constant Add ~ 1-5 x 1 0 - 1 6 cm 3 /s. Table 1. Lithium reactions with positive Q-values extrapolated S-factors at E = 0. Reaction 6
4
Li(d,a) He Li(d,t) 5 Li 6 Li(d,an) 3 He 6 Li(d,ap) 3 H 6 Li(d,n) 7 Be 6 Li(d,p) 7 Li 6 Li(d,7) 8 Be 6 Li(p,a) 3 He 7 Li(d,n)2 4 He 7 Li(d,a) 5 He 7 Li(d,n) 8 Be 7 Li(p,a) 4 He 6
and
Q-value (MeV)
S (MeV-barn)
22.37 0.59 1.80 2.56 3.38 5.03 22.27 4.02 15.12 14.23 15.03 17.24
18.8, 1 5 16.9, 16 18.7 16
30 ± 6 1 7
We expect that nuclear reaction rate constants for reactions 6 Li( 6 Li, 5 Li)7Li
721
(Q = 1.86MeV) and 6 Li( 6 Li,a)2 4 He (Q = 20.897MeV) are much smaller than Ai6LiFor the BEC mechanism, the (d+ 7 Li) reaction rate is expected to be suppressed compared with the (d + 6 Li) reaction rate due to the selection rule (1). This is consistent with the observation of depletion of 6 Li 1 8 , 1 9 as inferred from increased 7 Li/ 6 Li abundance ratio in Arata-Zhang's particulate Pd exposed to deuterium gas 20 " 22 (see Table 2). The excess heat and 4 He observed in electrolysis experiments 23 may be due to 6 Li(d,a) 4 He in addition to other reactions leading to the final states without 4 He (see Table 1). This would be an alternative scenario to the (d + d) reaction scenario which has been proposed by many. Table 2. 7 L i / 6 L i ratios in palladium exposed to gaseous hydrogen and deuterium from TOF-SIMS analyses. Sample designation Pd—D from Arata (Virgin) P d - A from Arata (Active) Pd—B from Arata (Active) P d - C from Arata (Active) SRI-H2O (Arata Experiments) SRI—D2O (Arata Experiments) Arata S-8 Powder Arata S-5 Powder Arata S-2 Powder Arata S-l Powder Li Tsinghua Sample E Li Tsinghua Sample D Li Tsinghua Sample B (Virgin) SC-1 Unused Catalyst (Case 4 6 ) SC-2 (SC-l)(prod l l p p m He) SC-19(SC-20)(prod 9 p p m He) SC-20 (Prod. No He)
7
L i / 6 L i Ratio 13.6 14.5 22.0 16.2 14.5 13.8 14.6 13.5 12.3 13.1 23.3 13.1 12.9 16.7 17.5 12.6 10.2
Uncertainty 1.0 0.3 1.4 0.1 1.7 0.1 3.4 1.8 0.8 0.5 1.8 1.1 0.8 1.4 3.3 0.7 0.8
One Sigma range 12.6-14.6 14.2-14.8 20.6-23.4 16.1-16.3 12.8-16.2 13.7-13.9 11.2-18.0 11.7-15.3 11.5-13.1 12.6-13.6 21.5-25.1 12.0-14.2 12.1-13.7 15.3-18.1 14.2-20.8 11.9-13.3 9.4-11.0
Note: Terrestrial Lithium (Handbook) 12.48.
2.4. LENR and Transmutation Region
Processes
in the Metal
Surface
As pointed out recently by Storms, 4 ' 24 there are many experimental observations 26-37 suggesting that LENR and transmutation processes in condensed matter may be occuring in nuclear active environment (NAE) or nuclear active spot (NAS) created in the surface region of deuterated metals. If this active spot contains a high-density plasma (positive ions (nuclei) and electrons) trapped in a micro/nanoscale cavity in the metal surface region, our theoretical model for the BEC mechanism is appliciable and could provide an appropriate theoretical description of LENR and transmutation (cold nucleosysthesis) processes.
722
3. Experimental Evidences for (D + Li) and Other Two-Species Reactions A number of hints have been evident over the past 16 years that lithium and possibly other light elements such as beryllium and boron were the source of excess heat production by various possible nuclear reactions with deuterium. Many of these reactions produce heat without appreciable emission of neutrons or tritium, but are indeed capable of producing the small levels of these products that have been detected. The most obvious hint was the almost complete absence of neutrons or tritium commensurate with the observed levels of excess heat. When finally detected, these products were not even in the same ratio with each other as expected from the D + D reaction. The ratio expected was 1:1 and the observed ratio was more like one million to one, favoring tritium. Even tritium was about one million times smaller than expected from D + D, if indeed that reaction had been the source of the excess heat observed. Since those early observations many attempts have been made to explain how D + D reaction channels could be modified in a solid to favor 4 He reaction by 10 million times over the expected value and the almost complete, and unequal, suppression of the channels leading to tritium or neutrons. 38 ' 39
3.1. Possible
Roles of
Impurities
Another early hint was the observation that there was a batch effect present among the palladium samples used as cathodes in the electrochemical cells producing excess heat. Some were noticeably more productive of excess heat episodes than others. These more productive cathodes were among the least pure palladium batches. Here was a hint that the impurities in palladium were playing a role in the heat production process. It was assumed at the time that such a role might be in the physical strengthening of the metal to prevent cracking during its 10% volumetric expansion upon being loaded with deuterium. The idea that these impurities might be direct participants in the nuclear reactions producing heat was not seriously considered in those early few years. The impurities were measured and found to be not overwhelmingly different among the various batches of palladium, but one element stood out as a major consitituent among those present. This was boron, element number 5. Among the electrolytes used in the electrochemical cells, the impurity levels were not readily distinguished from each other, but all had beryllium and boron present at parts per billion levels in addition to the predominant lithium. It was noticed that small additions of aluminum and boric acid to the electrolyte were apparently beneficial to increasing the frequency of excess heat episodes in a given cell. Again, the trace impurities showed some sign of influencing the output of excess heat. Pursuit of the boric acid electrolyte addition was truncated at SRI International by McKubre after their observation of a disturbing change in the curve of electrical resistivity vs. deuterium loading. The changed nature of that curve from one maximum at
723
around 0.7D/Pd to one with two-peaks was such as to make definite monitoring of deuterium loading ratios highly uncertain. 40 The loading ratio was believed at that time to be the primary variable determining the appearance of excess heat episodes, so that boric acid addition was stopped. Of course, boron at around 50-100 ppm by weight, was still present in the various batches of palladium (actually 1000 ppm as atom fraction since boron atoms are one tenth the mass of palladium atoms). The fact that such minor additives of aluminum and boric acid to the electrolyte (~200ppm each by weight) had such a large effect on the system shows that the cathode surface nature is a determining factor in excess heat appearance. It was surprising that the boric acid additive should so dramatically influence the bulk metal property of electrical resistivity by which the loading ratio D/Pd was measured. One could speculate that boron is loading into the bulk Pd along with the deuterium. However, we must not overlook the fact that the element boron appears to increase the appearance of excess heat episodes and that it is plausible that the boron atom can move within the bulk lattice of the palladium sufficiently to affect the electrical resistance, as already observed for deuterium atoms.
3.2. Initiation
Period
and Surface
Effect
Another factor widely observed in the electrochemical methods of producing excess heat was the 200-600 h "initiation" period before any episodes of excess heat were observed. This fact suggests that some slow process must be completed to achieve the conditions necessary for excess heat production. Speculation on such a slow process has included diffusion of some atom or ion to some required location at the cathode surface or within the bulk, such as at grain boundaries. Lithium ions in the lithium deuteroxide electrolyte along with the impurities always present in this electrolyte are the prime suspects for this process. Another slow process is the gradual buildup of a surface layer on the cathode from well known cathodic deposition of any positive ion in the electrolyte, whether initially present or dissolved from the cell anode (platinum in most cases) or from the glass or quartz or Teflon cell walls. Observation of a black layer of porous material on the cathodes of many cells that ran for long times is well established. The composition of this black layer has occasionally been analyzed. Platinum, palladium, and calcium, silicon, and boron are among the elements observed, but no systematic study of the layer is known to have been performed. Evidence from a study by Storms 41 using platinum cathodes suggests that this layer is the likely locale of the excess heat effect. The impurities as well as the metals present there in a finely divided form of high surface area may be the source of excess-heat episodes. A surface source is all the more plausible from the observation of helium of mass 4 in the gas phase of heat-producing electrochemical cells.42 If helium had been formed initially within the palladium cathode lattice, it would not easily move to the gas phase of the closed cell. In fact helium in solids lies sequestered for many years if it is initially produced within the solid by nuclear processes driven by high energy particles in cosmic rays. 25
724
3.3. Evidence for (D + Li) 6
Reactions 7
Lithium has two isotopes, Li and Li with a natural ratio of 12.5 favoring 7 Li. Both may plausibly react with deuterium or protium in a set of 12 exothermic reactions, nine of which produce helium of mass 4 as listed in Table 1. However, it is likely that the reaction rate for each of these isotopes may be different enough in various cold fusion type experiments to show a change in the 7 Li/ 6 Li ratio remaining after the excess heat episodes are sufficiently productive of excess heat to burn out one of the two more than the other. Therefore, several investigators measured the 7 Li/ 6 Li ratio in materials known or alledged to have produced a substantial quantity of excess heat. 1 8 , 1 9 ' 4 3 The major problem in this effort is to avoid lithium that is depleted in 6 Li in the initial surface. The use of 6 Li for thermonuclear devices was intense enough to have left behind a legacy of lithium depleted in 6 Li below its natural level. The TOF-SIMS method is particularly well suited to this measurement since there are no significant interferences at those two mass numbers and lithium is more readily ionized than most other elements by the input gallium-71 beam of the instrument. Also, if the active region of excess heat production is at the surface of the material, this surface analysis method is all the more appropriate. Tables 2 and 3 give the 7 Li/ 6 Li ratios measured in a number of palladium samples from experiments that reportedly produced substantial amounts of excess heat. Needless to say, a much more comprehensive effort on many more candidate samples is necessary to fully confirm these initial suggestive findings. Table 3. Ratios of 7Li—6Li in active samples relative to the virgin materials or materials from the same batch giving no excess heat or 4 He. Samples ratioed Pd-A/Pd-D Pd-B/Pd-D** Pd-C/Pd-D SRI-D2O/SRI-H2O SRI-D20/Pd-D SRI-H20/Pd-D Arata S-8/Pd-D Arata S-5/Pd-D Arata S-2/Pd-D Arata S - l / P d - D Li Tsinghua E / B * * Li Tsinghua D / B SC-2/SC-1 SC-19/SC-20*
Ratio 1.066 1.618 1.191 0.952 1.015 1.066 1.074 0.993 0.904 0.963 1.806 1.016 1.053 1.232
Uncertainty 0.082 0.159 0.088 0.114 0.075 0.148 0.268 0.151 0.090 0.081 0.181 0.107 0.221 0.120
Note: *High by ~ 2 sigma; **High by 3-5 sigma.
One might wonder how lithium might be the nuclear reation source of excess heat in experiments apparently lithium free. The TOF-SIMS measurements of numerous solid samples convinced us that lithium, like sodium, is a surface contaminant on
725
ALL surfaces exposed to handling in the earth's atmosphere. The amounts DID vary, but lithium always showed up. We believe it would take a determined effort to perform an experiment with a surface free of lithium.
3.4. Possible
Roles of Boron
Impurity
Beryllium with only one stable isotope, 9 Be, is not susceptible to this sort of experimental test. However, boron with the two isotopes 1 0 B and n B is subject to a similar test. Just as with 6 Li and 7 Li, both boron isotopes produce excess heat and 4 He without neutrons or tritium, but in any situation, reactions with one will most likely favor one over the other hence leading to a difference from the natural ratio of 4.0 favoring n B . No appreciable data on 1 0 B/ 1 1 B ratios are yet available. However, depletion of 10 B has been reported in several cathodes that reportedly produced substantial excess heat. These measurements were performed by prompt gamma neutron activation analysis (PGNAA), 44 but the method is not sensitive to n B .
3.5. Summary
of Section
3
The case favoring non-D + D reactions as the source of excess heat in cold fusion type experiments has been given here. The light elements have been favored because they are almost universally present at low levels in all the materials used in such studies and all three of them have known reactions producing excess heat and 4 He without predominantly neutrons or tritium, even though such reactions are known. Some hints of other nuclear reactions such as the fission of palladium isotopes to elements in the region around iron (element 26) exist 18 but are not considered sufficiently robust to treat in detail here. Such reactions may indeed be present and would produce excess heat without commensurate neutrons or tritium (with positive exothermic energies per reaction of 20-30 MeV). However, 4 He would not be produced in such reactions. The evidence does point to a reaction on large surface area materials of a catalytic nature 2 0 - 2 3 , 4 5 and seems to indicate the possibility of a gaseous interface with the catalyst as being the key. For example, even in liquid electrolyte experiments, the high deuterium loading criteria may be signaling the need for a high rate of hydrogen bubble formation at the cathode surface, maximizing the time spent as a gaseous interface of bubble and surface. The long time required before observation of excess heat may signal the need to build a high surface area deposited film to contact that continual series of gaseous deuterium bubbles after loading is complete to a high level. In the case of Arata-Zhang, 2 0 - 2 2 the production of excess heat seems to favor palladium particle sizes under 40 nm exposed to high pressure deuterium gas inside their hollow cylindrical cathode.
726
4. P r o p o s e d E x p e r i m e n t a l T e s t s In order to test the possibility t h a t (D + Li) reactions are involved in the L E N R processes in condensed m a t t e r and also to test the predictions of the B E C mechanism as described in Sec. 2, we propose t o use 6 Li and 7 Li separately and also to use microporous or nanopourous materials in the following types of experiments: (1) electrolysis experiments of Fleischmann-Pons t y p e , 4 6 - 5 4 (2) gas experiments,2.20-22,45,55 (3) nuclear emission experiments. 5 6 ' 5 7 T h e microporous or nanoporous materials include: vycor glasses, 5 8 aerogels, 5 9 nanogels, 6 0 ordered nanoporous thin films, 61 carbon arerogels, 6 2 and pocofoams. 6 3 T h e use of microporous or nanoporous materials in these experiments recently proposed by Kim et al,64 is expected to enhance the observed effects by many orders of magnitude if the observed processes are surface phenomena, since active surface is substantially larger for these materials compared with the surface area of a bulk metal.
5. S u m m a r y a n d C o n c l u s i o n s There are now a substantial number of L E N R experimental d a t a indicating t h a t (D + Li) reactions are involved in L E N R processes in condensed m a t t e r s . In addition, there are many indications t h a t the L E N R processes in condensed m a t t e r s are surface phenomena. T h e B E C mechanism may provide a suitable theoretical description for the surface phenomena involving high-density plasma (D, Li, e~) formed in micro/nanoscale cavities. T h e possibility of (D + Li) reactions and the predictions of the B E C mechanism for L E N R processes can b e tested by carrying out (1) electrolysis experiments of Fleischmann-Pons type, (2) gas experiments and (3) nuclear emission experiments, using 6 Li and 7 Li separately and also using porous materials instead of bulk metals, as recently proposed by Kim et al.64
References 1. Y.E. Kim and A.L. Zubarev, Mixtures of charged bosons of confined in harmonic traps and Bose—Einstein condensation mechanism for low-energy nuclear reaction and transmutation processes in condensed matters, submitted to ICCF-11 (Marseilles, France, 2004), and references therein. 2. Y.E. Kim, D.S. Koltick, R. Pringer, J. Meyers, and R. Koltick, Proceedings of the ICCF-10 (Cambridge, MA, USA, 2003). 3. Y.E. Kim, D.S. Koltick, and A.L. Zubarev, Proceedings of the ICCF-10 (Cambridge, MA, USA) 4. E. Storms, What conditions are required to initiate the LENR effect ? in Proceedings of the ICCF-10 (Cambridge, MA, USA, 2003). 5. D. Letts and D. Cravens, Proceedings of the ICCF-10 (Cambridge, MA, USA, 2003). 6. J. Kasagi, Proceedings of the ICCF-10 (Cambridge, MA, USA, 2003). 7. J. Kasagi, Proceedings of the ICCF-11 (Marseilles, France, 2004).
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8. 9. 10. 11. 12. 13. 14. 15. 16. 17. 18.
19.
20. 21. 22. 23. 24. 25. 26. 27. 28. 29. 30.
31.
32. 33. 34. 35.
G.K. Hubler et al., Proceedings of the ICCF-10 (Cambridge, MA, USA, 2003). T.O. Passell, Proceedings of the ICCF-10 (Cambridge, MA, USA, 2003). Y.E. Kim and A.L. Zubarev, Fusion Technol. 37, 151 (2000). Y.E. Kim and A.L. Zubarev, Italian Phys. Soc. Proc. 70, 375 (2000) for ICCF-8 (Lerici, La Spezia, Italy, 2000). Y.E. Kim and A.L. Zubarev, Phys. Rev. A64, 013603 (2001). Y.E. Kim and A.L. Zubarev, J. Phys. B: At. Mol. Opt. Phys. 33, 55 (2000). Y.E. Kim, Progr. Theor. Phys. Suppl. 154, 379 (2004). S. Engstler et al., Z. Phys. A342, 471 (1992). A. Musumara et al, Phys. Rev. C64, 068801 (2001). J. Yan et al., Nucl. Phys. A621, 127c (1997). T.O. Passell, Evidence for Litium-6 depletion in Pd exposed to gaseous deuterium and hydrogen, in Proceedings of the Ninth International Conference on Cold Fusion, May 19-24, 2002 (Beijing, 2002). T.O. Passell, Pd-110/Pd-108 Ratios and trace element changes in particulate palladium exposed to deuterium gas, in Proceedings of the Tenth International Conference on Cold Fusion (Cambridge, MA, USA, 2003). Y. Arata and Y.C. Zhang, Italian Phys. Soc. Proc. 70, 11 (2000) for ICCF-8 (Lerici, La Spezia, Italy, 2000). Y. Arata and Y.C. Zhang, Jpn. J. Appl. Phys. 37, L1274 (1998). Y. Arata and Y.C. Zhang, Jpn. J. Appl. Phys. 38, L774 (1999). M. McKubre et al., Italian Phys. Soc. Proc. 70, 3 (2000) for ICCF-8 (Lerici, La Spezia, Italy, 2000), and references therein. E. Storms, The APS Conference (Austin, TX, USA, March 3-7, 2003). W.J. Camp, Helium detrapping and release from metal tritides, J. Vac. Sci. Technol. 14, 514 (1977). E. Storms and C. Talcott-Storms, The effect of hydriding on the physical structure of palladium and on the release of contained tritium, Fusion Technol. 20, 246 (1991). P.A- Mosier-Boss and S. Szpak, The P d / ( n ) H system: transport processes and development of thermal instabilities, Nuovo Cimento A 112, 577 (1999). S. Szpak, P.A. Mosier-Boss, and M.H. Miles, Calorimetry of the Pd + D codeposition, Fusion Technol. 36, 234 (1999). J. Dash and S. Miguet, Microanalysis of Pd cathodes after electrolysis in aqueous acids, J. New Energy 1(1), 23 (1996). G.H. Miley, et al, Quantitative observations of transmutation products occuring in thin-film coated microspheres during electrolysis, in Proceedings of the Sixth International Conference on Cold Fusion, Progress in New Hydrogen Energy (Lake Toya, Hokkaido, Japan, 1996); New Energy and Industrial Technology Development Organization, Tokyo Institute of Technology, Tokyo, Japan. Y. Iwamura, et al., Detection of anomalous elements, X-ray and excess heat induced by continuous diffusion of deuterium through multi-layer cathode ( P d / C a O / P d ) , in Proceedings of the Seventh International Conference on Cold Fusion (Vancouver, Canada: ENECO Inc., Salt Lake City, UT, 1998). J.O.M. Bockris and Z. Minevski, Two zones of 'Impurities' observed after prolonged electrolysis of deuterium on palladium, Infinite Energy 1, 67 (1996). T. Ohmori, et al, Transmutation in the electrolysis of lightwater - excess energy and iron production in a gold electrode, Fusion Technol. 3 1 , 210 (1997). D.S. Silver, J. Dash, and P.S. Keefe, Surface topography of a palladium cathode after electrolysis in heavy water, Fusion Technol. 24, 423 (1993). G.H. Miley, et al, Multilayer thin film electrodes for cold fusion, in Proceeding of the Third International Conference on Cold Fusion, Frontiers of Cold Fusion (Nagoya
728 Japan: Universal Academy Press Inc., Tokyo, Japan, 1992). 36. E. Storms, A critical evaluation of the Pons-Fleischmann effect: Part 2, Infinite Energy 6(32), 52 (2000). 37. R.T. Bush and R.D. Eagleton. A calorimetric study of the excess heat effect in thin films of palladium, in Proceedings of the Second Annual Conference on Cold Fusion, The Science of Cold Fusion (Como, Italy: Societa Italiana di Fisica, Bologna, Italy, 1991). 38. P.L. Hagelstein, Proceedings of the ICCF-8 (Lerici, La Spezia, Italy, 2000); Proceedings of the ICCF-10 (Cambridge, MA, USA, 2003), and references therin. 39. S.R. Chubb and T.A. Chubb, Proceedings of the ICCF-8 (Lerici, La Spezia, Italy, 2000); Proceedings of the ICCF-10 (Cambridge, MA, USA, 2003), and references therin. 40. M. McKubre, et al., SRI EPRI Report TR-104195 (August 1994), pp. 3A-1 to 3A-22. 41. E. Storms, Proceedings of the ICCF-8 (Lerici, La Spezia, Italy, 2000), pp. 55-61. 42. M. McKubre, et al., SRI EPRI Report TR-107843, Vol. 1, 1998, pp. 3-226 to 3-235. 43. D. Thompson, Proceedings of the ICCF-1 (Salt Lake City, Utah, 1990). 44. T.O. Passell, Search for nuclear reaction products in heat-producing palladium, in Proceedings of the ICCF-6 (Hokkaido, Japan, 1996). 45. L.C. Case, Fusion Technoi, 20, 478 (1991); Proceedings of the ICCF-6 (Vancouver, Canada, 1998; see also [23]). 46. P.L. Hagelstein, M.C. Mckubre, D.J. Nagel, T.A. Chubb, and R.J. Hekman, New physical effects in metal deuterides, submitted to DOE for a review, July 2004, and references therein. This report was posted December 1, 2004 at the DOE website: http://www.sc.doe.gov. 47. See experimental papers in the Proceedings of the 10th International Conference on Cold Fusion (ICCF-10) (Cambridge, MA, USA, 2003). 48. E. Storms, Why cold fusion has been so hard to explain and duplicate, in Proceedings of the APS Conference, March 3-7, 2003 (Austin, TX, USA, 2003). 49. D. Letts and D. Cravens, Laser stimulation of deuterated palladium: past and present, in Proceedings of the ICCF-10 (Cambridge, MA, USA, 2003). 50. S. Szpak, P.A. Mosier-Boss, J. Dea, and F. Gordon, Polarized D + /Pd-DaO system: hot spots and 'mini-explosions', in Proceedings of the ICCF-10 (Cambridge, MA, USA, 2003). 51. S. Szpak, P.A. Mosier-Boss, M.H. Miles, and M. Fleischmann, Thermal Behavior of polarized Pd/D electrodes prepared by co-deposition, Thermochim Acta 410, 101 (2004). 52. M. McKubre, et al, Italian Phys. Soc. Proc. 70, 3 (2000) for ICCF-8 (Lerici, La Spezia, Italy, 2000). 53. G.H. Miley, et al, Quanitative observations of transmutation products occuring in thin-film coated microspheres during electrolysis, in Proceedings of the Sixth International Conference on Cold Fusion, Progress in New Hydrogen Energy (Lake Toya, Hokkaido, Japan, 1996): new Energy and Industrial Technology Development Organization, Tokyo Institute of Technology, Tokyo, Japan; Proceedings of the ICCF-10 (Cambridge, MA, USA, 2003). 54. D.S. Silver, J. Dash, and P.S. Keefe, Surface topology of a palladium cathode after electroylsis in heavy water, Fusion Technoi. 24, 423 (1993). 55. Y. Iwamura, et al., Jpn. J. Appl. Phys. 41, 4642 (2002); Proceedings of the ICCF-10 (Cambridge, MA, USA, 2003). 56. S.E. Jones, et al., Charged-partiele emissions from metal deuterides, in Proceedings of the ICCF-10 (Cambridge, MA, USA, 2003). 57. S.E. Jones, et al., Neutron emissions from metal deuterides, in Proceedings of the
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ICCF-10 (Cambridge, MA, USA, 2003). P. Levitz, G. Ehret, S.K. Sinha, and J.M. Drake, J. Chem. Phys. 95, 6151 (1991). J. Fricke and A. Emmerling, J. Sol-Gel Sci. Technol. 13, 299 (1998). http://www.cabot-corp.com. L. Menon, Nanoarrays Synthesized from Porous Alumina, Dekker Encyclopedia of Nanoscience and Nanotechnology (Marcel Dekker, Inc., New York, NY, 2004), pp. 2221-2238. 62. R.W. Pekala, et al., in Y.A. Attia (ed) Sol-Gel Science and Applications (Plenum Press, New York, 1994), p. 369. 63. MRS Bulletin, December 2000, p. 10; http://www.pocofoam.com. 64. Y.E. Kim, et al., Proposal for new experimental tests of the Bose-Einstein condensation mechanism for low energy nuclear reaction and transmutation processes in deuterium loaded micro- and nano-scale cavities, in Proceedings of the ICCF-11 (Marseilles, France, 2004). 58. 59. 60. 61.
3
H e / 4 H e P R O D U C T I O N RATIOS B Y T E T R A H E D R A L SYMMETRIC CONDENSATION
AKITO TAKAHASHI Osaka
University, Yamadaoka 2-1, Osaka 565-0871, E-mail:akito@sutv. zaq.ne.jp
Japan
The present paper treats application of the Electronic Quasi-Particle Expansion Theory (EQPET) model for Tetrahedral Symmetric Condensate (TSC) of H / D mixed systems for Pd host metal. Production ratios of 3 H e / 4 H e for multibody fusion reactions in H / D mixed TSC systems are calculated as a function of H/D mixing rate. The model is further extended to treat direct nuclear interactions between host-metal nucleus and TSC of pure four protons (or four deuterons), since TSC can become very small (far less than 1 pm radius) charge-neutral pseudoparticle. Results for the case of Ni + 4 p / T S C are discussed with Ni + p capture reactions and Ni + 4p fission reactions.
1. Introduction Tetrahedral Symmetric Condensate (TSC), for example, by orthogonal coupling of two D 2 molecules (four deuterons plus four electrons), has been proposed as a seed of clean fusion in condensed matter/ 1 ) Applying the Electronic Quasi-Particle Expansion Theory (EQPET) model, modal fusion rates for 2D, 3D, 4D, and 8D fusion reactions in TSC and Octahedral Symmetric Condensate (OSC) were numerically estimated. These analyses could explain consistently the major experimental results of excess heat with 4 He ash, minor tritium generation, very weak neutron emission, and transmutation and fission of host metal nuclei. 1 ~ 3 In this work, the theory was extended to analyses for H/D mixed systems. It is concerned that usual D2O electrolysis experiments with open cells and Pd cathodes would be contaminated with hydrogen (H) as experimental time elapses. Modal fusion rates for HD, DD, DDDD, HDDD, and HDHD fusion reactions were calculated by EQPET, as a function of H/D mixing ratio. 3 He is produced by HDHD and HDDD reactions. As a result, 3 He/ 4 He ratios were given as a function of H/D ratio, to be for example 3 He/ 4 He = 0.1% for H/D = 1% and 3 He/ 4 He = 25% for H/D = 60%. Secondary transmutation reactions by 3He-particles were estimated to have very small reaction rates. Discussions are added for the pure hydrogen TSC (4p + 4e). Since the EQPET model gives approximate size of TSC to be less than 1 pm in radius, TSC will behave as a "charge-neutral pseudoparticle" when it approaches to a host metal atom which has much larger atomic (electron cloud) radius than 100pm (1 A). We may expect therefore direct nuclear interaction between TSC and host metal nucleus, because 730
731
TSC can drastically reduce Coulomb barrier to host nucleus. Thus, we have a possibility of nuclear reactions as Ni + p, Ni + 4p, Pd + 4d, W + 4p, Cs + 4d, etc., with highly enhanced reaction rates. The present theory may, therefore, explain a variety of claims for H- or D-systems. For candidate places where TSC is formed, we have considered two cases: (1) TSC may be formed within a thin layer (1-100 nm thickness) of the surface lattice of metal deuteride with full D-loading. TSC-induced multibody fusion in PdDx lattice dynamics is modeled for this case. 1 - 3 The following case of theoretical modeling of H/D mixed systems with PdDx has done for the case of (A), namely for regular metal-deuteride lattice. (2) D 2 trapping points on fractal metal surface, which is such place like corner holes near ad-atoms plus dimmers will be the second candidate. In the case (B), we consider a trapped D 2 has lost freedom of rotating motion but is vibrating and waiting for coming-in D 2 molecule to make an orthogonal TSC coupling. When these meet coherence in vibrations of two D 2 molecules with antiparallel spin arrangement, TSC formation probability will be drastically increased. The following case of theoretical modeling for Ni + H systems has done for the case of (B). 2. H / D Mixed Systems Some works have reported observation of significant amount of 3 He generation in heavy water electrolysis with Pd cathodes. They claimed that observations were ascertained by high-resolution mass spectrometry (QMAS). Especially, Arata et a/.,4 claimed very high amounts of 3 He production, namely 3 He/ 4 He atomic ratio 0.25 with IE + 18 to IE + 19 4 He atoms which are comparable to excess heat level assuming 23.8 MeV per 4 He. Note that 4D/TSC fusion produces two 23.8 MeV 4 He particles in 180° opposite directions by the break-up (final state interaction) of 8 Be* compound nucleus of 4d multibody fusion.1"3 The author predicts that 3 He have come from products of multibody fusion reactions in H/D mixed TSC pseudoparticles. In open-cell-type electrolysis experiments, the researchers keen an the contamination of hydrogen in liquid (electrolyte), when we continue long-time run of experiments. By applying the TSC model with EQPET, we can estimate 3 He/ 4 He production ratios for H/D mixed systems. By replacing one or two deuterons in 4D/TSC with one or two protons, we treat the system. Basic four-body fusions in mixed H/D systems will be the following three multibody fusion reactions: D + D + D + D - * 8 Be* -* 4 He + 4 He + 47.6MeV,
(1)
D + D + D + H - ^ 7Be* - • 3 He + 4 He + 29.3MeV,
(2)
D + H + D + H-^6Be*^3He+3He+11.0MeV minor out-going channels of three reactions are discussed elsewhere.
(3) 5
732
Combination probabilities of T S C for H / D mixed system can be approximately estimated using Y = H / D atomic density ratio, as follows: CDDDD = k(l - Y)\
(4)
C D D D H = A(l - Y)3Y,
(5)
C D H D H = *(1 - Y)2Y\
(6)
C D H H H =fc(l- F ) F 3 ,
(7)
CHHHH = *r4,
(8)
we set here normalization constant k to keep t h e total probability to be unity. Calculated combination probabilities as a function of H / D ratio are shown in Fig. 1. T h e contamination rate of hydrogen is given as Y/(l + Y), and we need to convert it from Y value. For instance, 50% H / D ratio corresponds to t h e contamination of 33.3%. Microscopic fusion rates for mixed H / D E Q P E T molecules are calculated by t h e following equations. Here barrier penetration probability for four-body reaction is approximated by the product of two-body probabilities as rapid sequential twobody processes. 3 T h e P ( d d ) denotes t h e barrier penetration probability for d - d interaction, and P ( p d ) denotes for p - d interaction. Adddp = ( S d d d p / £ > P ( d d ) P ( d p ) ,
(9)
Adpdp = ( S d p d p / £ ) ^ ( d p ) P ( d p ) .
(10)
We estimate S'-values using P E F = 9 for D D D H and P E F = 6 for DHDH, as we have discussed for strong interaction and shown scaling law in Ref. 3. S d d d p = 1.0£ + 9keV&,
(11)
Sdpdp = l - 0 £ + 8 k e V 6 .
(12)
And the barrier penetration probability P ( d p ) for d - p fusion (or d - d fusion) is given as P ( d p or dd) = e x p ( - 2 r „ ) .
(13)
And Gamow integral is given by b
Tn = J(VS - E)ll2dE/{h/i:)l{2^ll2.
(14)
ro
Here, we carry out integration from ro (5fm) to b-value. Screening potentials for pde* become the same curves as dde* E Q P E T molecules which we have shown
733
Combination probability forTSC cluster
1.2
DDDD DDDH DHDH
0*' 0
Figure 1.
0.1
0.2
0.3 H/D ratio
0.4
0.5
0.6
Combination probabilities of H / D mixed TSCs as a function of H / D ratio.
Table 1. Fusion rates of H / D mixed E Q P E T molecules; values with parenthesis show virtual reaction rates. E Q P e* (1.1) (2.2) (4,4)
dde* (f/s/cl) l.OE-137 l.OE-20 (l.OE-16)
dpe* (f/s/cl) l.OE-120 l.OE-23 (l.OE-21)
dddde* (f/s/cl) 1.0E-252 1.0E-17 1.0E-9
dddpe* (f/s/cl) 1.0E-232 l.OE-16 1.0E-10
dpdpe* (f/s/cl) l.OE-228 1.0E-14 1.0E-10
elsewhere. 1 ' 3 And [i is reduced mass for two-body system, which is 0.667 for d-p pair and 1.0 for d-d pair, respectively. Microscopic fusion rates of EQPET molecules for mixed H/D system are calculated and given in Table 1. We omit here three-body reactions for simplicity. Electronic quasiparticle states are represented here as e*(l,l) for normal electron, e*(2,2) for Cooper pair and e*(4,4) for quadruplet, 1 ' 3 respectively. Wave function of TSC cluster is written by EQPET 1 " 3 as linear combination of EQPET molecule dde* wave functions: *tsc = a i * ( l , 1) + a 2 *(2, 2) + a 4 *(4,4).
(15)
Modal fusion rates are given by A = o?A(l, 1) + a\\{2, 2) + a|A(4,4).
(16)
Using the same weights (a-parameters) for spin arrangement given in Refs. 1 and 3, and using fusion rates of EQPET molecules in Table 1. We obtain modal fusion rates as shown in Table 2. Using the combination probabilities in Fig. 1 and modal fusion rates in Table 2, we obtain 3 He/ 4 He production ratios as shown in Fig. 2.
734 Table 2. DDDD-TSC A d d = 2E-21 (f/s/cl) A 4d = 3E-11 (f/s/cl)
Modal fusion rates for H / D mixed TSC. DDDH-TSC A d p = 1E-23 (f/s/cl) A d d d p = 4 E - 1 2 (f/s/cl)
DHDH-TSC A d p = 1E-23 (f/s/cl) A d p d p = 1E-12 (fr/s/cl)
Note: Here fusion rates are given as fusions per second per cluster.
With H/D ratio of 1%, we predict to have 3 He/ 4 He ratio of 0.1%. With H/D ratio of 50%, we have 3 He/ 4 He ratio of 16%. To get the same value of 3 He/ 4 He ratio by Arata-Zhang experiment, 4 we assume H/D ratio of 60% (37.5% H-contamination in heavy water).
3
He/ 4 He production ratio for TSC fusion
1 0.1
1
0.01 («•*» 3He/4He I
CD
X 1B
0.001
X CO
0.0001
0
0.1
0.2
0.3
0.4
0.5
0.6
H/D ratio Figure 2.
3
H e / 4 H e production ratios as a function of H / D atomic density ratio.
The production of 3 He by H/D mixed systems must become very important, when it will be confirmed by experiments. Since 3 He is stable isotope and we can convert to tritium by irradiating with fission reactor neutron flux and extract tritium rather easily, 3 He production has a great potential for stable nuclear fuel. 3. TSC-Induced Nuclear Reactions 3.1. Minimum
Size of
TSC
In our theoretical view, size of TSC of four deuterons (or protons) + four electrons (with antiparallel spin arrangement) will become very small as far less than 1 pm, as shown in Fig. 3. This is because of the three-dimensionally constrained chargeneutral (energy-minimum for Coulomb interaction) squeezing motion to a central
735
focal point, and TSC will expand finally when four deuterons reach the strong force range (in the domain of several femto-meter radius volume) to make a pseudoatomic state e*(4,4)8Be* which has 0.8pm radius for e*(4,4) orbit (atomic radius). The charge-neutral state of TSC corresponds to the energy-minimum state of system Hamiltonian, and therefore satisfies the solution of variational principle of quantum mechanics. This special condition of TSC makes semiclassical treatment of motion possible. We note here that electrons do not make strong interaction, and thus have to go outside of 8 Be* compound nucleus when 4d/TSC gets into the range of strong interaction. The size (radius) of TSC pseudoparticle decreases linearly and semiclassical treatment of motion is possible, due to three-dimensionally constrained motion to central focal point, until the time when TSC charge-neutrality is broken by getting into the range of nuclear strong interaction (about 5fm range). This feature is illustrated in Fig. 3.
1000
TSC radius
0.001 0.001
0.01
0.1
1
10
100
1000
f? dd , inter-nuclear distance (pm)
Figure 3.
3.2. Sudden
Squeezing of TSC by 3-dimensionally constrained motion.
Tall Thin Barrier
Approximation
In the case of 4p/TSC, we have no strong interaction for fusion (except scattering among protons) and Pauli's exclusion principle for fermions will be the only limitation to stop squeezing of 4p/TSC. This is why heavy water electrolysis produces 4 He ash of 4d multibody fusions with excess heat, but light water electrolysis makes neither 4 He production nor excess heat, by cluster fusion induced in TSC itself. However, we have had to consider more for pure proton-TSC.
736
There is the case that very small condensate of TSC can behave as a chargeneutral pseudoparticle; not only 4d/TSC but also 4p/TSC can "freely" (like a neutron) penetrate through shell clouds of electrons (which have outer-most radius more than 100 pm and innermost K-shell radius of about 1pm), thus "almost" avoiding Coulomb repulsion, to make direct nuclear-strong interaction with host metal nucleus with drastically enhanced reaction rate. The feature is illustrated in Fig. 4.
Target atom outer electron cloud (ca. 100 pm) K-shell e " and nucleus
Neutral pseudo-particle
GO^— — —
_ TSC, <1 pm (4P + 4e): neutral
How deep can TSC penetrate through e-cloud? Figure 4. Penetration of neutral-pseudoparticle of TSC through electron clouds of host metal atom, of which inner most K-shell electron orbit has about 1 pm radius for Z > 30. Minimum size of TSC attained in about 60 fs will be far less than 1 pm.
Therefore, we have the possibility that TSC will make a direct nuclear interaction with host metal nucleus, when TSC gets into the strong interaction range, as shown in Fig. 5. Strong interaction between M-nucleus (host-metal) and TSC takes place as charged-pion exchange between protons of TSC (or virtual-neutrons and virtualprotons for deuteron-TSC) and virtual-neutrons in nucleus. Number of pion exchange force (PEF) is again the scaling rule for estimating the reaction S'-values.3 Electrons in the TSC do not make strong interactions, and are rejected outside when the TSC gets into the strong interaction range for exchanging charged pions (for fusion) and neutral pions (for scattering). Note here that the conjecture of neutron plus proton states in nucleus is virtual, since no independent n with long life or p particles exist within nucleus. An independent neutron decays in about
737
lOmin (hence it destroys nucleus to disintegration). Therefore, strong force exchange (pion-exchange between virtual n and p) is so fast that n plus p image is only virtual for hadron-admixture of nucleus. When the strong interaction starts, the charge-neutrality of TSC is suddenly broken and four protons (or four deuterons) suddenly feel Coulomb repulsion against M-nucleus. The Coulomb barrier height is very large as lOMeV, but its width is very small since the TSC has already approached very close (2-5 fm distance) to Mnucleus. Because of such special conditions, we can formulate simple mathematics to treat the M-nucleus plus TSC nuclear interaction, which we call the Sudden Tall Thin Barrier Approximation (STTBA), as follows.
Range of strong interaction (3-5 fm) Figure 5.
M-nucleus + TSC nuclear interaction mechanism; smaller circle in TSC show electron.
As shown in Fig. 5, we need to consider the topological conditions for PEF, the selection process of plural protons (or deuterons) to be picked up by M-nucleus and the M + (1-4) protons (or deuterons) capture reactions. When p (or d) of TSC gets into the strong force range, electrons in TSC will have to separate and p (or d) will "feel suddenly" a very tall but thin Coulomb repulsion barrier against the host metal nucleus. And four protons (nor four deuterons) of TSC are not combined by the strong force and, therefore, behave independently. The nuclear reaction rate between TSC and M-nucleus can be calculated by the following sudden tall thin barrier approximation (STTBA). A = SMp(E)vPM(E)Pn(E)/E,
(17)
PM(E)=exp{-G),
(18)
738
G = 0A36{nV(R1/2))1/2{b-r0).
(19)
Here we write V in MeV unit and r in fm unit. The Gamow integral Eq. (14) is replaced with a simple approximated formula G. And Ri/2 =r0 + (b- r 0 )/2,
(20)
b = r0 + Xn,
(21)
r 0 = 1.2A 1/3 .
(22)
And Pn(E) gives the coexistence probability of plural p (or d) in the strong interaction range. The range of pion Xn is used here to be 2.2 fm. Pn(E) is approximated by using barrier penetration probability of p-p pair for sudden tall thin barrier height VpP (about 0.24 MeV) in mutual distance Rpp (about 6fm) for minimum radius of TSC drawn in Fig. 3. Pn(E) = exp(-0.218n(/xy pp ) 1/2 J R P p) = 1.0
for n > 1,
for n = 1,
(23) (24)
In Eq.(17), S-values for M + p to M + 4p (M + d to M + 4d) reactions are treated as same values, since PEF numbers for M(A, Z) + p to M(A + 3, Z + 3) + p are considered not to change significantly due to the saturated trend of charged pion exchange between p of TSC and neutron-nucleons in the near surface of M-nucleus. An example of STTBA calculation for Ni of host atom, we obtain microscopic reaction rates as 3.7E-8 (f/s/pair) for Ni + p, 2.1E-7 (f/s/pair) for Ni + d, 1.0E-8 (f/s/pair) for Ni + 4p, 3.4E—9 (f/s/pair) for Ni + 4d reactions, respectively. Here we use S M P ( 0 ) = 1.0E8 keVb and SMd(0) = 1.0E9 keVb, and P(pp) = 0.527 and P(dd) = 0.404. With assumption of M+TSC pair density of 1.0E17 in 10 nm layer of Ni surface, we obtain 1E+9 f/s/cm 2 reaction rate, which is about 5mW/cm 2 for Ni + 4p to fission process.6 Fission products for Ni + 4p reactions have revealed to be mostly radiation-less (clean), coming from higher mass isotopes of Ni as 62 Ni, for example, 62
Ni + 4p - •
66
Ge(Ex = 24.0 MeV) -> fissionproducts.
62
(25)
Major fission channels of Ni + 4p fission is shown in Table 3. From Table III, we see fission products are almost all stable isotopes. However, we may have small branch (less than 3%) of neutron emission channel, of which we need further careful study. Element (Z) distribution of fission products for natural Ni is shown in Fig. 6a, compared with Miley-Patterson Ni-H system experiment. 7 We see consistent agreement for two peak groups over Z = 10 (Ne), though law-Z data are not available in experiments. 7 Probably O and C, if they exist, are difficult to analyze due to contaminants. The formation of TSC in near surface region of host Ni layer will be classified by the mechanism B) as written in Introduction, since it is well known that volumetric
739 Table 3. cooling. 2
Major fission channels for
Ni(3.6%) + 4p
62
Ni + 4p reaction, after one month
66
Ge(Ex=24.0MeV)* 11.0 MeV + n + 6 5 G e ( E C ) 6 5 G a ( E C ) 6 5 Z n 21.4 MeV + 4 He + 6 2 Z n ( E C ) 6 2 C u ( E C ) 6 2 N i 11.5 MeV + 8 B e + 5 8 Ni 18.9 MeV + 1 2 C + 5 4 Fe 10.5 MeV + 1 4 N + 5 2 M n ( E C ) 5 2 C r 8.2 MeV + 1 6 0 + 5 0 C r 13.9 MeV + 2 0 Ne + 4 6 T i 15.2 MeV + 2 4 M g + 4 2 C a 13.7 MeV + 27 A1 + 3 9 K 18.9 MeV + 2 8 Si + 3 8 A r 18.6 MeV + 3 2 S + 3 4 S
Note: Natural abundance of 62 Ni is 3.6%.
hydrogen (deuterium) absorption with full loading is very difficult for a nickel layer. The situation will be in quite a different form in the case of hydrogen (deuterium) loading into Pd layer, for which we proposed the mechanism A). We speculate therefore that Ni + H reaction will be catalyzed on the highly fractal surface to form TSC with incoming H 2 (or H + ) flux. As shown in Fig. 3, the size of TSC is changes dynamically from about 100 pm radius to its minimum radius of about 6 fm within its lifetime (about 60fs). During this dynamic motion, TSC will approach the host metal nucleus. We have not yet studied how to treat this dynamic motion correctly. STTBA is the first order approximation. The inner most K-shell orbit of electron for Ni has 1.9 pm radius, which is larger than 1.15 pm for Pd and 0.58 pm for U, respectively. Therefore the charge-neutral pseudoparticle TSC can have a longer interaction time for M + TSC nuclear interaction for lighter elements like Ni. When TSC makes a strong interaction from a more distant b-parameter than we used in the above mentioned example calculation of STTBA, proton of 4p/TSC has much larger barrier penetration probability than the deuteron of 4d/TSC: this may be the reason why Ni + protons interaction were thought to be more easily observed in experiments. 7 ' 8 So, we need further studies with different host metals with different size K-shells, according to the dynamic interaction between M and TSC. Applications of STTBA to other M + TSC reactions as Pd + 4p, W + 4p, Cs + 4d, Au + 4p, U + 4p, etc. are under way. When we apply STTBA to 4d fusion, we get Xid = 4.9E-5 f/s/cl which is a very high value, and by assuming TSC density as 1E20 (per cm 3 ) we predict the macroscopic yield (see below) to be on the order of 1E15 f/s/cm 3 that is equivalent to a power level of 10 kW/cm 3 . This will give maximum 4D fusion rate attainable in PdD systems. For assuming TSC density, we considered the mechanism A) with high phonon excitation (0.22 eV for PdD) and about 3% weight for anti-parallel spin arrangement for four electrons of TSC, also assuming D density on the order of 1E22 (atoms/cm 3 ).
740 100
Ni + 4p (Ni: Nstural) SCS
SCS Zn
10
S Si
. C
2
Fe Ni
' Ar
O
Cr
Q.
Mg ' * Ne • CI
Ca
10
20
Ti
0.1 0
0
15
25
30
35
40
45
50
Atomic number
Data from Miley - Patterson7 100
_ * „
•
1
10
n
n *
•
t
1
• NAA • EDX1
"0 CD
EDX2 *
0.1
• 0.01 m
0.001
) (
10
i
l
20
30
40
50
Atomic number
Figure 6. Comparison of Ni + 4p fission products and Miley-Patterson results, (a) SCS theory calculation. 6 (b) Yield of "foreign atom" distribution by Miley-Patterson. 7 ' 3 8
The macroscopic reaction rate Y (f/s/cm 3 ) for M + TSC reaction is given by Y = NiM + T S O
(26)
741
Here we have to estimate the density iVM+TSC of "united molecule" M + T S C in atomic level.
iV M +Tsc = <7ANMNTSCVTTSC-
(27)
NM is the host-metal a t o m density, iV T S C the time-averaged T S C density, CTA the atomic level cross section (about 1 . 0 E - 1 6 c m 2 ) for M + T S C combination, and TTSC the mean life of T S C (about 60 fs), respectively. If we can assume Nu = 1E23 (per cm 3 ) and 7V TSC = 1E20 (per c m 3 ) , we obtain roughly NU+TSG - 1E19 (per c m 3 ) .
4.
Conclusions
From our studies, we can conclude first: (1) T h e Cluster Fusion Theory was elaborated to give numerical results, and revealed t h a t anomalous experimental results were explained by Clean Fusion with 4 H e Ash, and TSC-induced Nuclear Reactions including Selective Transmutation and Cleaner Fission. (2) Experimental results show the existence of linked phenomena between nuclear physics and condensed m a t t e r physics. (3) T h e E Q P E T theory was applied for H / D mixed systems t o estimate 3 H e production rates in addition to 4 H e production. Second, T S C was proposed as Seed of Condensed M a t t e r Nuclear Effects. And we m a y speculate future studies: (4) Further studies on TSC-induced nuclear effects are likely, since the S T T B A model has well explained the Ni + H experiment transmutations. (5) W h e n the principles of Clean Fusion, Cleaner Fission and Transmutation are established, we can be very hopeful they will be applicable to portable energy sources and radioactive waste incineration.
Acknowledgment T h e author is grateful to Dr. Francesco Celani, INFN Frascati, Prof. George H. Miley, University of Illinois, and Dr. Yasuhiro Iwamura, Mitsubishi Heavy Industry for their kind discussions.
References 1. A. Takahashi, Mechanism of deuteron cluster fusion by EQPET model, in Proceedings of the ICCF10, in press, http://www.lenr-canr.org/. 2. A. Takahashi, Clean fusion by tetrahedral and octahedral symmetric condensations, in Proceedings of the JCF5, pp. 74-78, http://wwwcf.elc.iwate-u.ac.jp/jcf/. 3. A. Takahashi, Deuteron cluster fusion and ash, in Proceedings of the ASTI5, http://www.iscmns.org/. 4. Y. Arata, et al, in Proceedings of the ICCF10,(Cambridge, MA, USA) Internet Version, August 24-29, 2003, http://www.lenr-canr.org.
742
5. 6. 7. 8.
A. Takahashi, et al., Fusion Technol, 27, 71 (1995). M. Ohta, Private communication, 2004. G. Miley, J. Patterson, J. New Energy 1(3) p. 5 (1996). E. Campari, et al., Surface analysis of hydrogen loaded nickel alloys, in Proceedings of the ASTI5, 2004, see http://www.iscmns.org, This paper is submitted to Proceedings of ICCF11 (Marseilles, France, Nov. 1-5, 2004).
P H O N O N - E X C H A N G E MODELS: SOME N E W RESULTS
PETER L. HAGELSTEIN Research Laboratory of Electronics, Massachusetts Institute of Technology, Cambridge, MA 02139, USA and Spindletop Corporation, Mountain View, CA 94040, USA E-mail: [email protected] We have continued our studies on phonon-exchange models. Here we address the question of the deuteron-deuteron separation, and what materials maximize overlap and concentration. A new figure of merit is proposed that depends on the D2 concentration to the 3/2 power and the square root of the fusion rate. We present a simplified picture of the dynamics in which we separate the problems of excitation transfer and energy coupling between nuclear and low energy degrees of freedom. The dynamics of the excitation transfer in a simple unbalanced model is presented. A new classical picture for coupling with phonons is discussed. We examine an excess heat example with the unbalanced excitation transfer model.
1. I n t r o d u c t i o n In recent years the focus of our theoretical effort on anomalies in metal deuterides has focused on coupled nuclear and phonon models. 1 ' 2 T h e premise of the model is t h a t if condensed m a t t e r effects are taken into account at the outset of a nuclear calculation, t h e n t h e new effects responsible for t h e anomalies are included in a natural way. T h e most significant of the new effects are new site-other-site interactions, in which nuclei at one site are coupled to nuclei at other sites through phonon exchange with a common highly excited phonon mode. Over the years, we have p u t in much effort trying to understand the new models, and trying to see whether there are connections with experimental observations. In a lengthy write-up in the ICCF10 proceedings, we described the underpinnings for the model (and the associated ideas), and discussed what we viewed as connections with a wide variety of experimental observations. 3 Theoretical issues t h a t have been considered so far include: • Generalization of the resonating group method to include the lattice ' or other kinds of condensed matter effects. • Observation that deuterium in a molecular D2 state within condensed matter is required to drive reactions within the D2/ He reaction pathway. • Initial study of phonon exchange in the case of a scalar Gaussian nuclear model. • Initial formulation of phonon exchange in the two-site problem. 743
744
• Formulation of uniform many-site models based on reduced three- and four-level models at each site. • Quantum flow analysis of the probability distribution for a coupled phonon and multi-site (nuclear) two-level system, which provided evidence that nuclear energy can couple efficiently to a highly excited phonon mode. As in any area of applied science, the experimental observations must come first, and theory must find a way to account for the observations in a way consistent with our understanding from other disciplines. T h e new models are born consistent with known nuclear physics and condensed m a t t e r physics, as these are constituents of the new model. T h e model appears to be relevant to a wide variety of experimental observations in the cold fusion field, as we have discussed previously. 3 Some of the specific connections with experiment t h a t we have proposed include: • A connection between experimental conditions in cold fusion experiments with metal deuterides between positive results and large molecular D2 concentration within the condensed matter environment. • A connection between the model provision for highly excited phonon modes, and the apparent need for stimulation (or triggering) in the experiments. For example, the observation that the flow of a deuterium flux inside the solid seems to stimulate reactions in many experiments, as connected to the physical statement that such a deuterium flux is efficient in generating phonons. • A connection between the model prediction that reaction energy can be exchanged between reactions occuring at different sites, and the observation of low-level fast alpha ejection from metal deuterides. • A connection between the model prediction of the transfer of excitation due to phonon-induced reduction of molecular deuterium in the metal to He (D2 —> n + He —> He) to other sites, producing localized mass 4 states arising from the promotion of He, and the new three-body reaction observed by Kasagi. • A connection between model predictions of efficient coupling between nuclear and phononic degrees of freedom, and the observation of quantitative (slow) He generation correlated with energy production. ' • A similar connection in the case of slow tritium production, and the absence of an associated slow neutron production channel. • The models are consistent with the existence of a single new physical process that is at the heart of the new effects, and that which reaction products are expressed depend on which regime the experiment operates in. For example, the model suggests that low-level dd-fusion products are seen at low phonon excitation, and under conditions where the coupling is not so strong, and that excess heat and helium production occurs at higher phonon excitation where the coupling is strong. In electrochemical experiments, neutron emission is seen at relatively low current density (20-30 mA/cm ), and in metal deuterides that are incompletely loaded. Excess heat is observed when cathodes are much more highly loaded, and when the current density is elevated (200mA/cm ). a This is discussed in Ref. 8. a
These specific numbers are for Fleischmann-Pons type experiments near room temperature. It is known that the current density threshold for heat depends on geometry and other conditions of the experiment.
745
2. Double Occupancy in Metal Deuterides We have discussed previously the presence of deuterium in what amounts to a molecular state within the condensed matter environment, as the tunneling matrix element is reduced by many orders of magnitude if this condition is not satisfied. We are interested here in some of the consequences that result. The thermodynamics of hydrogen atoms in metals has a long history, with a primary focus on the solubility of hydrogen in metals in equilibrium with molecular hydrogen gas. Hydrogen solubility in the case of palladium was understood at a basic level many years ago by Lacher.9 In this model, the dependence of the hydrogen binding energy in the metal on hydrogen loading was taken into account, generalizing previous results, and resulting in reasonably good agreement with experiment. We are interested here in the question of double occupancy for palladium deuteride, since we presume that to within an excellent approximation deuterons not in close proximity do not participate in the new processes that we are interested in. For this calculation, we can determine the occupation probability (of a single site) from P[21
£j(.i,) » e - < ^ - W * B T
.
W
where gj is the statistical weight of state j , Ej the state energy, Nj the number of deuterons in the state, and ji is the chemical potential of the deuteron. To proceed, we need simply to enumerate the states and their associated weights and energies. However, there is very little relevant data available for the states, and almost no relevant models for the energy levels in the case of double occupancy. Hence, an alternative strategy is called for. We, therefore, turn our attention to the loading as a function of the chemical potential, which will aid us later on. If we assume that the fraction of deuterons in states with double occupancy is small, and also that tetrahedral site occupation can be neglected, then the probability that a site is occupied is 3 e -(B D -M)/fcBT
PW
(2)
= i + ae-C^-zW-
If we identify x with the single-site occupation probability p[D], then we may express the term containing the chemical potential in terms of the loading
**
"
l-p[D]
"
l-x
[3)
Using a similar approximation, we can estimate the probability of double occupancy to be „rn 1 — ^ j
(D 2 only) VJ
,.,
746
We eliminate the chemical potential to give
PP2]
x2
1 g
1
g3e-^~2E^'k*T.
]T
(5)
j (D 2 only)
At this point, we cannot make much progress without making use of results from much more sophisticated models, or from experiment. Our thinking is that double occupancy in bulk Pd is not favorable, as the energy difference Ej — 2ED (which is essentially a D2 binding energy within the metal deuteride) is probably positive and large. Such a conclusion was reached in the density functional calculations of Sun and Tomanek 10 , and also in other calculations as well (see Refs. 11-16). We note that the D2 molecular state in bulk Pd in these calculations is also unstable; hence if we are to proceed, we need to modify our thoughts on where molecular D2 states are found.b To proceed, we first note that the summation can be divided into ortho- and para-deuterium contributions
53 j (D2 only)
gjQj = 6 Yl (2Z + l)Qz + 3 £ I, even
(21 + 1)Q,.
(6)
/, odd
This corresponds to the fact that even angular momentum states occur only for total nuclear spin S = 0, 2, and that odd angular momentum states occur only for total nuclear spin 5 = 1 (see Ref. 18). The molecular ground state (I = 0) has a larger tunneling matrix element than that associated with higher rotational angular momentum states. Consequently, it makes sense to focus on the I = 0 molecular ground state, in which case we may write
p[D2,GS] = I
e-(E0-2Eo)/kBT^
,ys
1
From the local density approximation results, the energy difference EQ — 2E-Q is of the order of 1 eV or greater, which precludes any significant fractional occupation in bulk Pd. In the Appendix, we examine a much simplified model for confined D2, from which we conclude that the electronic contribution is dominant in the determination of EQ — 2ED in the local density approximation calculations. This will presumably be different depending on the local chemical environment. Our expectation is that the D2 state is less exothermic in the vicinity of a host lattice atom vacancy. There exist calculations specific to hydrogen and deuterium near such a defect (see Refs. 19-21), but useful estimates of EQ — 2ED are not presently available. In the absence of relevant excitation energy estimates from the literature, we are tempted to turn to experimental results in excess heat experiments, where activation b
Some think that there is at present little evidence supporting the notion that the anomalies are associated with bulk P d . 1 7
747
energies have been measured. The exeess heal is observed to have a local dependence on t e m p e r a t u r e of the form P
~
,,-AEA-BT
where AE is 670 meV as reported by S t o r m s 2 2 in an electrochemical experiment, C30meV by Swartz 2 3 in an electrochemical experiment, and oGOnieV as reported by Case2"1 in a gas loading experiment. If one asserts thai Ihe excess power is linear in the D2 concentration, then these activation energies should be interpreted directly in terms of a promotion energy. Later on in this paper, we will discuss unbalanced excitation transfer between D 2 and many host nuclei, in which the maximum associated rate is proportional to the 3/2 power [so t h a t Px3 ~ e x p { - ( 3 / 2 ) ( £ , 0 2ED)/kBT}]. In this case we would take E0 - 2ED
= 370-450 meV.
In Fig. 1, we show the fractional occupation of sites with excitation energy of 410 m e V according to Eq. (7), with no account taken of how many such sites are present. One sees t h a t near room temperature, the fractional occupation increases rapidly as the loading increases above 0.90. In our view, defects appear near the
10~ 6
1CT5
0.2
10~ 4
0.4
0.6
1(T 3
0.8
D/Pd Figure 1. Fractional occupation of accessible D2 sites a t 410 meV in Pd (estimated for sites with a single host I'd vacancy), as a function of temperature on the vertical axis, and loading ratio on the horizontal axis. Although labeled as D / P d . in the case of high defect density, the formula would refer to the ratio of deuterium concentration to octahedral site concentration.
748
surface of PdD in time in the course of the Fleischmann-Pons experiment, which provide a high concentration of relevant sites. Under conditions of high loading, the associated high chemical potential produces strong double occupancy, which leads to excess heat production. In the Case experiment, the temperature is elevated to 500 K or higher, which at four atmospheres would produce a loading of about 0.12 in pure Pd (and perhaps higher loading in the defective structure of the Pd coating). If so, then the two experiments (Case and Fleischmann-Pons) which both produce excess heat begin to appear to be in somewhat similar operating regimes, if one accepts that D2 occupation is critical rather than loading. 3. Transition Metal Dihydrogen Complexes The relative difficulty of achieving a high D2 occupation in metal deuterides suggests that we should be looking for alternate routes to develop useful samples for cold fusion experiments and applications. The simplest solution to the problem should be in the use of solids which contain molecular D2 (or HD in the case of the protondeuteron pathway) as a primary constituent. This suggestion leads immediately to recent work in inorganic chemistry, as we discuss briefly. Hydrogen bonding in molecules and solids has a very long history, and over many decades there was no indication that two hydrogen atoms could develop sigma bonding in a molecule or complex. However, such in 1983 it was shown that intact molecular H2 could bond more or less as a molecule to a transition metal complex.25 In recent years, research on dihydrogen molecular complexes has been an important area of inorganic chemistry, with a large number of examples, and also with corresponding IR and NMR studies that help clarify the local interaction between the protons. Dihydrogen molecule complexes span a continuous range of behavior from near molecular behavior to near dihydride behavior. The separation between protons in H 2 is 0.74 A. The separation between protons in the complex Cr(CO)3(P/Pr 3 )2(H 2 ) is measured by solid state NMR to be 0.85 A. Separation distances in more classical transition metal dihydrides are on the order of 1.6 A. Examples of some dihydrogen complexes are given in Table 1. There are issues associated with the X-ray and neutron measurements that have to do with libration correction, which can lead to an underestimate of the proton-proton distance. This is Table 1. Selected results for dHH(^)> from G. J. Kubas, Metal Dihydrogen and a-Bond Complexes. Complex
X-ray
Cr(CO) 3 (P/Pr 3 )2(H2) Mo(CO)(dppe)2(H 2 ) W(CO)3(P/Pr3)2(H2) FeH(H2)(PEtPh2)3 [RuH(H 2 )(dppe) 2 ]+ Cr(CO)3P2(H2) Mo(CO)3P2(H2)
0.67(5) 0.75(16) 0.821(10)
Neutron 0.84 0.82(1) 0.88-0.90 0.94
Solid-state NMR
Solution NMR
0.85 0.88 0.89
0.84-0.85 0.85-0.87 0.86-0.88
0.85 0.87
749
one factor in the appearance of smaller numbers associated with the X-ray and neutron diffraction results. The use of isotopic metal dihydrogen complexes in cold fusion experiments seems to be an interesting prospect. The fractional occupation of D 2 in these materials will be much greater than in metal deuterides, and there are advantages in working with a well-studied material in which the separation distance is known. One question of interest in such a venture is how much is the tunneling matrix element reduced in these systems? To estimate this, we take advantage of the interpolation formula of Bracci and coworkers26 which in the case of the dd-reaction can be written in the form -i 3 / 2
l{d)
= kxC
H ao mP d
-ko
exp
A*
a
o\
me d J
(8)
where k\ = 3 x 10 c m - 3 , C is the reaction constant 1.5 x 10~ , k2 is a fitting constant (which is 3.51 for D2 and 3.41 for D j ) , \i is the reduced mass of the nuclei, m e is the electron mass, and ao is the Bohr radius. We have modified this formula by making k^ an explicit function of d
fe(d)
3.51(2.00 - d/ap) + 3.41 (d/a 0 - 1.40) 2.00 - 1.40 '
(9)
In addition, we have added 0.40 to the Logio of the rate in per second to obtain slightly better agreement with accurate calculations. One sees from Fig. 2 that the fusion rate is reduced by roughly 4-6 orders of magnitude relative to D2 in these
4HH
(A)
Figure 2. Fusion rate for D2 and D j (filled squares), modified Bracci approximation (line), and rate estimates for isotopic metal dihydrogen complexes with separation distances of 0.85, 0.87, 0.88, and 0.89 A.
750
systems. The matrix element is reduced by 2-3 orders of magnitude relative to that of D2. We note that simply obtaining a high occupation fraction of D2 and low deuteron-deuteron separation are not the only requirements for obtaining cold fusion effects from our modeling. Other requirements will be discussed later on in this paper. 4. Molecular D e u t e r i u m in Solids Another way to arrange for molecular D 2 to be present in a condensed matter environment is to take advantage of the finite solubility that is naturally available. For example, H2 is soluble in heavy ice (as cited in Ref. 27) at a level of 9.4 x 1(T 4 M/atom at 0°C. The rotational energy of H2 as measured by neutron scattering is less than that for free H2, which can be interpreted in terms of an increase in the proton-proton separation. According to Ref. 27, the reduction is about 3%, which is consistent with an increase of the proton-proton separation by 1.3 A. This is interesting, because it is much closer to the pure molecular H2 separation than we have seen in earlier examples, and leads to a coupling matrix element 2-3 orders of magnitude larger than in the case of isotopic dihydrogen compounds. In the case of H 2 in solid argon, spectroscopic observations are consistent with an increase in the equilibrium separation from free H2 by 0.0028 A, 28 which is indicative of an even weaker interaction as expected. As remarked above, the formation of sites with double hydrogen occupancy in palladium hydride is enhanced in the presence of defects (specifically, single atom host lattice vacancies). According to Pavesi and Gianozzi, hydrogen in GaAs forms molecular H2 in tetrahedral sites, which are deep wells for the molecular state. 29 Linn Hobbs has suggested that molecular hydrogen goes into vacancies in NaCl (Private communication). Theoretical studies for hydrogen in silicon indicate that molecular H2 should form in Si. 30 ' 31 The implication is that if these materials are loaded with deuterium, presumably at high deuterium pressure and temperature that molecular states will form in the bulk. The kinetics of this process according to these results is much favored energetically over the case of PdD once the deuterium is in the lattice. However, it is expected that the solubility of hydrogen in the semiconductors will be much less. 5. Caged D 2 Since it was announced that Ceo occurs as a fullerene, chemists have sought to develop materials in which various atoms or molecules are isolated within the interior of the cage of the fullerene. Over the years, research efforts have focused on the possibility of including molecular H2 in the interior of a fullerene, with mostly limited success until recently. Previous work on inert gas encapsulation involved heating the fullerenes in a rare gas atmosphere 32 (which produced a very low yield) and acceleration of rare gas atoms into stationary fullerenes. In the latter case, the atom could slip through the cage with sufficient noble gas atom velocity, and be
751
encapsulated with significantly higher yield. The encapsulation of 3 He and 4 He has been reported through this method. Methods to purify fullerenes with encapsulated atoms are discussed in Ref. 33. In 2003, Murata and colleagues published a paper claiming a method that allowed for 100% yield of molecular hydrogen into an open-cage fullerene derivative, 34 and gas phase generation of H2 in CQO. A discussion of the issues associated with such an open-cage structure, and the synthesis of this structure, is discussed in Ref. 35. The encapsulation of H2 in the open-cage structure was achieved by exposing a powder made of the open-cage fullerene to 800 atmospheres of H2 at 200° C for 8h. No loss of H 2 from the open-cage structure in a solution was observed at room temperature over 3 months, and H2 release was observed at 160°C and above. These results imply the possibility of working with D2 or HD encapsulated open-cage fullerene structures in solution (see Section 6 on the use of liquids), as reported in Ref. 34 or with D 2 or HD in closed cage structures in solution or as solid structures. Molecular H 2 , HD and D 2 encapsulated in Ceo was studied using NMR by Tomaselli and Meier.36 Prom the results of this study, one concludes that the molecular ground state within the cage is very nearly the same as in the free case. A relatively small crystal field splitting is observed for the first rotational states, where the first rotational state energy for HD is split to roughly 92 and 99 c m - 1 as compared to the free space value of 89.4 c m - 1 . Rubin and coworkers also studied encapsulated molecular hydrogen in an open cage fullerene by NMR. 37 In this work, the NMR signal for ground state HD inside the cage was split into a triplet with an associated coupling constant of 41.8 Hz, which is somewhat less than the free HD value of 43.2 Hz (which indicates that the proton-deuteron separation is close between the two cases). This can be compared with a similar splitting in the case of a deuterated dihydrogen complex W(CO)3(P/Pr 3 ) 2 (HD), where the coupling constant is 33.5 Hz, and the proton-proton separation is reported to be 0.89 A. Fullerenes have been made into solid structures through a variety of methods (as described in Ref. 38). Crystalline powders of C6o were found by X-ray diffraction to form random collections of hep and fee lattice structures formed of nearly spherical fullerenes with interstitial spaces (that can be filled). The formation of similar solids is expected in the case of D 2 and HD encapsulation. Intercalated fullerides are known, in which various atoms are placed into the interstices, which can lead to interesting physical effects such as superconductivity (as observed in alkali fullerides). Such materials can be produced with D 2 and HD encapsulation, and would be interesting for cold fusion applications. Polymerized fullerides are perhaps more interesting, due to the possibility of increased stability at elevated temperature, which would be important in the case of D2 and HD encapsulation for excess heat generation and other applications which for one reason or another must be carried out at high temperature. For example, Prassides and Margadonna present data for polymerized CsCeo as a function of temperature illustrating the different phases up to about 475 K. 38 Heterofullerenes, in which one or more carbon atoms
752
in a fullerene are substituted, are potentially interesting as the resulting structures are stable at very high pressure (which is interesting by itself, especially if the cages contain D 2 or HD, and perhaps interesting additionally if the D 2 or HD loading is maintained in part through a pressurized atmosphere).
6. Deuterium in Liquids There appears to be nothing within the models that we have studied that would prevent reactions taking place in a liquid, as long as the phonon excitation involves a relatively long wavelength such that nuclei do not move away from an amplitude maximum quickly. Metal dihydrogen complexes can occur in solution as one approach. Additionally, D2 is known to go into liquid solution with significant solubility under a pressurized deuterium gas atmosphere. In Fig. 3 we show solubility data for H2 (the solubility for D 2 is expected to be very similar). On observes that there are large differences in the H 2 solubility for different liquids - water is not very good in this regard, and cyclohexane is the best of the group shown. It might reasonably be asked whether D 2 in a liquid is similar to free D 2 . The rotational Raman spectrum of H2 in water was presented in Ref. 39. The focus in this work was on the question of the Raman line shape, which is broadened in the liquid environment. A comparison of the spectrum in water as compared with gas presented in this work shows a shift of about 5%, which is consistent with a change in the separation by about 0.019 A, indicative that the low-lying states in liquid are not very different from those in free space. This is encouraging.
o O
10
100
1000
Pressure (atm) Figure 3.
H2 concentration (cm
3
) in various liquids as a function of H2 pressure (atm).
753
7. Proposed Figure of Merit As a step toward evaluating candidate materials for cold fusion research, it is of interest to develop a measure of how good one material is relative to another material. If we focus only on the issues of how much molecular deuterium there is, and on how large the tunneling matrix element is, then we can develop a figure of merit that can be used to characterize a material with respect to these issues.0 According to our modeling, excess power should go as the three-half power of the number of D2 molecules embedded in condensed matter, and linear in the tunneling matrix element. Consequently, it seems reasonable to adopt a figure of merit that is proportional to (concentration) 3 / 2 , and also proportional to the square root of the conventional fusion rate. We define a figure of merit for the D D ^ 4 H e path defined according to
™D 2 -DD 'DD
We normalize the fusion rate 700 in this case to that of molecular D 2 (T D D)) for which accurate theoretical estimates exist. We normalize the concentration TIDD to that of solid molecular deuterium (rip D ), which has a known and large concentration. Table 2.
Figure of merit for selected materials.
Material D 2 (solid) D2 (liquid) D 2 at 100 atm in cyclohexane D2 at C60 Cr(CO)3(P/Pr 3 )2(D 2 ) W(CO)3(P/Pr3)2(D2) Fleischmann-Pons
Concentration (cm-3) 6.0 x 4.9 x 2.5 x 1.4 x 2.6 x 2.6 x 10 1 9
10 2 2 10 2 2 10 2 1 10 2 1 10 2 1 10 2 1
d
TDD
(A) 0.74 0.74 0.76 0.75 0.85 0.89 0.85?
1.0 0.74 3.0 x 1 0 - 3 2.1 x 1 0 - 3 3.5 x 1 0 " 5 5.4 x 10~ 6 8 x 10-9
A short table of selected candidates has been developed in Table 2. One sees that the figure of merit for liquid deuterium is close to that of solid deuterium, but is reduced because of the density. D2 in cyclohexane looks extremely interesting under the assumption that the deuteron-deuteron separation is close to that of D2 in water. D2 encapsulated in Ceo is also very interesting. In these cases, it is primarily the concentration effect that brings down the figure of merit. The isotopic transition metal deuterides are hindered because of the larger deuterondeuteron spacing. It would be reasonable to ask what the associated figure of merit c
We note that there are other issues as well; hence, we will not be developing a more universal figure of merit at this point.
754
Acceleration of dynamics
Figure 4. Illustration indicating that coherent acceleration is achieved when many two-level systems that make downward transitions are coupled to many two-levels systems that make upward transitions.
is for the Fleischmann-Pons experiment, or the Szpak experiment. If the observed dependence of the heat effect is in fact due to a requirement for excitation to D2 states as we have conjectured, then the D2 concentration may be as large as a few times 1019 c m - 3 . The deuteron-deuteron separation is unknown at present. If we assume an optimistic separation of 0.85 A, then the resulting figure of merit will be on the general order of 1 0 - 8 . 8. Reaction Dynamics and Decoupling The problem of reaction dynamics is in general complicated but quite interesting. Our purpose in this section is to discuss a simple way of looking at the problem which may allow us to enhance our understanding. We begin by looking at the different functions which are required. In the most basic view, there are three issues at hand: (1) tunneling of molecular D2 in the condensed matter to He; (2) transfer of excitation from this tunneling to other species; (3) transfer of energy from the nuclear system to other degrees of freedom. In what follows, we will separate the population dynamics from the coupling of the energy to the condensed matter. This will be a tremendously helpful separation conceptually. 9. Excitation Transfer To obtain an accelerated tunneling rate, we want a coherent enhancement as was discussed in papers presented at ICCF10 (Refs. 3 and 40). Such an enhancement, can be achieved using a collection of two-level systems that make a downward
755
transition, with equal coupling to a common oscillator (or other extended quantum system), and a second collection of two-level systems that make an upward transition through coupling to the same common oscillator. This is illustrated in Fig. 4. This is a many-site version of quantum excitation transfer, which we have remarked on in previous publications. We note here that resonant excitation transfer is presently an active area of research, as can be seen from Ref. 41. Given this approach, the question arises as to what equivalent two-level systems we should consider. For the initial set, we take the molecular D2 states embedded in condensed matter as the upper state, and 4 He as the ground state. For the second set, other systems can be considered. We have considered two general kinds of states for the second set. In one case, excitation from 4 He to n + 3 He compact states is a reasonably natural choice, as it is possible to have angular-momentum stabilized compact states in the general vicinity of the D2 energy. The resulting picture is illustrated in Fig. 5. We have focused on compact states with a free neutron, as in this case the lattice sees a different mass locally since the neutron is no longer part of the lattice. This is illustrated in Fig. 6. In this case, the neutron and 3 He initially have the same position and velocity as the 4 He, but the lattice accelerates the 3 He nucleus differently than would have been the case for 4 He. This generates angular momentum, as can be seen in the classical equivalent case illustrated in the figure. We note that the process will be virtual, so all such states must be included in the interaction; only low momentum intermediate states will behave something like indicated in the figure, and their contribution is thought to give rise to the new effects. The second kind of states which may accept the excitation are similar states in other nuclei within the condensed matter. For example, in the case of PdD experiments, there are analogous transitions in Pd which are expected to show a similar Massive excitation transfer I Compact n+3He Compact
^He
«He
4
DD/ He system transferring to ^He/compact state system
Figure 5. Specific example in of coherent excitation transfer scheme where molecular D2 states transition through n + 3 H e states to make 4 He states, with the excitation being transferee! to n + 3 He compact states. We note that it is more likely that a similar mechanism involving host metal nuclei on the RHS occurs in the Fleischmann-Pons experiment.
756
behaviour. In this case, one or more neutrons are removed from a Pd nucleus to form a high angular momentum compact state, with a similar mechanism used to transfer angular momentum from the compact state. We note that the coupling would be strongest in the event that many neutrons came together to form a cluster 42 in this intermediate state. There is at present significant experimental evidence in support of neutron cluster emission from experiments with metal deuterides and hydrides. For example, Oriani presented results from electrochemical experiments in which charged particle detection was made with CR-39 some distance away from the cathode. Charged particles were observed under conditions where they could not have originated in the cathode. 4 3 - 4 5 Fisher has suggested that these effects may be due to neutron clusters, which would penetrate as observed, and could also give rise to charged particle emission as observed.46 We agree with Fisher that neutron clusters are most likely involved in such experiments, but in our view the mechanism through which they are formed is related to the mechanism under discussion here rather than the mechanism discussed by Fisher. 10. Dynamics The many-site problem that comes out of the lattice resonating group method is very complicated, and we have sought to simplify the picture. In this paper, we propose a quite drastic simplification which may be useful. On the one hand, there is excitation transfer from the D2 molecular state to excited states of other nuclei. On the other hand, there is coupling to a highly excited low energy mode, which exchanges nuclear energy for phononic energy, or energy in other modes. Both occur at the same time, which makes the problem quite complicated. As discussed here we simply separate the two functions, and look at each individually. Duschinsky in simple terms
4
He
4
Hein
initial state
J
He 3
He +n in
final state
3
He looks different to the latice and accelerates
Duschinsky mechanism can produce phonon and angular momentum exchange
Figure 6. Cartoon version of phonon exchange with angular momentum exchange in the case of an intermediate compact state with a free neutron. We note that similar coupling mechanism exists for other nuclei in which a neutral partner is separated.
757
We consider here the transfer of excitation from the D2 states to resonant compact states composed of a daughter nucleus with a neutral partner with high angular momentum. We do not expect a precise resonance to occur, so we imagine that either through some phonon exchange or other routes that a suitable response of the lattice and nuclear system occurs at a matched frequency, that we can think about in terms of an equivalent matched two-level Dicke system. We analyzed the dynamics of this kind of system previously in the case of matched populations. i - 4 " Here, we are interested in what happens when the populations are not matched. In this case, we assume that there occur appropriate resonant states in the host lattice, and that there are many more nuclei of which ever isotope has the best match than there are D2 molecules. In this case, we have an unbalanced coherent Dicke transfer. Resonant excitation transfer occurs in this system much the same as in the case of the matched case we reported on earlier. Results for a representative calculation are shown in Fig. 7. One sees in this calculation that the population stays localized in the initial state for some time, ami then a rapid transition of the excitation from one two-level system to the other occurs. In the matched system, the excitation stayed for a significant time in the other two-level. In the unmatched system, the population returns rather quickly back to the initial state. This is quite interesting. From the
O.0O0
0.001
0.002
0.003
0.004
0.005
0.006
0.007
0.008
Figure 7. Excitation transfer dynamics for 200 two-level systems initially excited transferring population to 10.000 two-level systems initially in the ground state.
758
0.001
0.002
0.003
0.004
0.005
0.006
G
Wr t Figure 8. Rate as a function of time for the unbalanced Dicke coherent excitation transfer calculation shown in Fig. 7.
results of many calculations, this behavior is repeated with essentially only a change in scale factor. We find that
rn
G
3 / 2 ^ 1 / 2 VeJv host"
fr
(11) h The associated transition rate as a function of time is illustrated in Fig. 8. One of the effects of phonon exchange that we will consider shortly will be to dump the energy associated with the excited state population of the nuclei that accept the excitation. This will prevent the system from returning to the initial state in which the first system is mostly in the D2 upper state. 11. Energy Exchange with Phonons The second part of the simplification discussed in the previous section involved the coupling of energy between the nuclear system and other lower-energy degrees of freedom. Here we will focus on coupling to a highly excited phonon mode. d The lattice generalization of the resonating group method leads to a picture in which excitation is transferred rapidly from on site to another, with a small amount of phonon exchange occuring with every site change. We examined a model for the associated energy exchange previously using a quantum flow calculation, which suggested that this mechanism for energy exchange between the two quantum systmes is very efficient. Here, we are interested in a different model for energy exchange. d Qualities of the highly excited phonon mode appear to be different for the initial excitation transfer as discussed above (where a single mode interacting with all nuclei is best) and for energy transfer (where more localized modes may be useful since the coupling is much stronger).
759
Suppose that the phonon mode in question has regions where the vibrational motion is locally large, and other regions in which the vibrational motion is much less. Suppose also that the hopping of excitation from site to site is effective, so that the excitation is able to move between the two regions over an oscillation cycle. In this case, we have the possibility of using classical estimates to determine the maximum rate at which net energy exchange occurs. The natural associated classical picture that is suggested is that where excitation is present, the excited nuclei look lighter to the condensed matter (since neutral particles are effectively decoupled) . If the excitation oscillates between regions of high vibrational amplitude and low vibrational amplitude, then this can produce net energy gain in the condensed matter. We can estimate how much in the case of lattice vibrations through the following calculation |PJ )|2 " W 2m2Jt) dt
^ + £"«<'> s £ ( f ) = s E 2mj{t) %<j
).
(12)
The maximum power increase is obtained with when the mass decreases during maximum kinetic energy, which can occur with mass modulation at twice the mode frequency. In this case, an estimate for the maximum power is
Pmax
~ \r^
U o E o
'
(13)
where /* is the fraction of nuclei that are excited, Am/M the fractional mass difference due to the presence of excitation, Wo the oscillation frequency, and EQ is the mode energy. This result motivates us to think further about the associated dynamics. If we were to match the number of D2 molecules involved substantially to the number of nuclei that can accept the excitation, then we would end up with an inverted two-level system which we now imagine is to dump its excitation to the phonon mode. In this case, we would expect the associated dynamics to resemble that of laser dynamics, in that net gain should be present for all highly excited modes such that / * A m / 4 M is greater than the Q of the mode. Net gain should be present transiently also if the number of accepting nuclei is less than the number of D2 molecules, or greater by less than 2. In either case, one would expect that the nuclei would make use of the above mechanism to dump energy, and that phonon amplification should occur. If the initial and final sets are not well matched such that there are more nuclei accepting excitation, then the dynamics presented above indicates that a significant compact state excitation will be present, but no inversion and no gain. Under these conditions, the excited nuclei would couple incoherently as a very hot source, with an associated power transfer rate that would depend on the strength of excitation of the modes. To match the number of D2 molecules in condensed matter to the number of nuclei that can accept the excitation is not easy to do in a metal deuteride. However,
760
if we assume that carbon and other low mass nuclei are not well-matched at 24 MeV, then it may become possible to take advantage of isotopic dihydrogen compounds for this purpose. An isotopic transition metal dihydrogen compound can have one metal atom per D2 molecule, which leads to matched populations. In the case of fullerenebased systems, it would be possible to match the concentration of encapsulated D2 with the concentration of encapsulated heavy atoms that can accept the excitation (e.g., Kr or Xe in the case of noble gases). Alternatively, in fullerene polymers, it is possible to include heavier atoms interstitially so that the number of such atoms is matched to the number of buckyballs, which satisfies the gain condition if D2 is encapsulated in some fraction of the buckyballs.
12. Excess Heat Example Armed with the results in the previous sections, it seems reasonable to revisit the heat pulse calculation that we presented in Ref. 3. To proceed, we require an estimate for the tunneling factor e~ G . It is possible to make use published results for the molecular D2 problem. We may write
|-0CO)|2 =
P-2G
,
(14)
Wmol
where vmo\ is the volume associated with the molecule. It is possible to develop an estimate for |?/J(0)| 2 from calculations of 7DD, combined with the reaction constant
7DD
= A^(0)\2,
(15)
where A is 1.5 x 10" 1 6 c m ~ 3 s _ 1 . This gives |^(0)| 2 to be 2.0 x 1CT48 c m - 3 . If we take f mo i to be 1.4 x 10~ 24 cm 3 , we conclude that e~ G = 1.7 x 1(T 36 for free molecular D2. To be consistent with this way of looking at things, we revise our rate formula to read r
S
ATS/2AT1/2
r max ~ -ND{ N
lvnuc Ue~G
^
—
—
,
(16)
where U is the effective interaction strength for the coupled reactions measured on a nuclear volume wnUcIn the example discussed last year, we selected a heat pulse that lasted 5 h, and had a maximum reaction rate of 1012 s _ 1 to produce 5.65 x 1016 final state 4 He nuclei. We can analyze the reaction rate formula for self-consistency as follows. The deuteron-deuteron separation distance d is not well known in the experiment, so we will adopt it as a parameter. We also do not know whether all of the host nuclei participate, or whether only a few matched isotopes participate. Hence, we
761
determine the number needed as a function of the separation distance, matching the peak reaction rate
JVw = r L . ^ Atf'A/—^j \ 2 °2
•
(17)
Umol
The result of such a computation is illustrated in Fig. 9. From this figure it is clear that if the deuteron-deuteron separation is 0.85 A or greater, then a large fraction of the host nuclei will have to be involved in the excitation transfer. In a FleischmannPons experiment, the cathode might be 3 mm diameter, and 1-2 cm long, so that the total number of host metal atoms present is in the range of (2.8-5.6) x 10 21 . On the order of 2-4% of them would be needed in the case of a separation of 0.85 A. As single host lattice vacancies are present only within microns of the surface, the participation of host atoms a significant distance away from the surface would need to be involved in this model. 10'
10" -
U=0.03MeV 10'
U=3MeV 10'
10ID|
«• 0.75
0.80
0.85
0.90
of (A) Figure 9.
Number of host nuclei required to produce a maximum reaction rate of 10 1 2 s
13. Conclusions We have continued our studies of new nuclear reactions involving phonon exchange in condensed matter. In this work we have addressed a number of important topics within the theory. Some of the results that are new here include: (1) New materials that have lower deuteron-deuteron separation and high molecular D2 in condensed matter. (2) Modification of published fusion rate results from the literature to evaluate candidate materials.
762
(3) Development of a figure of merit to rate candidate materials. (4) Extension of the approach to include D2 in liquids on the same footing as solids. (5) Models in which the energy exchange between nuclear and low-energy degrees of freedom is decoupled from the excitation transfer associated with accelerated coherent tunneling of the D2. (6) A classical picture for angular momentum exchange with the lattice in the case of compact states involving neutrals. (7) An analysis of transfer dynamics in the case of unbalanced coherent transfer between sets of two-level systems, and estimates for the reaction rate. (8) A classical picture for an energy exchange scheme between nuclei and a highly excited phonon mode. (9) A consistency check of the unbalanced model in the case of an excess heat pulse from a Fleischmann-Pons experiment, which suggests that many host nuclei participate in the excitation transfer process. We remain very interested in the Kasagi 3-body accelerator experiment, 6 in the fast alpha emission experiments, 5 in the search for 3 He, and in experiments t h a t involve lattice excitation mechanisms. T h e use of new materials as discussed here looks particularly promising.
Acknowledgments T h e author acknowledges helpful discussions with, and also the contributions of, his friends and colleagues Michael McKubre, Fran Tanzella, M a t t h e w Trevithick, and Kevin Mullican. Support was provided by Spindletop Corporation. Appendix In this appendix, we are interested in a simplified model for molecular D 2 in a metal deuteride. 6 We take for a Hamiltonian the following
H = -^V? - ^
+ y 1 2 (r 2 - r i ) + ^ ( N ^ M 2 ) .
(18)
We have kinetic energy terms for b o t h deuterons, an interaction potential between the two deuterons, and confining potential terms in the vicinity of the potential minimum of the local well. As is known, this problem separates when center-ofmass and relative coordinates are introduced. 4 7 We take
R- = e
^ 1 +r2),
r = r2 - r i .
Note that H2 in solids and liquids has been of interest in the literature. For example, Henis and coworkers discuss the impact of confinement on the cold fusion rate. 47 Darby et al. discuss a crystal field theory for H2 in relation to the problem of solid hydrogen.48 Hunter et al. have focused on transitions between rotational states to account for the lineshape observed in water.49
763
The time-independent Schrodinger equation £* =
(19)
HV,
separates into
£ R $(R) = - ^ V ^ ( R ) + -(2iO|R|2$(R),
(20)
2M
Er6(r)
-Vim
+ W W + \(K/2)\rU(r),
(21)
where M = Mi + M2,
fi
1
1
Mi
M2
The center of mass ground state is a three-dimensional Gaussian, with an associated energy
IhJ2^.
En[GS] = 1 J
(22)
2 V M
1.5
2.0
3.0
Number of electrons Figure 10. Binding energy per proton as a function of the number of electrons present (filled squares). A parabola has been fit through the three points (solid line).
764
The solution of the relative problem is that of a weakly confined D2 molecule, and we can estimate the energy according to
ET[GS] = £ m o l +
±(K/2)(\r\2).
(23)
We might think of the molecular problem to be similar in some ways to that of the free space version of the model. However, we know from local density approximation calculations that protons and deuterons in this situation share electrons with nearby palladium atoms, so that not all of the electron wavefunctions are available for bonding. 10 This is something like changing the electronic charge in the case of the vacuum version of the problem. To see how this works, consider the variation in charge allowed in the case of H^, H2, and H^, which is shown in Fig. 10. The potential minimum in these three cases (which is approximately equal to (|r| 2 )) is shown in Fig. 11. In this simple model, we can compare the energy of the D2 molecule inside the metal with the energy for two deuterons each in separate locations inside the metal. We obtain
AE
= E[D2] - 2E[D] 1
3
Emo1 + ^K/2)(\r\2) +
r)K
-h]lw
3, K 3^ K -h.\ / — + -h\ / 2 \' M i 2 \ M2
(24)
1.10 1.05 %
1.00 •
c
<
c o 2
0.95 0.90
CO
a. CD CO
c o 2 o I
C
o o
0.85 0.80 • 0.75 0.70 1.0
2.0 Number of electrons
3.0
Figure 11. Separation distance between protons as a function of the number of electrons present (filled squares). A parabola has been fit through the three points (solid line).
765
Since 2K/M — K/M\ = K/M2 = UQ (where fao0 is the harmonic oscillator energy of the parabolic potential well that we have assumed), this simplifies to
A £ = Emol + ^ M ^ d i f ) - |fiw 0 .
(25)
From neutron scattering experiments, we can estimate fkoo to be about 56 meV, and ( 3 / 2 ) ^ 0 is 84 meV. If we assume that (|r| ) is (0.74 A) 2 , then we obtain
iMiwg(|r| 2 > = 210 meV (at 0.74 A). The calculations give a larger proton-proton separation, in one case roughly 0.95 A. For this larger separation, we obtain
~Mi^(|rf)
= 345 meV (at 0.95 A).
We would expect that D2 within the metal should be bound in such a model by several eV. Since it is not in the structure calculations, this is expected to be due to energy offsets due to the electronic part of the problem. It is of interest to try to understand the relatively large separation (or instability) obtained in the calculations published previously (see Refs. 10-16). In terms of the idealized model under discussion here, such a result is due either to too few electrons present (in the general direction of charge 1), or too many electrons present (in the direction of charge 3). From Coehn effect measurements, protons and deuterons act as if they have a fractional charge in the neighborhood of +0.5|e|, which would seem to be consistent with a result to the left of H2 in Fig. 11. However, there are other explanations for the Coehn effect than net positive charge (in fact, Sun and Tomanek see a transfer of net negative charge from Pd to D in their calculations 10 ). The results of Wei and Zunger indicate that contributions from anti-bonding states are responsible for the large inter-deuteron separation distance and instability. Within the simple idealized model under discussion, this situation corresponds more closely with the increased separation associated with H^ in Fig. 11, where there is excess electronic charge and occupation of antibonding states. We have plotted the logarithm of the dd-fusion rate for D 2 with different charges in Fig. 12. Molecular D2 gives the fastest fusion rate as expected; the rate is reduced by 12 orders of magnitude for the D^~ ion. If the reaction rate were linear in the matrix element (as for resonance tunneling models and phonon-coupled models), then one would expect six orders of magnitude difference in the rate.
766
1.5
2.0
Number of electrons
Figure 12. Logio of the dd-fusion rate in sec - 1 from the paper of Bracci et al. for D2 and D^" • We estimated the fusion rate for D^~ using the interpolation formula of Bracci, offset by 0.4 to agree better with the results of Koonin and Nauenberg. The upper solid curve is a simple parabolic fit through the three points; the lower solid curve is obtained using a modified version of the Bracci interpolation using a parabolic approximation for the separation distance.
References 1. P. L. Hagelstein, A unified model for anomalies in metal deuterides, in: Proceedings of the 8th International Conference on Cold Fusion (Lerici, La Spezia, Italy, May 2000), p. 363. 2. P. L. Hagelstein, A unified model for anomalies in metal deuterides, in: Proceedings of the 9th International Conference on Cold Fusion (Beijing, China, May 2002), p. 121. 3. P. L. Hagelstein, Unified phonon-coupled SU(N) models for anomalies in metal deuterides, in: Proceedings of the 10th International Conference on Cold Fusion (Cambridge, MA, USA, August 2003), in press. 4. P. L. Hagelstein, Phonon-induced nuclear reactions, Trans. Am. Nucl. Soc. (2005) in press. 5. A. G. Lipson, G. H. Miley, A. S. Roussetski, and E. I. Saunin, Phenomenon of energetic charged particle emission from hydrogen/deuterium loaded metals, in: Proceedings of the 10th International Conference on Cold Fusion (Cambridge, MA, USA, August 2003), in press. 6. J. Kasagi, T. Ohtsuki, K. Ishu, and M. Hiraga, Phys. Soc. Jpn. 64, 777 (1995). 7. M. H. Miles, Correlation of excess enthalpy and helium-4 production: A review, in: Proceedings of the 10th International Conference on Cold Fusion (Cambridge, MA, USA, August 2003), in press. 8. P. L. Hagelstein, M. C. H. McKubre, D. J. Nagel, T. A. Chubb, and R. J. Hekman, New physical effects in metal deuterides, in: Proceedings of the 11th International Conference on Cold Fusion (Marseilles, France), this proceedings. 9. J. R. Lacher, A theoretical formula for the solubility of hydrogen in palladium, Proc. Roy. Soc. Lond. A 1 6 1 , 525 (1937).
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10. Z. Sun and D. Tomanek, Cold fusion: how close can deuterium atoms come inside palladium, Phys. Rev. Lett. 63, 59 (1989). 11. F. Liu, B. K. Rao, S. N. Khanna, and P. Jena, Nature of short range interactions between deuterium atoms in Pd, Solid State Gommun. 72, 891 (1989). 12. P. K. Lam and R. Yu, Phys. Rev. Lett. 63, 1895 (1989). 13. O. B. Christensen, P. D. Ditlevsen, K. W. Jacobsen, P. Stolze, O. H. Nielsen, and J. K. Norskov, H-H interactions in Pd, Phys. Rev. B 40, 1933 (1989). 14. X. W. Wang, S. G. Louie, and M. L. Cohen, Hydrogen interactions in P d H n (1 < n < 4), Phys. Rev. B 40, 5823 (1989). 15. S.-H. Wei and A. Zunger, Stability of atomic and diatomic hydrogen in fee palladium, Solid State Commun. 73, 327 (1990). 16. A. C. Switendeck, Electronic structure and stability of palladium hydrogen (deuterium) systems, PdH(D)„, 1 < n < 3, J. Less Common Metals 172-174, 1363 (1991). 17. E. Storms, What conditions are required to initiate the LENR effect? in: Proceedings of the 10th International Conference on Cold Fusion (Cambridge, MA, USA, August 2003), in press. 18. H. L. Johnston and E. A. Long, J. Chem. Phys. 2, 389 (1934). 19. P. Nordlander, J. K. Norskov, F. Bessenbacher, and S. M. Myers, Multiple deuterium occupancy of vacancies in Pd and related metals, Phys. Rev. B 40, 1990 (1989). 20. F. Bessenbacher, B. Beck Nielsen, J. K. Norskov, S. M. Myers, and P. Nordlander, Interaction of hydrogen isotopes with metals: deuterium trapped at lattice defects in palladium, J. Fusion Energy 9, 257 (1990). 21. K. Tsuchiya, Y. H. Ohashi, K. Ohashi, M. Fukuchi, Interaction between two neighboring deuterium atoms in palladium, J. Less Common Metals 172—174, 1371 (1991). 22. E. Storms, Some characteristics of heat production using the 'cold fusion' effect, in: T. O. Passell and M. C. H. McKubre (eds.), Proceedings of the Fourth International Conference on Cold Fusion (Maui, Hawaii, December 1993), Vol. 2, p. 4-1. 23. M. R. Swartz, Photo-induced excess heat from laser-irradiated electrically polarized palladium cathodes in D2O, Proceedings of the ICCF10 (Cambridge, MA, 2003). 24. L. Case, in his oral presentation at ICCF10 (2003). 25. G. Kubas, Metal dihydrogen and a-bond complexes (Kluwer Academic/Plenum Publishers, New York, 2001). 26. L. Bracci, G. Fioentini, and G. Mezzorani, Nuclear fusion in moelcular systems, J. Phys. G: Nuclear Physics 16, 83 (1990). 27. Z. Chen, H. L. Strauss, and C.-K. Loong, J. Chem. Phys. 110, 7354 (1999). 28. R. J. Kriegler and H. L. Welsh, The induced infrared fundamental band of hydrogen dissolved in solid argon, Can. J. Phys. 46, 1181 (1968). 29. L. Pavesi and P. Giannozzi, Atomic and molecular hydrogen in gallium arsenide: A theoretical study, Phys, Rev, B 46, 4621 (1992). 30. P. Deak, L. C. Snyder, and J. W. Corbett, State and motion of hydrogen in crystalline silicon, Phys. Rev. B 37, 6887 (1988). 31. C. G. Van de Walle, P. J. H. Denteneer, Y. Bar-Yam, and S. T. Pantelides, Theory of hydrogen diffusion and reactions in crystalline silicon, Phys. Rev. B 39, 10791 (1989). 32. R. J. Cross and M. Sanders, Fullerenes-Fullerenes for the New Millennium, Electrochemical Society Proceedings, Volume 2001-2011, 298 (2001). 33. Y. Kubozono, Encapsulation of an atom into Ceo cage, in: T. Akasaka and S. Nagase (eds.), Endofullerenes, A New Family of Carbon Clusters (Kluwer Academic Publishers, Dordrecht, 2002). 34. Y. Murata, M. Murata, and K. Komatsu, J. Am. Chem. Soc. 125, 7152 (2003). 35. G. Schick, T. Jarrosson, and Y. Rubin, Angew. Chem., Int. Ed. 38, 2360 (1999).
768 36. M. Tomaselli and B. H. Meier, Rotational-state selective nuclear magnetic resonance spectra of hydrogen in a molecular trap, J. Chem. Phys. 115, 11017 (2001). 37. Y. Rubin, T. Jarrosson, G.-W. Wang, M. D. Bartberger, K. N. Houk, G. Schick, M. Saunders, and R. J. Cross, Insertion of helium and molecular hydrogen through the orifice of an open fullerene, Angew. Chem. Int. Ed. 40, 1543 (2001). 38. K. Prassides and S. Margadonna, Structures of Fullerene-Based Solids, in: K. M. Kadish and R. S. Ruoff (eds.), Fidlerenes: Chemistry, Physics, and Technology (Wiley-Interscience, NY, 2000). 39. D. G. Taylor III and H. L. Strauss, The rotational spectrum of H2 in water, J. Chem. Phys. 90, 768 (1989). 40. P. L. Hagelstein, Resonant tunneling and resonant excitation transfer, in: Proceedings of the 10th International Conference on Cold Fusion (Cambridge, MA, USA, August 2003), in press. 41. D. L. Andrews and A. A. Demidov, Resonance Energy Transfer (John Wiley and Sons, New York, 1999). 42. F. M. Marques, M. Labiche, N. A. Orr, et at, Detection of neutron clusters, Phys. Rev. C*65 044006-1 (2002). 43. R. A. Oriani and J. C. Fisher, Detection of energetic charged particles during electrolysis, in: Proceedings of the 10th International Conference on Cold Fusion (Cambridge, MA, USA, August 2003), in press. 44. R. A. Oriani and J. C. Fisher, Energetic charged particles produced in the gas phase by electrolysis, in: Proceedings of the 10th International Conference on Cold Fusion (Cambridge, MA, USA, August 2003), in press. 45. R. A. Oriani and J. C. Fisher, in presented at ICCF11. 46. J. C. Fisher, Theory of low-temperature particle showers, in: Proceedings of the 10th International Conference on Cold Fusion (Cambridge, MA, USA), in press. 47. Z. Henis, S. Eliezer, and A. Zigler, J. Phys. G: Nucl. Part. Phys. 15, L219 (1989). 48. M. I. Darby, S. Papaconstantinopoulou, and K. N. R. Taylor, A crystal field theory for molecular hydrogen, J. Phys. C: Solid State Physics 13, 2881 (1980). 49. J. E. Hunter, D. G. Taylor III, and H. L. Strauss, Calculation of the rotational Raman spectrum of H2 dissolved in water, J. Chem. Phys. 97, 50 (1992).
COLD F U S I O N P H E N O M E N O N A N D SOLID STATE N U C L E A R PHYSICS
HIDEO KOZIMA Cold Fusion Research E-mail:
Laboratory, Yatsu 597-16, Aoi-ku, Shizuoka-shi, 421-1202, Japan [email protected]; [email protected]
Shizuoka
The cold fusion phenomenon (CFP) is investigated in the wider perspective of modern physics including the physics of transition-metal hydrides, nuclear physics, and the science of complexity using quantum mechanics. The characteristics of C F P including the stability effect in nuclear transmutation and the inverse power law of excess power generation are consistently explained using concepts of the cf-matter presented at ICCF10 by the present author.
1. Introduction We investigated the cold fusion phenomenon (CFP) phenomenologically at first1 and then quantum mechanically. 2 ' 3 Now, we are able to understand 4 the total image of this complex phenomenon as a whole without reference to Fleischmann's hypothesis (immense acceleration of D-D fusion reaction rate in solid transitionmetal deuterides) which led to the pioneering work.5 The cold fusion phenomenon is an outstanding phenomenon revealing complexity, a science closely related with self-organization and chaos, in solids corresponding to such meteorological and geophysical phenomena as the typhoon, hurricane or the earthquake. Its cause is defined by characteristics of the complex system and the phenomenon destined to be irreproducible in a strict sense conditioned by stochastic and/or chaotic processes occurring in the microscopic atomic milieu in the sample. While atomic processes govern the cause, the effect is nuclear and therefore quantitative ratio of energies relevant with the effect and the cause reaches up to 107. The effect accordingly is not completely averaged out as in atomic effects usual in solid-state physics and appears exotic for solid-state scientists. On the other hand, conventional mechanism of nuclear reactions between charged particles to overcome the Coulomb barrier is excluded in this situation: To reach a mutual distance of about 1 fm where the nuclear force works, the kinetic energy of the mutual motion of two charged nuclei should be 105 times larger than their thermal energy at the equilibrium state in solids. The large size of the effect (about 107 times greater that of the cause in energy scale) combined with the smallness of the effective microscopic process (about 10~ 5 times that of the cause in space dimension) together induce spectacular events 769
770
rarely seen in nature. The chaotic nature of the process producing CFP includes qualitative but not quantitative reproducibility, which is popular in simple systems usually treated in modern physics. These features of CFP make it difficult to accept it in the field of scientific investigation for many scientists. In this paper, we show a consistent explanation of the total feature of CFP using two laws discovered in the experimental data - the inverse power law of the excess power and the stability effect of the nuclear transmutation - as clues to understand this complex phenomenon.
2. Solid State-Nuclear Physics of CFP Revealed by Experimental Data Schematically, the characteristics of CFP are itemized as follows.
2.1. Phenomenological
of CFP1'*
Characteristics
Al. There are optimum combinations of the body material and hydrogen isotope. Experimental data obtained in these more than 10 years shows Pd-d and Ni-p satisfy this condition and are good combinations for CFP. A2. Formation of composite system (inhomogeneous and unsteady distribution of occluded hydrogen isotopes in a body metal) is a source of chaotic behavior in CFP. A3. There are optimum combinations of the body material and the electrolyte metal to realize active nuclei in the appropriate surface/boundary regions: e.g., Pd-Li, Ni-K, Na, and Ti-Li, A4. Production of tritium requires deuteron and that of 4 He requires 6 Li in the surface/boundary regions. A5. CFP is fundamentally irreproducible and has at most qualitative reproducibility in short time range. A6. The nuclear reactions may destroy necessary condition(s) for CFP and therefore CFP is fragile.
2.2. Microscopic
Processes
in CFP2
4
Bl. Lattice nucleus should have neutron levels at around the zero energy level (the evaporation level). Pd, Ti, and Ni satisfy this condition. B2. Interstitial protons/deuterons with wide spread wave functions which interact with neutrons in lattice nuclei. B3. Super-nuclear interaction of neutrons in lattice nuclei mediated by interstitial protons/deuterons. B4. Formation of neutron bands around zero level. B5. Formation of cf-matter at appropriate boundary/surface regions. B6. Neutron drops ^ A (in the cf-matter) - nucleus ^X interaction.
771
2.3. Realization of Necessary Formation1'2
Conditions
for Neutron
Band
CI. Ordered lattice nuclei with excited neutron levels around zero energy (evaporation level). C2. Nearly saturated occluded proton/deuteron with wave functions spread out at lattice nuclei. C3. Neutron (in a lattice nucleus) - proton/deuteron interaction by the nuclear force. C4. Neutron (in a lattice nucleus) - neutron (in another lattice nucleus) interaction mediated by the occluded protons/deuterons (super-nuclear interaction). C5. Formation of neutron bands due to the super-nuclear interaction. C6. Local coherence of neutron waves in a band at surface/boundary regions. C7. Enough number of neutrons in the band to realize cf-matter where are neutron drops (^A) composed of neutrons and a few protons. C8. Existence of exotic/disordered nuclei (active nuclei) at the surface/boundary regions to realize CFP by interactions with the neutron drops. C9. Nuclear reactions between a neutron drop (^A) and a nucleus (%X) occur in a chaotic state and production rates of new nuclides governed by their stability.
2.4. On the Wave Functions of Protons/Deuterons Transition-Metal Compounds4
in
We give here short explanation of some properties of interstitial protons/deuterons with wide spread wave functions in transition metals. We know that CFP occurs only in fee and hep transition-metal hydrides and deuterides. In the transition-metal alloys, it is noticed that there are optimum combinations of metal and hydrogen isotopes: Some examples are Pd-d, Ni-p, and Ti-d, p. Data of physical properties of transition-metal hydrides and deuterides show following nature of the wave functions of hydrogen isotopes. In PdH and PdD lattice, hydrogen or deuterium atoms occupy octahedral sites in ground states. In excited states, however, they are in tetrahedral sites and have more spread wave functions over several interstices. There are several different characteristics in PdD and PdH: In PdD, Pd-D interaction is relatively weak and D-D interaction has the characteristic that the second neighbor D-D interactions is fairly strong comparable to the first neighbor D-D interaction. In PdH, H-Pd interaction is comparable to H-H interaction even if H-Pd distance (2.03 A) is less than that of H-H and the large value of the nuclear charge of
772
Pd (Z = 46). Furthermore, it is probable that there is a repulsion of H atoms on next-nearest neighbor sites, which would overcompensate the attraction of nearest neighbor H atoms at high concentrations. Activation energies for diffusion of D and H in Pd are 0.206 (T = 218-333 K) and 0.23 eV (T = 230-760 K), respectively. These are some properties of Pd alloys, one of the most well investigated transition-metal hydrides and deuterides. Similar properties have been investigated in other alloys and they should be combined with data of CFP to elucidate quantum mechanical states of protons and deuterons in them. 2.5. Electrochemistry
of CFP6
It is now evident that the cold fusion phenomenon occurs mainly in surface/boundary regions of solid materials including high-density hydrogen isotopes. 1 ' 6 Especially in electrolytic systems, we have noticed the existence of optimum combinations of electrodes-electrolytes; some examples are P d / D 2 0 + LiOD/Pt, Ni/ H 2 0 + KOH/Pt. A special case, in addition to the above ones, successively used by John Dash of Portland State University and others is a combination P d / D 2 0 + H 2 S 0 4 / P t . Unfortunately, this problem of optimum electrode-electrolyte combinations is not clarified yet. It is clear, however, that the formation of a surface layer with a composition appropriate to occlude hydrogen isotopes into cathode and to initiate nuclear reactions relevant with CFP is decisively important to realize CFP successfully. 3. Empirical Facts of C F P Show Its Complexity There are too many experimental data sets to grasp physics behind them with out a sound viewpoint. From those data sets, we could deduce two laws related the essence of CFP. 3.1. Inverse
Power
Law of the Excess Power
Production4,
The analysis of the data by McKubre et al.,7 in this section is far from complete. They will be able to give more extensive and complete analysis of the data along the same line of investigation as ours. We have counted number of observations N(P) from their Fig. 6 as shown in Table 1 and made a data table to depict a log AT vs. logP graph as shown in Table 2. The inverse power law of excess power generation is clearly seen in the region from logP = —1 t o + 0.1 (from 1 to 12 of the abscissa). The data depicted in Fig. 1 expresses that N(P) is inversely proportional to P: N{P) = const. P~a with a w l . The characteristic expressed in the graph of the excess power spectrum reveals that CF system shows "the self-organized criticality." This characteristic is common to
773 Table 1. Gross number N(P) of measurement point for the excess power P(W) grossly counted from Fig. 6 of McKubre et al., 7 using Pd wire with a dimension 1 mm <j> x 36 cm (surface area of 11.3cm 2 ). P{W) N(P) P{W) N(P)
0.1 400 1.1 30
Table 2. logP N(P) logiV
-2.1 400 2.6
0.2 240 1.2 30
0.3 160 1.3 20
0.4 140 1.4 10
0.5 120 1.5 8
0.6 100 1.6 8
0.7 60 1.7 5
0.8 60 1.8 2
0.9 40 1.9 5
1.0 40 2.0 1
Dependence of log N(P) on l o g P estimated from the data given in Table 1. -1.7 240 2.4
-1.6 160 2.2
-1.5 140 2.15
-1.4 120 2.08
-1.3 100 2.00
-1.2 90 1.95
-1.15 70 1.86
+0.1 60 1.78
0.2 38 1.58
0.3 21 1.32
Note: The data given in Table 2 are plotted in Fig. 1.
many phenomena occurring in complex systems; a most well known example is the 1 / / noise of electric resistance noticed in 1925 by Johnson (the index a = 1). Other examples include the frequency of earthquakes vs. their intensity (Gutemberg-Richter's law, a = 0.47-0.73) and the intensity distribution of winds. The distribution of wind speeds at heights 80 and 150 m were measured in Japan at the time of a typhoon. The index for a (the two heights) was determined to be 1 and 5/3, respectively. Another interesting example of this behavior is the intensity of the cosmic ray measured at upper atmosphere. It obeys the l//-law. The interesting point is its relation with the fluctuation of the inter-galactic magnetic field that obeys also the l//-law. It is considered that the fluctuation of the intensity of cosmic ray reflects that of the magnetic field. 3.2. Stability
Effect of Nuclear
Transmutation
of
CFP3'4
The stability effect of nuclear transmutation in good coincidence with the abundance of elements in universe found in experimental data sets 3,4 clearly indicates
Figure 1. Plot of logN vs. l o g P from Table 2 showing linear dependence of logN on l o g P with a negative gradient with - 1, the inverse power law. Linear line is drawn for the benefit of eyes.
774
20 2
15
°a
10
a: O
- • — logH -m—Nob
°
0 1
3
5
7
9 11 13 15 17 19 21 23 25 27 29 31 33 35 37 Z
Figure 2.
Stability effect of nuclear transmutation. 3 ' 4
-10 logH -Nob
imiMi 1
4
7
10
13
16
19
22
25
28
31
34
37
40
43
46
Z-37
Figure 3.
Stability effect of nuclear transmutation. 3 ' 4
the existence of compound states of nucleons in CF materials where stable configurations of nucleons are easily formed. This is a complex many-body system looked at from a somewhat different point from that given in the preceding subsection about the inverse power law. 4. Discussion Experimental data sets obtained in the 15 years after the discovery of CFP 5 probably number more than a thousand, and we have concentrated too long on a narrow perspective with poor prospects. In our opinion, the data obtained until now have not been fully utilized to give a sound perspective for future development of CFP research. Perhaps it would be useful to depart from Fleischmann's hypothesis for a while and to look at the whole situation from various different points of view. Our approach has been a trial to reconcile experimental data such as the two laws explained in this paper with principles of modern physics. We have to recall from statistical stability, a characteristic of the chaos that the trajectory in the phase space of a chaotic system is unstable to a small perturbation and non-reproducible but a time average of a physical quantity on the trajectory is stable and is reproducible. The most direct evidence of this nature in CFP is shown in Fig. 1 as the inverse power law of the excess power generation and less directly in Figs. 2 and 3 as the stability effect of nuclear transmutation.
775 As we have emphasized several t i m e s , 1 _ 4 t h e system where t h e cold fusion phenomenon occurs has t h e characteristics of complexity and phenomena occurring in t h e m have inevitably qualitative reproducibility b u t not quantitative one. A somewhat theoretical verification of t h e complexity of C F P is seen as follows. There are several situations in t h e microscopic process crucial t o realize C F P . If other necessary conditions are fulfilled, it is necessary to have (a) an appropriate distribution of protons/deuterons to realize the super-nuclear interaction (Section 2, B3, C4), (b) an appropriate boundary/surface conditions to realize t h e local coherence (C6), (c) high density neutrons (B5, C7) to form t h e cf-matter including neutron drops, a n d (d) appropriate exotic nuclei to realize nuclear reactions with the neutron drops (B6, C8). These conditions can be realized as self-organization, from a chaos-theory point of view. We have to look at C F P from t h e above point of view if we notice t h e existence of t h e two laws in C F P - t h e inverse power law of excess power and t h e stability effect of N T . T h e necessary conditions for C F P explained in Section 2 from our point of view should be examined more carefully using experimental data. It should be mentioned about a pioneering computer simulation on t h e selforganization in nuclear physics. Negele et al.,8 showed a formation of a regular lattice by self-organization in neutron star matter. This is an example of selforganization exactly corresponding to t h e situation (C7) in C F P discussed above.
References 1. 1) H. Kozima, Discovery of the Cold Fusion Phenomenon (Ohtake Shuppan Inc., Tokyo, 1998). ISBN 4-87186-044-2. Essential parts of this and following works by the author are accessible in the Cold Fusion Research Laboratory (CFRL) website: http://www.geocities.jp/hjrfq930/; http://web.pdx.edu/ pdx00210/. 2. H. Kozima, Quantum Physics of Cold Fusion Phenomenon Developments in Quantum Physics, F. Columbus and V. Krasnoholovets (Eds.) pp. 167-196 (Nova Science Publishers Inc., New York, 2004). ISBN 1-59454-003-9. 3. H. Kozima, Cf-Matter and the cold fusion phenomenon, in Proceedings of the ICCFIO (to be published). 4. H. Kozima, Cold Fusion Phenomenon, Rep. Fac. Science, Shizuoka University, 39, 21-90 (2005). 5. M. Fleischmann, S. Pons, and M. Hawkins, Electrochemically induced nuclear fusion of deuterium, J. Electroanal. Chem., 261, 301-308 (1989). 6. H. Kozima, Electroanalytical chemistry in cold fusion phenomenon, S.G. Pandalai (Ed.), Recent Res. Devel. Electroanal. Chem. 2, 35-46 (Transworld Research Network, Trivandrum, India, 2000). ISBN 81-86846-94-8. 7. M.C.H. McKubre, S. Crouch-Baker, Riley, S.I. Smedley, and F.L. Tanzella, Excess power observed in electrochemical studies of the D / P d system, in Proceedings of the ICCF3, pp. 5-19 (1993). 8. J.W. Negele and D. Vautherin, Neutron star matter at sub-nuclear densities, Nuclear Phys., A207, 298-320 (1973).
N E U T R I N O - D R I V E N N U C L E A R R E A C T I O N S OF COLD F U S I O N A N D TRANSMUTATION
VENIAMIN FILIMONOV National Academy of Sciences of Belarus, Belarus http://www. cold-nuclear-fusion, com
1. Introduction Cold fusion and transmutation [more recently condensed matter nuclear science (CMNS)] investigation is carried out for more than 15 years by an international community of scientists. Nevertheless, until now there has been no answer to this vexing question: does CMNS agree with conventional nuclear physics and, if not, what "hidden factor" defines the border between conventional physics and CMNS? To solve this problem, we suggest the hypothesis of neutrino-driven nuclear reactions (NDR). This hypothesis is a particular instance of a more comprehensive concept of non-high-energy neutrino (NNN) interactions with matter that results from analysis of a set of the so-called "anomalous phenomena" of some unconventional low-energy radiations interaction with matter at the atomic, molecular, and crystalline level of organization of the latter. It can be shown that a noted set of phenomena can best be interpreted by assuming they are initiated by NNN flows amplified under the experimental conditions. On the other hand, analysis of noted phenomena discloses conformities to the natural laws of NNN manifestation and therefore establishing real criteria for stable, self-sustained and reproducible CMNS reaction implementation. According to the NDR hypothesis, the so-called spontaneous nuclear reactions of decay {(3 decay at least) and fission - conventional ones - are initiated by natural flows of NNN and every nuclide to be stable in hypothetical situation outer action on nuclei elimination, say, by NNN flow screening. Implementation of anomalously fast CMNS reactions is caused by the real possibility of NNN flow density varying under experimental conditions. Earlier we suggest the concept of neutrino as a quantum of radiation (being a fermion contrary to the photon being a boson), the energy of which one is determined by its characteristic frequency (with numerical factor of 1/2): £v =
\HD
(1)
and the probability of which one capture by matter depends on the energy of the former resonantly.1 776
777
This consideration reveals various cases of NNN interaction with matter. Indeed, the meaning of neutrino inertness is based on the fact that v, contrary to other particles, does not have any electric charge, mass, etc., except for a spin. The correlation of v with a photon 7 that is even more "featureless" particle, but not so inert, allows us to doubt the conventional insight on neutrino universality. The consideration of the suggested concept corollaries carried out in the paper, proves a fruitfulness of the former. Certainly, all effects circumscribed below, can be observable and measurable under intensity of NNN flow that exceeds essentially a natural background. The energy rate of NNN is defined as follows: from the first 10s of eV, that is, the ionization energy of valence electrons of atoms, up to zero point. Hereinafter the sign of a NNN spin (±1/2) is not regarded, despite it is noticed specially. 2. The Basic Mechanism of N N N Interaction with Matter: Formation of an Electron—Neutrino Couple in an Atom The key point of the NNN interactions with matter is the suggestion of an electronneutrino (ev) couple formation in atom. According to Pauli's exclusion principle, the existence of two particles having identical quantum numbers (except for spin one) in an atom is possible. They used to suggest electrons, however, identity of considered particles to electrons is optional, which is proved by the opportunity of an electron in hydrogen atom substitution by a muon (that is a negatively charged fermion having a mass m^ = 206m e ). We figure that the negative charge of the particle nor is the factor defining quantum mechanical interaction, and the formation of a couple with an electron (or substitution of the latter) by neutral fermion is also possible. Here is a scheme relevant to the suggested process:
T+ ^ '
(2a)
e + v = ev ,
n + ^ = n + T, ee
+ v = ev
+e ,
where the upper pair of equations shows a formation of a couple from uncoupled electron and neutrino, and lower one a substitution of an electron in ee couple by a neutrino. As to atoms having charge of nuclei equal to (+1), that is hydrogen isotopes, the suggested interactions should result in the most significant effects. However, the effects of formation of ev couple may be noticeable in multielectronic atoms, too. It is worth noting that the energy of NNN, absorbed along with excitation of electron, is not equal to a difference of energies of the latter in initial and eventual states, so the energy level, which is occupied by a new-formed ev couple may differ from an initial level of an electronic couple. It is easy to see that: e„ = | A e | - | A e * | ,
(3)
778
where Ae is the energy difference between ground and excited electron states and Ae * is the difference between ground electron state and diminished energy level of ev couple and e„ value can be both positive and negative. 1
3. N N N Interaction with Condensed Matter: Numerous Non-Nuclear Secondary Effects The numerous sequels of hypothetical NNN interactions with electrons forming covalent and metallic bonds in solids are listed in our paper. 2 It is possible to imagine a realization of the following effects under NNN interaction with metals: (1) The formation of ev couples by mobile electrons of metal should promote embodying of phase transition (PT) of metal - high-temperature superconductor (HTSC). In this case the ev couple occupies one of the conduction band energy levels that has not been localized near certain atom, but is shared by all atoms of metal, and is a single-charged analog of a Cooper electron couple that causes a superconductivity of HTSC. The formation of ev couples by electrons of metal along with its further NNN loading would provide gradual filling of all conduction band energy levels, that results in drop of electrons mobility and in metal-dielectric FT implementation. We state that the circumscribed phenomena were observed earlier but misinterpreted. 3 Similarly, the NNN interaction with semiconductors (SC) results in SC - metal, SC - dielectric PTs implementation and in variation of p-n-transitions conductance and capacity. We state that the above effect was already applied in detectors of NNN radiation, though the latter were interpreted erroneously. 4 ' 5 Similarly, the NNN interaction with dielectrics can proceed, taking into account the minute conductance electrons concentration. In this case the formation of ev couples can result in enhancing their mobility, and NNN pairing with valence band electron - in occurrence of extra current carriers. Another probable effect is concerned with a change of magnetic properties of a dielectric under splitting electron (ee) couples by NNN: when uncoupled electrons would appear, that provides magnetic properties to dielectric material. The latter effect was already observed3 but misinterpreted.
4. Nuclear Secondary Effects of N N N Interaction with Matter: Neutrino-Driven Reactions The possibility of neutrino participation in nuclear reactions may, in our opinion, enhance many types of the latter, including fusion, direct and revertive /3-decay (including an electron capture), a-decay and fission. The numerous examples of abnormally fast nuclear reactions (AFR) are listed in Ref. 6, but it is impossible to perform a complete review of the former within a journal paper. AFR with hydrogen isotopes participation proceed, in our opinion, via hydrogen atom electronic orbit
779
(cloud) squeezing due to formation of ev couple. Such an atom behaves as a quasineutron (a quasi-bineutron, etc.) and is able to fuse an adjacent atom nucleus quite easy because of Coulomb repulsion screening. The existence of excited states of hydrogen atom having an electron orbit squeezed up to 0.01 of equilibrium radius of the latter was already suggested for AFR explication earlier (the so-called BarutVigier's atom, 7 Mills's hydrino, 8 ), but was not linked with v participation. The wide variety of fusion AFR - from D-D one (see, e.g., Ref. 9) and of light nuclei ones 10 up to adding a proton to heavier nuclei with a set of secondary reactions of /3-decay11 - is observed. The latter also proceeds with abnormally high rates in the same conditions as those of fusion AFR implementation. Except for reactions of an electron capture, which one can be ascribed by the above-stated mechanism with the subsequent absorption of a "reduced" electron by a nucleus, these reactions require some more guesswork to explain. We do not dispute here conventional theory of /3-decay that ascribes "normal" reactions of this type and, mainly, does not deal with participation of v on an inlet of reactions. However, as we noted earlier,2 the equation of a radioactive decay rate dependence on time will not change within the suggestion that the decay is "externally" driven and occurs under action of the exterior factor having a stationary value or feebly varying intensity: Ai = Iv(TiPi,
(4)
where Ajis a constant of decay, Iv is an intensity of the exterior factor (a space neutrino flow), Ui is a neutrino capture by a nucleus cross-section, and pi is a probability of /3-decay of a nucleus resulted from the former. As to AFR, we figure that the ev couple has (according to quantum-mechanical consideration) deflection probability of its occurrence within a nucleus. Thus, being a boson, the former represents itself as an ersatz substitute of conventional weak interaction carriers, namely of intermediate bosons W° and Z^. By virtue of a minute mass of an ev couple the time of its occurrence within a nucleus is much less than the lifetime of W° and Z1*1 bosons. It means, in particular, that the single-pass of an ev couple does not causes inevitable nucleus decay and that the probability of the latter deduces during many passes. The value of this probability P/3 depends essentially on the fact whether the constituents of a couple oscillate (i) synchronously or in opposite phases or (ii) independently from each other: Pp = ^ " >
(5a)
where ap is a section of a /3-decay reaction, a is a cross-section of a nucleus, Pe is a probability of an electron occurrence within a nucleus and power factor n = 1, 2 for situations (i) and (ii), respectively. We suggest a similar explication for observed AFR of fission12 and a-decay. 10 In this case the ev couple occurring within a nucleus fulfills a role of an ersatz substitute for the boson responsible for transmission of strong interactions, namely
780
of the 7r-meson. The resulting equation for probability of fission or a-decay P / , a is similar to the latter one: Pf,a = ^P?a
(5b)
We have to consider briefly a problem on why AFR observed with both radioactive and stable (within conventional consideration, i.e., while disregarding the below nuclides interactions with NNN) nuclides participation proceed without any ionizing radiation yielding (see Ref. 9, etc.; the latter fact is one of obstacles preventing the AFR incorporation in conventional nuclear physics). Let us note the equations were based on two possible types (/3-decay, both direct and reverse one, on the one hand, a-decay and fission, on the other one) as follows: A{u, vPe~)B, A{v,va)B,
A{v, vve+)B,
(6a)
A{v,vC)B.
(6b)
We guessed earlier 13 that the energy e of antineutrino v yielding from the above reactions, is unanimously determined by the duration of the elementary act of reaction:
where h is a Plank's constant, \ stands for the dimensionless value, the so-called coordinate of reaction, and TX is a duration of the act of reaction. AFR are certainly more fast processes than conventional reactions of /3-decay, a-decay and fission, because of the fact that the ev couple is not the rigorous substitute for W° and Z^ bosons and 7r-mesons, correspondingly. As a sequel, practically entire energy effect of reaction is blown by a vigorous antineutrino, and these reactions result in the stable nuclei having non-excited energy state. 5. Brief Review of Anomalously Fast C M N S Reactions The significance of a radioactive decay rate variation and its correlation with the solar activity variation is demonstrated after some decades long observations. 14 The variation of the decay rate after variation of crystalline and chemical environment has been observed for 40 years. The rates of 7 Be decay by means of an electron capture differ by 0.1% in pure beryllium and its oxide BeO. 15 It was stated, that the rate of 9 9 m Tc decay by internal conversion increases in compounds such as RTCO4, where R is the alkali metal, as related to pure metallic technetium. 16 It is also shown that the decay of 32 Si is retarded by 6% after substitution of its crystalline environment by a specially designed matrix. 17 The variation of nuclear transmutation rates is even more significant after lowenergy non-nuclear actions on media (the so-called cold fusion and transmutation of
781
nuclei). So, the activity of tritium 3 T, absorbed by Ti, may possibly vary reversibly within 30% by a temperature variation. 18 There are data about an opportunity of a variation of decay rates by means of electronic excitation, action of pressure, temperature, electrical and magnetic fields, of mechanical stresses in monomolecular layers, etc. 16 The various nuclear reactions occur under water (H2O and D 2 0 ) electrolysis. After electrolysis of an 8 7 Rb radioisotope containing solutions 11 decay of the former accompanied by formation of short-lived radioisotopes (half-decay period of about 3.8 days) was detected. Formation of a set of stable nuclides affiliated to 8 5 Rb, 87 Rb was also observed, down to 1 0 8 _ 1 1 4 S n . n These products are supposed to be derived as a result of total reactions of a type: ^"Rb-^H^^Sr.etc. 86
A shift of stable nuclides Sr/ 8 8 Sr relation towards the diminution of the latter nuclide share as related to the natural isotopes mixture testifies convincingly for the benefit of the above. The opportunity of massive transmutations of Fe, Cr, Ni to Cu, and Zn was exhibited in experiments on a high-voltage electrolysis of water and other liquids using stainless steel electrodes. 19 Transmutations of stable nuclides into radioactive by-products of fusion (and fission) were detected during electrolysis of potassium carbonate solution K2CO3 in light water on Pt and Ni electrodes:20 190p t _> 190 A U ) 1 9 0 ^ 191p t j 192 Ir) 1 9 3 O S ;
i96pt ^ 1 9 5 m p t ; i97Pt) 198p t _> 199p t ) 198 A U ;
199 A U ;
6 4 N i _> 6 5 M ; 6 5 Z n i 6 7 C U ; 39K
^
40K; 42K ^
6 7 ^
43K
The formation of a series of Cr, Mg, Fe, Co, Cu, Zn, and Ag isotopes was observed under electrolysis of light water (H 2 0) solution of lithium sulfate Li2S04 using a boiling bed of plastic beans covered with a Ni thin film as the cathode. 21 Those isotopes to be the products of fusion: £8Ni + lR = ... followed by a-, /?-, and p-decay.21 The data on an effective method of long-lived radioisotopes ( 232 Th and disintegration in an electrolysis cell appeared: 10 232Th _ ^ 2 6 5 C u
+
2
so T i ( + 2
239
Pu)
i R? )_
The nuclear transmutations 1 0 5 Pd —> 107 Ag, 1 0 6 Pd —> 108 Ag, etc. were observed during glow discharge in deuterium gas using Pd electrodes. 22 A method permitting the decomposition of long-lived radioisotopes under action of the atomic hydrogenoxygen torch flame was designed. 16,23 In particular, a drop of a radioactivity of a 60 Co containing waste from 580 to 220-240 mR/h and from 115-120 to 42mR/h is reported, and also drop of activity of a 241 Am-containing waste from 300 down to 1.5 Cu after a 5-min exposure. 23 The data on implementation of accelerated
782
fission of long-lived radioisotopes 2 2 6 Ra and 2 3 2 Th under a detonation of explosives were also reported. 24 (It is worth noting that the possibility of such a process was predicted earlier. 25 ) The transmutations accompanied by formation of a mixture of short-lived nuclides, the activity of which ones is reduced down to a natural background level for 60 days, were reached by the latter method. There are some data on initiating radioisotope decay and other nuclear transmutations by means of some sort of unconventional radiation (named in various ways, and similar to electromagnetic method, but not identical to). The properties of the latter are manifested, in particular, by a reorientation of nuclear spins and magnetic moments of atoms 26 that causes a disordering of matter structure and variation of nuclear reactions rates. 1 6 ' 2 7 It is reported that the generator of such radiation having power of 5 W is capable of lowering radioactivity of a sample with a mixture of radioisotopes from 0.5 down to 0.015 mR/h, or by 97% (the time of action is not indicated). 16 The "installation for nuclear transformations of light elements of ferromagnetic substances" based on the generator of torsion high-power fields is tested, 10 and transmutation of a set of stable nuclides is implemented:
31
28
P (+ : H) ^ 3 2 S, Si -+ C ( + 1 6 0 ? . . . + 12 C + 4 He?). 12
It was stated 28 that radioisotopes (in particular, 137 Cs) produced after the Chernobyl accident during some years after their fallout had reduced half-life periods (3.5 and 17years for 1988 and 1992years' samples, respectively), hereinafter asymptotically incremental up to the conventional values (30.6years).
6. Explication of Anomalously Fast C M N S Reactions Within N D R Hypothesis The difficulty of universal description of the above phenomena is caused by a vast variety of low-energy actions initiating anomalously fast nuclear transmutations. However, a general property of the former is strong non-equilibrium of systems and irreversibility in principle of the processes the transmutations are implemented under (see, e.g., Ref. 29). As for transmutation, all experimental observations of nuclear reactions acceleration - irrespectively of a type of reaction (fusion, decay, and fission) and of participating nuclides features (radioactive or "stable" ones) - occur in non-equilibrium and (or) self-organizing systems under intense flows of matter and energy. This qualitatively confirms the thesis. We suggest the concept of neutrino-driven nuclear reactions for explication of abnormally fast nuclear reactions surveyed above and conformities to natural laws observed under the noted reactions proceeding.
783
This concept based on the series of the author's papers 1 ' 2 , 6 according to which the non-high-energy (
784
under highest non-equilibrium conditions. As to the latter conditions, the processes of solids detonation exceed by some orders of magnitude the burning processes having a subsonic rate of combustion front, so being the strongest intensifier of abnormally fast nuclear reactions. 24 As to the action of some unconventional radiation (sometimes named "torsion" radiation or the same fielding Russian issues) on the transmutation rate of radioactive and "stable" nuclides, it testifies convincingly for the benefit of that radiation quanta ("torsions") identification with neutrinos of the relevant energies. 1 ' 13 Also, observed Chernobyl track radioisotopes "aging" 28 along with magnification of their half-life periods (up to conventional values) is conditioned by these nuclides formation under activity of high intensity neutrino flows produced by the nuclear reaction of fission. This experimental fact can demonstrate that the absorption of neutrinos by nuclei causes a prolonged aftereffect. No doubt similar facts could have been observed earlier. However, only neutrino-saturated products of fission reactions implemented under above-critical mode of the reactor have maintained their neutrino-induced anomalous behavior after several years, which has allowed authors of28 to find out and to identify products in natural media. The concept is consistent with an entire set of the facts and observations concerning transmutation without any exception. This can also explain various facts of other fields of science that have not accepted till now by conventional science; namely, it concerns the "torsion" fields research area, some data of an elementary particle physics, astrophysics, cold fusion and transmutation of nuclei, and also biologic transmutation. 35 The space NNN flow focusing might result in deducing (and the former shielding in reducing) the radioactive decay rate. Some possibilities of the above operation of NNN flow are described in our previous papers. 1 ' 2 , 1 3
7. Conclusion The NDR concept explains how the nuclear transmutation rate varies in low-energy non-nuclear actions, and explains all features of the phenomenon. The concept unites a series of observed phenomena in various fields; some of them have been outside conventional scientific consideration until now. Attempts to ascribe phenomena to neutrino interactions were made earlier 26 ' 36,37 but they were hindered by a known point of conventional neutrino theory: according to that the sections of a neutrino interaction with a matter are extremely small, dependent proportionally of a neutrino energy and essentially distinct from zero point if the latter is more than 100 eV. This is a reason for the fact that a series of NNN interactions with matter observed in various types of experiment, were misinterpreted and erroneously ascribed to the action of other (hypothetical) particles. Neutrino-driven nuclear reactor based on the above 1 , 2 , 1 3 ideas has been constructed and experiments started since recently. Results to be placed on http://www.cold-nuclear-fusion.com site. English versions of1,2'13 and other relevant papers of the author will be placed there, too.
785
References 1. V.A. Filimonov , FUR (Phys. Ideas Russia) 3, 89-92 (2000) (in Russian). 2. Item., Ibid. 2, 56-61 (2001). 3. I.M. Shakhparonov, in R.F. Avramenko, et al. (eds.), Ball Lightning in Laboratory (Khimiya Publ., Moscow, Russia, 1994), pp. 184-198 (in Russian). 4. A.I. Veinik, Thermodynamics of Real Processes (Minsk, Navuka i Tekhnika Publ., 1991), 576p (in Russian). 5. A.I. Veinik and S.F. Komlik, Complex Investigation of Chronophysical Properties of Materials (Minsk, Navuka i Tekhnika P u b l , 1992), 96p (in Russian). 6. V.A. Filimonov, in Transactions of International Congress- 2000 "Fundamental Problems of Natural Sciences and Technique" (St.-Petersburg, Russia, July 4-8, 2000); 1 (1), pp. 242-247 (2000) (in Russian). 7. J.-P. Vigier, in H. Fox (ed.), "Cold Fusion Source Boot?. International Symposium on Cold Fusion and Advanced Energy Sources. (Minsk, Belarus, May 24-26, 1994; Salt Lake City, USA, 1994), pp. 95-104. 8. R.L. Mills and S.P. Kneizys, Fusion Technol. 20, 65-70 (1991); R.L. Mills, W.R. Good, and R.M. Shaubach, Fusion Technol. 25, 103-107 (1994). 9. H. Kozima, "Discovery of the Cold Fusion Phenomenon" (Ohotake Shuppan Inc., Tokyo, 1998), 370 p. 10. B.V. Bolotov, N. A. Bolotova, and M.B. Bolotov, Fundamentals of a Structure of Matter. (ZGIA Publ., Zaporozhye, 1996), 110 p; B.V. Bolotov, M.B. Bolotov, and N.A. Bolotova, Installation for nuclear transmutations of light elements of ferromagnetic matters. Patent application of Russia No. 94024136/25 of 28.06.1994/10.04.1998. 11. R. Bush and R. Eagleton, Proceedings of the Ath International Conference on Cold Fusion (Lahaina, Maui, Hawaii, December 6-9, 1993). Trans. Fusion Technol. 26, (4T, Part 2), 344-351 (1994). 12. R. Bass, in R.R. Liversage (ed.), Low-Energy Bulk-Process Alchemy. One-tenth Gram of Thorium Becomes Titanium and Copper (News Release, June 16, 1997), pp. 1-6; Infinite Energy 3 (13-14), 20-24 (1997). 13. V.A. Filimonov, FMR 1 86-89 (2001) (in Russian). 14. S.E. Shnol, V.A. Kolombet, E.A. Pozharskii, et al, UFN(Uspekhi Fizicheskikh Nauk), 168 (10), 1129-1140 (1998) (in Russian). 15. T. Bearden, J. Bockris, Y. Brown, et al, Planetary Assoc. Clean Energy Newslett. 8 (4), pp. 18-24 (1996). 16. Canadian Environmental Assessment Agency (CEAA), Clean Energy Review. Technical and Scientific Discussion. Planetary Association for Clean Energy (PACE) (Ottawa, Canada August 8, 1995), 24 p. 17. E.A. Rausher and R. Bruch, S-matrix theory of Alpha decay (Book manuscript, to be published); K. Harada and E.A. Rausher, Phys. Rev. 169, 818 (1968); Item., Alpha decay of Po 2 1 2 -> P o 2 0 8 , Po 2 1 0 - • P o 2 0 6 , treated by the Unified Theory of Alpha Decay. UCRL-70513, May 1967. 18. O. Reifenschweiler, Cold Fusion 10, 7 (1995). 19. G.S. Rabzi and A.E. Fabrikant, in Transactions of International Symposium Cold Fusion and Advanced Energy Sources (Minsk, Belarus, May 24-26, 1994), pp. 186189 (in Russian). 20. R. Notoya, T. Ohnishi, and Y. Noya, The Best Ever! in Proceedings of the 1th International Conference on Cold Fusion (Vancuver, Canada, April 19-24, 1998; ENECO, Salt Lake City, USA, 1998), pp. 269-273. 21. G.H. Miley and J.A. Patterson, Infinite Energy, 9, 19 (1996). 22. LB. Savvatimova and A.B. Karabut, Cold nuclear fusion, in Proceedings of the 2nd Russian Conference on Cold Fusion and Transmutation of Nuclei (Sochi, Russia,
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23. 24. 25.
26. 27. 28. 29. 30. 31. 32. 33. 34. 35.
36.
37.
September 19-23, 1994; Moscow, Research Center F T P Erzion Publ., 1995), pp. 68-83 (in Russian). Y. Brown, US Patent No. 4,014,777, March 29, 1977. Item., US Patent No. 4,081,656, March 28, 1978. R. Monti, Proceedings of the Fifth International Conference on Cold Fusion (Monte Carlo, Monaco, April 9-13, 1995). Book of Abstracts, p. 626. V.A. Filimonov and V.A. Lishnevskii, in H. Fox (ed.), Cold Fusion Source Book. Proceedings of the International Symposium Cold Fusion and Advanced Energy Sources (Minsk, Belarus, May 24-26, 1994; Salt Lake City, USA, 1994), p. ? G.I. Shipov, The Theory of Physical Vacuum. New Paradigm (Moscow, MNTZ VENT Publ., 1993), 362 p (in Russian). W. Smith, The New Science (The Keith Press, Ottawa, Canada, 1964), 72 p. N.I. Sanzharova, S.V. Fesenko, R.M. Alexakhin, et al., Sci. Total Environ. 154, pp. 9-22 (1994). V.A. Filimonov, in Proceedings of the International Symposium Cold Fusion and Advanced Energy Sources (Minsk, Belarus, May 24-26, 1994), pp. 389-390 (in Russian). F. Bowm and P. Vogel, Physics of Massive Neutrino (Mir Publ., Moscow, 1990), 240 p (Russian translation). N.V. Samsonenko, F. Ndakhayo, and E. Kharelitana, Izvestiya Akademii Nauk. Seriya Fizika 62, pp. 12-20 (1988) (in Russian). A.E. Akimov, G.I. Shipov, and A.V. Loginov, et al., Priroda 6, 9-17 (1996) (in Russian) . G.I. Shipov, The Theory of Physical Vacuum. The Theory, Experiments and Technologies. 2nd edn. (Nauka Publ., Moscow, 1996), 450 p (in Russian). V.S. Barashenkov, et al., FMR 3 / 4 , 101-123 (1996) (in Russian). V.I. Vysotskii, A.A. Kornilova, and I.I. Samoylenko, Cold Nuclear Fusion. Transactions of 3rd Russian Conference on Cold Fusion and Transmutation of Nuclei, Dagomys, October 2-7, 1995. Moscow, Research Center F T P Erzion, 1996, pp. 96-122 (in Russian). N.I. Kobozev, Investigations in the Field of Thermodynamics of Processes of the Information and Thinking (MGU Publ., Moscow, 1971), 194 p (see also: N.I. Kobozev, Selected Transactions (MGU Publ., Moscow, 1978); 2, 3-240 (1998) (in Russian). G. Toquer, Cold Fusion 8, 10-15 (1995).
LIGHT MONOPOLES THEORY: A N OVERVIEW OF THEIR EFFECTS IN PHYSICS, CHEMISTRY, BIOLOGY, A N D N U C L E A R SCIENCE (WEAK I N T E R A C T I O N S )
GEORGES LOCHAK Fondation Louis de Broglie, 23 rue Marsoulan, 75012 Paris, France Our aim is to show that our theory can predict the existence of a light magnetic monopole, a lepton, which can play a role in various effects, including weak nuclear interactions.
1. Historical Points (1) The concept of a magnetic charge was first mentioned by Maxwell (1873) in his famous Course of Electromagnetism, vol. 1, part III, Ch I. 1 He shows that such charges obey the Coulomb law and produce a magnetic current created by a unipolar vector, contrary to the electric current, which is created by a polar vector. Maxwell identifies a unipolar vector to a rotational vector. This is none other than an axial vector. Maxwell therefore perfectly understood its nature, but he did not mention either the laws of symmetry or the possibility of observing those charges and currents. (2) It was necessary to wait for Pierre Curie (1894) who following his great paper on Symmetry in physical phenomena2 with another on the possibility of existence of magnetic conductibility and free magnetism.3 He hypothesized on the possibility of observing this, and showed that a sphere magnetically charged would obey the enantiomorph symmetry group COLQO. In modern vocabulary: a pseudo-scalar symmetry. The language of Curie is the one of crystallography (these laws are developed in a modern form in Ref. 4). He showed that two spheres, respectively, charged boreal and austral are mirror images of each other. We will find this in a quantum form. Curie does not talk yet of particules (monopoles), but let us not forget that at the time he wrote, even the electron was not known. (3) Dirac (1931) rediscovered the magnetic monopole5 while trying to determine if there exists a minimum electric charge e (the electron) such that hc/e2 w 137 so that all other charges are multiple of it. He showed using a gauge reasoning that if a Coulombian center interacts with a magnetic pole with charge g, the now famous relation is obtained: eg/He = n/2 (n being an integer and g being measured with the same units as e). Without quite answering the question, this shows that the existence of a single monopole 787
788
would explain the quantification of electricity. However, Dirac does not at all mention the symmetry laws. (4) Dirac's article was followed by thousands of others. Two of them brought some weight to the theory, without bringing anything new regarding the possible observation of a monopole. In 1974, t'Hoff and Poliakov showed that non-Abelian gauges in the Grand Unification Theories impose the existence of magnetic monopoles. However, they do not describe their symmetry laws and they assume a mass of 1016 GeV/c 2 which excludes any laboratory production, it is therefore believed that they were only produced at the time of the Big Bang. (5) Due to the difficulties in observing monopoles, it has been thought that they have a very high mass. It was assumed also that they are bosons with strong interaction. Therefore, the theory that I proposed in 1983 of a Fermionic monopole with zero mass and weak interaction might have looked absurd, even though it was anchored in the Dirac's electron equation, and looks like the magnetic side of the electron (which a monopole is very close to), while obeying other symmetry laws. Moreover the theory is based on experimental arguments and Curie's symmetry laws come out automatically from this formalism. 2. Formal Basis of the Theory Given the Dirac's matrices 7 P and r^v of Clifford: Tiv = {I, In, ilp.lv, ilpls, 75 = 71727374} (M = 1 , . . . , 4; N = 1 , . . . , 16) : They are linked by the Pauli relations (the sign ± depends of /J, and N):10 7 ^ * 7 / . = ±TN.
(1)
As a result, only two matrices T^ commute the same way with the four 7^ matrices: Ti = I (with the + sign) and r 1 6 = 75 (with the — sign). The first defines the phase invariance of Dirac's equation ip -^ e^ip: 1 , 8 ^ + ^ = 0.
(2)
The second defines another invariance, ip -> e i 7 5 V,
(3)
= 0.
(4)
but for the null mass equation:
l M
The usual phase invariance allows the introduction in (2) of a covariant derivative and a local gauge: VM = a M - i ^ A M ;
$^jW*1>,
A^A^
+ d^,
(5)
789
they define the Dirac's equation for the electron:
Similarly, thanks to the global gauge we can define (3) a covariant derivative and a local gauge: VM = ^ - ^
7
5 ^ ;
1>->jW*h**fr
B^B^
+ id^.
(7)
We obtain an equation, which is the magnetic analogue of the Dirac's one: 7 - 1 1
7^ (aM - j-.^B>)
(8)
* = °-
Due to the presence in (7) and (8), of the pseudo-scalar-matrix 75, g is a scalar quantity, just like all other physical constants, contrary to what is usually admitted for the magnetic monopole charge. This present theory is purely a quantum theory, and the chirality of the magnetism is expressed through the charge operator: G = 575-
(9)
As (6) produces vectorial electric current conservation: V
M
= 0
(J^ = i ^ 7 ^ ) -
(10)
Equation (8) conserves a pseudo-vectorial-magnetic current E^: 0 ^
= 0
(EM = ^ 7 M 7 5 ^ ) ,
(11)
JM and S^ are linked together by the algebraic formulas:
Vt\ and f^2 a r e ; respectively, the invariant and the pseudo-invariant of Dirac. From (12), the electric current JM is as expected time-like, but the magnetic current is of space like, which appears catastrophic for a current. But this is not the case as we can see it in the Weyl's representation: -^=(74+75^= Q ) ,
(13)
because it splits Eq. (8) in two parts left and right:
1 &
-Cdt+s-v+[hw-s-B^
(14)
\
= °>
s are the Pauli matrices, iB M = {B, \W} where B and W are, respectively, a pseudovector and a pseudo-scalar in R3. The component B4 = W is real because B^ is axial. The left and right currents
Xl* = {t+Z,S+a€h
Yy. = {(+C(+sQ
(15)
790
are conservative: d^X^ = 0; d^Y^ = 0 and they are isotropic, this is normal for a massless particle. The previous two currents are equal to: JM = X^ + y„;
EM = X^ - r M .
(16)
We see that SM is not the total magnetic current but the difference between the left and right currents. Therefore, its genre is not defined and the fact that it is space like is due to: X^Y^ = 4|£ + C|2 > 0, which is without relation to causality a . 3. Can We Talk About Monopole? Theoretical Answers (1) The P, T, and C symmetries of Eq. (14) are Ref. 4: P •
g -> g, xk-^ -xk, t -> t, Bk ^Bk, W - - W , $ <- C
T:
g-*g, xk^xk, t^-t, Bk^-Bk, W^W, £->s2f, g^g, t^-is2(*, C-^^r
C:
.
(17)
C-«2C*
This is in agreement with Curie's laws, 2 ' 3 completed by the transformations of time t and charge g. P, T, and C invariances are obtained because chirality is given by the charge operator G = gy$ and the sign of its eigenvalues ±g(2) The pseudo-potentials iB^ = {B, iW} are those of Cabibbo and Ferrari 12 and come from the gauge law (7). Actually, they already appear in my theory of the "magnetic photon" and in the old theory of light of de Broglie. 13 ' 14 (3) The currents JM and S^ are not colinear, therefore the theory cannot be reduced to the theory of the electron (classical objection against the monopole: see Refs. 8 and 10). (4) In geometrical optics, Eq. (14) becomes 8 ' 10 the Poincare equation, 15 which is the Birkeland effect theory. In the Birkeland experiment, a magnet pole (therefore a fixed monopole) focalises cathode rays (electrons) in a Crookes tube. Symmetrically the light monopoles must do the same in a Coulombian field. Therefore, the optical geometry approximation (14) gives rise to the Poincare equation. Let us introduce in (14): £ = a&lS'h. At zero order in h we find:
"1 fdS_ gw\ - (VS + ^B) c \dt
a = 0.
(18)
By cancelling the determinant we obtain the massless Hamilton-Jacobi equation:
MM 2 -( vs+ ' B ) 2 =°a
(19)
If we make the sum and the difference of two isotropic vectors, one is time like, and the other is space like. For Dirac, the sum is time like. This is why we can interpret J M as an electric current and as a probability current. This is where the causality principle intervenes.
791
In a Coulombian field it gives the Poincare equation: d2r
1 dr
,
egc
.„_,.
The minus sign comes from the choice of a left monopole in (14). Poincare had found A = eg/mc because the impulsion was p = mv. Here we have: m = 0 but as there is energy conservation, p = (E/c2)v; this is the origin of our value for A. Poincare showed that the symmetry axis r that passes through the two charges (electric and magnetic) draws a cone around the total moment of the momentum: dr r A = r x ^ + A-. at r
(21)
The expression A(r/r) is the moment of the field (J.J. Thomson). The Poincare cone is identical to the Poinsot cone because the angular momentum of the monopole around an electric charge is the one of a symmetric spinning top around a fixed center. 10 The fact that all comes from (14) is a strong argument for the theory, because the Birkeland effect is an experimental proof of the equation of Poincare, and by symmetry a proof of a monopole around an electric charge. Let us see the quantum problem for the angular part. 8 ' 10 Dirac introduced a potential, which has no definite symmetry. But we choose an axial symmetric gauge: e yz &x = -—^-]—o'
e —xz ^s = " T ^ — 2 '
Bz
=
°'
( 22 )
From (14), we deduce the left and right conservative moments. We find h A+ + is
A_
'C
h A
l +-B
(23)
A± = r ( - i V ± DB) ± D(D = ^-,B = eB) r V nc ) where D is the Dirac number eg/he (that we have seen above) and A^ is the quantum expression of the Poincare moment (21). It can be shown that the A1*1 are infinitesimal operators of the rotation group. Their eigen states are therefore elements of matrices Dj1 'm(9,
792
- All these make sense only if the eigen functions of the operators A^1 are continuous on the rotation group. We need: g(7
2/7,
D = ^ - = m ' = -j, -j + 1 , . . . , j - l , j ;
1
j=—-—ou:j
= n.
(24)
We see that the values of D are not deduced arbitrarily from the phase, but from the continuity of the movement on the rotations group. This quantifies the projection hm' of the total moment on the symmetry axes. This is what quantifies the charge: m' ff = e —
( e2 . I a = — ;m = -J,-J+
\ 1,... ,j - 1, j 1 .
(25)
- For a given electric charge e, the values of g split in families having (2j + l) elements, associated to the values j of the kinetic moment. These families are divided in pairs of opposite signs of m', corresponding to opposite magnetic charges. But these opposite values do not correspond to a charge conjugaison and cannot be exchanged through any unitarian transformation. They correspond to half angles at the summit >7r/2 or <7r/2 of the Poincare's cone. Two monopoles of opposite charge can therefore be either of opposed chirality and charge conjugate or have same chirality with supplementary half angles at the summit. - The families of values of g split again in two categories corresponding to the Dj representations of order j (and therefore m'), half integer or integer. For m! integer the charge of the monopole is g = 137m'e: we find Dirac's result. - Fundamental point: the integer m' includes the value m! = 0, therefore 5 = 0 and the Eq. (14) become the neutrino equation. The neutrino is therefore a zero charge monopole. We can therefore assume that the monopole is a magnetically excited state of the neutrino. It can therefore play a part in weak interactions, and be produced in place of a neutrino in /^-disintegration, or inversely produce them. 4. Can We Talk About a Monopole? Experimental Answer The first experiments started in 1998 at the Kurtchatov Institute near Moscow under the direction of Leonid Urutskoiev. He inspired a trend developed in particular at the Unified Institute of Nuclear Research in Dubna under the direction of Vladimir Kouznetsov, in the General Physics Institute of the Russian Science Academy under the direction of Henri Rukhadze and at the University of Kazan under the direction of Nicolas Ivoilov (who also takes part in the Urutskoiev team). As often happens, it is an adventitious aspect of the theory, the hypothesis of the action of monopoles on weak interaction that attracted attention. The Urutskoiev team unexpectedly discovered a redistribution of isotopes in titanium foils following electrical discharges (0.1 ms, 5 kV, 60 kJ) in a liquid medium, as well as the appearance of chemical elements that were initially absent, and this without radioactivity. The effect is reproducible with great precision in spite of
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some variations 1 6 - 1 9 . The nuclear aspect of the observed effect, the absence of strong interactions and the low energies implied have suggested the role of the weak interaction, but their small cross section suggests the presence of a catalyst that needs to be found. In addition, this phenomenon produces "strange radiation," in part electromagnetic. It includes lines produced by the newly created elements following the electric discharge, and also identified by mass spectrometry on the titanium scraps. But it also carries "something else": particles that produces tracks on photographic emulsions that specialists had never seen before, thick broken lines in the shape of caterpillars corresponding to an electric charge of 1 GeV. But this is not confirmed by the presence of electrons 5 and by the fact that the particles can go through several meters of other materials. Therefore, they cannot be electric charges, however, they cannot be neutral either, since they produce tracks that neutral particles do not. 4.1. On the Contrary,
the Particles
React to a Magnetic
Field
(1) A magnetic field of 20 oersted applied at the source of the radiation changes the tracks in the form of "comets" several meters away. (2) A happy coincidence is that Fe 57 , the isotope most sensitive to the Mossbauer effect, is at the same time magnetic. It is a monopole trap. A sample of Fe 57 submitted to the "strange radiation" a few meters away from the source with the pole of a magnet that pushes out the (assumed) monopoles of a given sign and attracts the others. The sample is then studied for the Mossbauer effect with its characteristic gamma ray. This line is clearly displaced. When the experiment is repeated, changing the pole of the magnet, the displacement is in the other direction. This suggests that we have trapped the North and South monopoles in the incident mixture. (3) The preceding section shows that the "strange radiation" produces an induced magnetism that remains during transportation of the samples. In reality, the irradiation was performed in Moscow and at Urutskoiev's lab; and the Mossbauer measurement was made in Kazan several hours later at Ivoilov's lab, with the Fe 57 sample being transported by air several hours later. Another sign of induced magnetism is the fact that we have noticed that titanium fragments after the electric discharge is attracted by a magnet (even though titanium is not a magnetic metal). In addition we have noticed that a Pietri box irradiated a few meters from the source, then moved away and placed in a cabinet on a photographic film wrapped in a black paper shows the caterpillars type tracks. (These observations are dedicated to Henri Becquerel!)
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But all those effects induced by the monopoles disappear after about 3 days: this lifetime is not predicted by the present theory.
4.2. Other Distance
Effects
(a) Chemical action: the monopoles destroy ammonium nitrate (NH4NO3) several meters away. Experiments have been performed following the AZF disaster in Toulouse by L. Urutskoiev, with the contribution of an explosives specialist. The purpose being to check if it is possible that a powerful electrical discharge can emit a flow of monopoles that can ignites a stockpile of ammonium nitrate. This hypothesis was made because the same suspicion had been assumed about the electrical explosion that occurred in the engine room of the Chernobyl nuclear plant a few seconds before the disaster. That might have been the origin of the disaster by sending a flow of monopoles in the reactor. In both cases, the answer appears positive, but obviously without being able to prove that it has been really the case. In any case, the experiment with the ammonium nitrate demonstrates the action at distance of the "strange radiation." (b) Biological action: A team of biologists from Chelyabinsk has performed experiments under the direction of Pryakhin, with the help of Urutskoiev. They have submitted mice to the "strange radiation" one meter from the monopole source. 20 They have noticed that the radiation increases the number of cells in the bone marrow by increasing cell division. The radiation does not seem, until now, to produce gene toxicity, but it decreases one and half times the gene toxicity effect produced by gamma rays. Biologists see there an "adaptative response." (c) Chiral images: In Kazan, Ivoilov has produced monopoles having much less energy than those made by Urutskoiev. They even leave tracks on photographic films, but with more turbulent shapes. Moreover Ivoilov, using a monopole mirror, has obtained on the same photographic film the outward and return tracks that we can consider as the one of the same monopoles after reflection. Tracks exhibit such complex inverted patterns that it is possible the same monopole is detected. The fact that tracks are identical seems to be attributed to the chirality of the monopole, which should be an important result. However, two questions remain: (a) Both tracks are rotated by ' V one with respect to the other in the mirror plane, (b) These observations raise the same question as the one observed by all tracks of monopoles: they are in a plane perpendicular to the source. If they were in an arbitrary plane, we could understand it easily because of the random interaction with the nuclei and the surrounding air. But why the orthogonality? All this is part of the charm of a new science. But the apparition of the chirality is so dear to the theory that it deserves to be mentioned.
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4.3. Last Questions:
Uranium Enrichment
and
j3-Radioactivity
We have just described the distance effect that suggests the phenomenon produced by electric discharges in a liquid is due to the propagation of a radiation transporting particules. Some of their effects show that they must be charged with magnetism. But almost all the effects described above are not of a classical nuclear origin; we assert that they are transmutations - and more precisely, isotopic composition changes - of some elements. This attracted the attention of Urutskoiev, and led him to support the monopole theory described in this paper. Several physicists have suggested that these transmutations could be due to electron accumulation, clusters created by the electric discharge, but made elusive by the proximity of electrons and Coulomb repulsion. Urutskoiev and I do not believe this. However, I will not try here to give all the details of his experimental refutation, which is fairly complicated. I will simply sketch it by referring the reader to Ref. 18 and references thereof. 1. Enrichment Uranium 238 U —> 235 U: Urutskoiev et al. have experimented with this example. In a compressed polystyrene test tube filled with water, with a thin titanium conductor that will explode following the electric discharge, they dilute in the water a uranium salt UO2SO4,18 with the natural isotopic distribution. The two isotopes 238 U and 235 U are easily identified by their respective radioactivity. Following the electric discharge, the uranium is considerably enriched with 235 U. In fact it is easy to demonstrate that there was no transmutation of 238 U in 235 U. Both have decreased, although at different rates in favour of 2 3 5 U. But how much have they decreased? There are two possibilities: either the quantity of isotopes decreases only in the thin plasma region that surrounds the titanium conductor (therefore by the accumulation of the electric charges that are produced) or this quantity decreases in all of the test tube (the uranium salt is uniformly diluted). We can predict a large difference since the volumes of the test tube and the plasma region are in the ratio of 2000:1. This shows that the phenomenon is not located near the plasma region, but is produced over a large volume of the test tube. We favour the thesis that the phenomenon was created by a radiation emitted by the titanium conductor propagating in space. This confirms the examples quoted above: the monopole hypothesis is reinforced. The difference with the previous examples being that this is a nuclear phenomenon. 2. p-radioactivity: It is known that there are atoms that have nuclear states so unstable their half life is influenced by the chemical state of the atom, i.e. the electronic cloud. 2 1 - 2 4 This is the case of some /3-radioactivity: for example in the case of rhenium 187 Re its P half-life decreases by 25% if the atom is entirely ionized.24 Urutskoiev has compared this phenomenon to the Kadomtsev effect, which is the deformation of the electron cloud under the influence of a strong magnetic field.25 The atom takes a cigar-like shape around which the atomic trajectories wind up. The resulting extension moves away the electrons from the nucleus during part of
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their revolution. This is equivalent to ionization. If the nucleus is /3-radioactive one can expect a decrease of the half time. Unfortunately, calculation shows t h a t the magnetic field t h a t would be necessary to reach a sufficient deformation of the electronic cloud would be gigantic, around 10 9 oersteds. But Urutskoiev and Filippov have noticed t h a t since nothing prevents a monopole from approaching the nucleus, a moving monopole (which we should not forget, is very light) will be able to create a large magnetic field. Preliminary experiments seem to indicate t h a t the half time of a /3-radioactive sample decreases under the effect a flow of monopoles. Indeed, in the disintegration of uranium there is the formation of thorium, which is /3-radioactive. T h o r i u m has disappeared; there is no trace left, which is very abnormal. Therefore we can make the hypothesis t h a t its half-life time has been strongly decreased under the effect of the monopoles flow. Future research will determine if this is true.
References 1. J. C. Maxwell, A treatise on electricity end magnetism(1873), 3rd edn (Clarendon Press, 1891, Dover, 1954). 2. P. Curie, Sur la symetrie dans les phenomenes physiques, J. de Phys. 3 e serie, t.III, 393 (1894); Annates de la Fondation Louis de Broglie 19, 137 (1994). 3. P. Curie, Sur la possibility d'existence de la conductibilite magnetique et du magnetisme libre, id. p.415. (Annates de la Fondation Louis de Broglie, 19, 159 (1994). 4. G. Lochak, Les symetries P,T,C, les solutions a energie negatives et la representation des antiparticules dans les equations spinorielles, partie I, Annales de la Fondation Louis de Broglie, 22, 1 (1997); partie II, id. 22, 187 (1997). 5. P. A. M. Dirac, Proc. Royl Soc. Ser. A 133, 60 (1931). 6. W. Pauli, Annales de I'Institut Henri Poincare 6, 109 (1936). 7. G. Lochak, Sur un monopole de masse nulle decrit par l'equation de Dirac, et sur une equation generale non lineaire qui contient des monopoles de spin 1/2 Annales de la Fondation Louis de Broglie, 8, 345 (1983) (I). 9, 5 (1984) (II). 8. G. Lochak, Wave equation for a magnetic monopole, IJTP 24, 1019 (1985). 9. G. Lochak, The symmetry between electricity and magnetism and the wave equation of a spin 1/2 magnetic monopole, in Information, Complexity and Control in Quantum Physics (Springer, Wien, 1987). 10. G. Lochak, The Symmetry Between Electricity and Magnetism and the Problem of the Existence of a Magnetic Monopole, Contribution au Recueil: Advanced Electromagnetism, T.W. Barrett and D.M. Grimes (eds.) (World Scientific, Singapore, 1995), pp. 105-148. 11. G. Lochak, L'equation de Dirac sur le cone de lumiere. Electrons de Majorana et monopoles magnetiques, Annales de la Fondation Louis de Broglie 28, 403 (2003). 12. N. Cabibbo and G. Ferrari, Nuovo Cimento 23, 1147 (1962). 13. G. Lochak, Sur la presence d'un second photon dans la theorie de la lumiere de Louis de Broglie, Annales de la Fondation Louis de Broglie 20, 111 (1995). 14. Th. Borne, G. Lochak, H. Stumpf, Nonperturbative Quantum Filed Theory and the Structure of the Matter (Kluwer, Dordrecht, 2000). 15. H. Poincare, Comptes rendus, 123, 530 (1896). 16. L. Urutskoiev, V. Liksonov, V. Tsinoev, Oservation of transmutation of chemical elements during electric discharge, Journal de radioelectronique, No. 3, 2000 (in Russian), Annales de la Fondation Louis de Broglie, 27, 701 (2002), (in French).
797 17. V. Kuznetsov, G. Mishinsky, F. Penkov, V. Arbuzov, Zhemenik, Low energy transmutation of atomic nuclei of chemical elements, Annales de la Fondation Louis de Broglie, 28, 173 (2003). 18. G. Lochak, L. Urutskoiev, in Proceedings of ICCF11 (Marseilles 2004: quoted thereafter as CCTBEM 2004). 19. Proceedings of the Russian participants at: CCTBEM 2004. 20. E. Priakhine, L. Urutskoiev, G. Tryapitsina, A. Akleyev, Assessment of the biological effects of "Strang" radiation, CCTBEM 2004. 21. R. Daudel, M. Jean, Lecoin, J. Phys. Radium 8, 238 (1947). 22. K. T. Brainbridge, M. Goldhaber, E. Wilson, Phys. Rev. 84, 1260 (1951). 23. S. Batkin, Izvestia of the Academy of Sciences of S.S.S.R. (en russe) 40, 1980 (1976). 24. F. Bosch, T. Faesterman, J. Friese, F. Heine, P. Kienle, E. Wefers, Zeitelhack, K. Beckert, B. Franzke, O. Klepper, C. Kozhuharov, G. Menzel, R. Moshammer, F. Nolden, H. Reich, B. Schlitt, M. Steck, T. Stolker, T. Winkler, K. Takahashi, Phys. Letters 77, 5190 (1996). 25. B. Kadomtsev, Selected papers (in Russian) t. I, II, Fizmatlit, Moscou, 2003, Matter in a super powerfulmagnetic field, II p.483.
ELECTRONS CLUSTERS A N D M A G N E T I C MONOPOLES
M. R A M B A U T 57H rue De La Hacquiniere, 91440, Bures-sur-Yvette, E-mail: [email protected]
France
It is shown that there exists the possibility of producing bursts of magnetic monopoles using properties of largely ionized condensed media, where electron accumulations or clusters are used. A spontaneous gauge symmetry breaking occurs when the electrons, constituting the cluster, are sufficiently close together to open the way to the creation of a topological defect, which is known to have in this case the properties of a magnetic monopole. Those properties of magnetic monopoles, grounded in this way, in the context of quantum theory of fields, are not contradictory with the initial concept proposed by Dirac, but conversely complete this model, showing the possibility of producing monopoles and to observe them in laboratory with relatively low energy devices.
1. Introduction An accumulation of electrons, or cluster, is a macroscopic entity first brought into evidence in Russia by Mesyats 1 as early as the 1960s. Mesyats called this cluster an "Ecton." Later in the United States, during the 1980s, Kenneth Shoulders2 created clusters and named them "Electrum validum" (from Latin, "Strong Electron"). According to specific experiments, the shape of an electrons accumulation is spherical and a typical cluster of radius 3/xm may contain as many as 2 x 1010 electrons. 3 To perform Coulomb barrier screening and obtain D-D nuclear fusions, some 103 electrons may be sufficient.4 The mean distance between electrons in the cluster is typically in the range of the electron Compton wavelength (2.426 x 1 0 - 1 2 m). The most typical way of obtaining electron clusters seems to have been the use of rough surfaces of electrodes in a discharge device.1 To account for the transitory cohesion of electron clusters, it seems sufficient to take into account the interaction between the spin of electrons. Other causes such as the Casimir effect seeming to be ruled out. 5 The electron clusters seemed at first to be only interesting for their great energy density. But the capacity they have of producing "screening" of two colliding charged particles opened the way for a new use of those macroscopic entities in physics experiments. 4 It seems that the role and efficiency of electron clusters is being progressively recognized as being fundamental to low energy transmutation processes. In many experiments that are known not to involve any thermonuclear process, yet which lead nevertheless to fusion reactions, one can invoke the role of electron clusters as being essential. But in some experiments, when photo798
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graphic emulsions were used, strange tracks appeared. Given their large transversal dimension and their length, they could correspond to any charged particle. Urutskoev et al.7 were the first to go on record with the proposal that those tracks could be due to magnetic monopoles. Their experiments were successfully reproduced in two other laboratories. 8 ~ n Given the shape of those abnormal tracks, they were called "caterpillar" in a picturesque and vivid way. But, some years before, there was at least one experiment where similar tracks were observed and curiously called also "caterpillar" without any mention to magnetic monopole by Dash et al.12 The experiments consisted of making nuclei to react in a glow discharge chamber, the plasma being rich in electrons. Those experiments were in fact very close to the ones of Urutskoev, if we consider them from the point of view of electrons accumulation. 5 ' 6 In another terms, it appears that the same phenomenon has been independently observed in several laboratories: a particle track having the shape of a "caterpillar" in a film. The magnetic monopoles production in plasmas becomes an heuristic hypothesis.
2. Process of Electron Cluster Formation There are many ways of creating electron accumulations. The life of those accumulations is typically between 10 ns and 10/xs. For example, Mesyats makes a rough cathode, which produces bursts of electrons, owing to the roughness of this cathode. But there is another method, which consists of creating, from a plasma, an LPS ("Large Poincare System"), according the terminology of Ilya Prigogine. 13 Many various different resonances occur in an LPS. One has to emphasize that the term LPS was coined initially to describe energies at the atomic level, but seems well suited for larger ones, typically from a few keV up to some tens of keV, and perhaps above. This method is valuable in the case of monopole creation, as it is shown below. Given the existence of LPS, charged particles, that is atom nuclei and electrons, can be considered as being quasi-free. Their 3D distribution is ruled by Poisson law. Thus, the Pp probability for a microvolume V, containing p nuclei, /x being the mean number of nuclei per V-volume, reads: Pp = e - " ( ^ / p ! ) " .
(1)
Considering this ^-microvolume leads to evaluate the order of range of the mean number of trapped electrons v around two colliding nuclei. The interesting sites of this distribution are the ones where two nuclei collisions occur. The probability of finding two nuclei in the V volume is
P2 = e-»{n2/2\r.
(2)
Given the high electron mobility in comparison with the one of nuclei, when two nuclei come close, this produces a small potential well, which prompts a transitory electron accumulation. 4 The ratio between the probability of filling a F-microvolume by one unique nucleus, and the probability of filling it by two nuclei is equal to the
800
number of electrons v surrounding two colliding nuclei (whose distance is smaller than the Bohr atom radius) v = 2/fiv.
(3)
This model, originally built to take into account non-thermonuclear fusion reactions in a plasma, seems to be valid for other processes that put a condensed medium into cold conditions (Fig. 1): (1) Cells for cold fusion (Fleischman and Pons). (2) Beams of D2O impinging on a metallic target filled with D nuclei (Brookhaven National Laboratory during the 1980s). (3) Pulsed currents through a condensed and deuterated medium (NRL, Kiel, during the 1970s and 1980s, and others). This model is grounded on two specific particulars: 4-6 • The use of specific dimensional relationship replacing the "Lawson criterion," which is only applicable to a thermonuclear process. • The fractal dimension of the two nuclei collision space, deduced from use of the Poisson statistic. Moreover, this model is not restricted to fusion reactions, as it is in agreement with pulsed low energy transmutations, for example those that have been put in evidence in experiments performed in the Kourtchatov Institute. 7 ~ u
Tm3/s
f
/Jt/
D—D (Thermonuclear)
X Kiel P NRL '}<( Brookhaven —• Cold fusion (typical range)
1
10+5
_i__
_i
E
eV
Figure 1. Representative points of typical non-thermonuclear experiments, showing the specific place of cold fusion. Bach straight line corresponds to a specific electron number.
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3. Monopole Creation One has to emphasize the difference between our hypothesis and conventional thinking about the magnetic monopole problem. In our case, one has to describe the system inside the electrons accumulation, by mathematical entities, which are as much as possible faithful to reality, in the framework of quantum field theory. Whereas from the purely theoretical point of view, people are "free" to choose, for example, any gauge group, which ensures the success in any way of theoretical magnetic monopole creation but without any other requirement. Let us keep the hypothesis that the electrons that constitute a transitory accumulation initially take part in the LPS: they are quasi-free, as mentioned before. From the quantum field theory point of view, the Hamiltonian at some x site remains quasi-constant as long as it not submitted to a local interaction, particularly to the field gradient around two colliding nuclei. From a pure experimental point of view, as long as the spatial distribution of electrons is loose enough that we can neglect their interaction, a gauge group G rules the space structure at this specific x place. Apparently, to describe a non-interacting electron, one has to take into account only the rotation, no matter what the interval is between electrons, if one can suppose they do not interact. The evident choice is thus SO(3), the continuous group of all proper rotations in 3D Euclidean space. The Hamiltonian H of two electrons constituting a non-interacting system is the sum of the Hamiltonians H\ and H2 of two electrons: H^H1+H2.
(4)
Thus G, the gauge group, is the product of the combination law, between of two elements of SO (3): G = SO(3) x SO(3).
(5)
But, when the electron accumulation is sufficiently formed, a gauge symmetry breaking occurs and the only invariance which remains is ruled by SO(3) alone, a subgroup of SO(3) x SO(3). There are two causes for gauge breaking: (1) The repulsive Coulomb forces of the negatively charged electrons. (2) The spin-spin interaction whose range is shorter. 5 ' 6 According to this general scheme, topologically non-trivial field configurations are classified according to the second homotopy group 7T2(G/SO(3)). Moreover, in this specific case, one has the equality (6), SO(3) being considered as containing the U(l) of electromagnetism: 14 7r 2 (G/SO(3))=7r 1 (SO(3)) = Z 2 ,
(6)
7i"i is the first homotopy group. Thus, given (5), there is, in this case, one specific sort of monopole with the first and the second homotopy group being identical.
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In this process one unique sort of monopole is produced. It corresponds to the element -1 of Z%. This case, involving an electron accumulation, is thus different from the one considered by 't Hooft and Polyakov.15 According to their model, magnetic monopoles, which are considered as being extended field configurations,14 arise when a simply connected group G is broken to the U(l) of electromagnetism. The topology relationship between homotopy groups is different from the preceding one: 7r 2 (G/U(l))=7r 1 (U(l)) = Z.
(7)
Z is the group of addition of positive and negative numbers. It means that the topological defect, which constitutes the monopole may be considered as being made of an infinity of curves. 15 One shows that such a magnetic monopole carries a quantum number u, which is an integer positive or negative. This r\ number is called the "winding number". The group structure of Z shows that this r\ quantum number is conserved. Thus, in the 't Hooft case, two monopoles can fuse together to form a monopole whose quantum number is the sum of the two quantum numbers (77+77/). As for the magnetic moment g, it is proportional to the winding number and inversely proportional to the electric charge: g = -(r]/e)ar]a,
(8)
a being the fine structure constant. In our case of magnetic monopole creation by electron accumulation, there is only one sort of monopole, which can annihilate only in pairs. And the absolute value of g is unique: g = (l/e)aa.
(9)
Those relationships giving g are somewhat in agreement with the point of view of Dirac who demonstrated, with the help of the classical formalism, and supposing each pole to be at the end of an unobservable string, that: g = -{v/e)a/2va.
(10)
In fact, various experiments show that the multiplying factor should be a / 6 (the value quoted in Ref. 16). To prove the existence of a monopole in the most direct and convincing way, Lochak uses the Dirac equation which has been initially developed to describing relativistic electrons. As shown by Lochak, this equation admits not only one local gauge invariance, but two, and no more. 16 Moreover, the magnetic monopole could be a magnetically excited neutrino. But this way does not seem to give the possibility of describing any monopole creation channel. 3.1. Energy and
Mass
't Hooft and Poliakof utilize a relativistic Lagrangian density to get an evaluation of the monopole energy and mass. This Lagrangian is useful in the domain of particle physics. They obtain for the mass: M m = (4ir/c2)MwC(/3)nP,
(11)
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C(/3) depends not much of /3: it varies between 1.1 and 1.4 for 0.1
Bursts
of Magnetic
Monopoles
By the way, we must mention that it is possible to get experimentally an important magnetic monopole number, if they are generated in electron accumulations, which are on the sites of the two-nuclei collisions. Assuming it is so, each electron accumulation would prompt a magnetic monopole, With this hypothesis, n being the number of electrons per volume unit, the (/x2n/2) term is equal to the magnetic monopole number which are generated in the volume unit. This volume being supposed turned into a unique LPS. For example, if the mean number of nucleon per V volume reads: (V = Bohr radius) 3 = (0.529 x 10~ 8 cm) 3 , n = 1022 nuclei/cm 3 ,// = 1 0 " 3 , e - " ^ l , i / = 2 x 10 3 (/x 2 n/2) = 5 x 10 15 , n = 10 23 nuclei/cm 3 , a = 2 x 1 0 - 3 , e _ / J ^ l,v = 103(/Lt2n/2) = 2 x 10 17 . Suppose the magnetic monopole generation takes place during the trailing edge of a pulse current, as in the case where an electron accumulation prompts fusion reactions by lowering of Coulomb barrier. Then one gets what can be called a "burst" of 5 x 1015 to 2 x 10 17 magnetic monopoles per cubic centimeter. But we must emphasize this hypothesis: the whole volume appears to be turned into an LPS, and every electron accumulation prompts a magnetic monopole. 3.3. Experimental
Evidence
Let us consider two kinds of results: first, ones relating the working of electron accumulations as a screening device for lowering the Coulomb barrier and prompting low energy nuclear reactions. Second, ones relating its working as magnetic monopole creation. We must emphasize the fact that results at this time indicate that if we succeed in creating a Large Poincare System in a condensed medium,
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it produces low energy nuclear reactions and bursts of magnetic monopoles on an equal footing. 5 ' 6 Systematic experiments are still necessary to understand if there exists the probability of magnetic monopole production, versus a low energy nuclear reaction probability, and perhaps of simultaneous production, which we have no reason to exclude at present. From a purely experimental point of view, one can only put forward the fact t h a t transmutation at atomic level energies shows u p when a capacitor bank is discharged through a metallic foil and a volume of liquid, connected in series. T h e liquid can be ordinary t a p water. It has been sufficient to use a 4.8 kV, 50 kJ capacitor bank. 7 So one can use a very simple experimental device. T h e simultaneous occurrence of atomic level transmutations and of a plasma-like sphere, or ball lightning, is the mark of an experiment t h a t is working well. 7 - 1 1 ' 1 7 It is also relatively simple to detect transmutations by examining the remains of t h e foils, inside which atomic t r a n s m u t a t i o n s occur, and to analyze t h e m by mass spectrometry. It seems, given their creation process, t h a t the interaction of magnetic monopoles with m a t t e r is rather different from the one with charged particles. But the simple use of nuclear films has been sufficient, during the first experiments to estimate t h a t the process is completely replicatable. 7 - 1 1 4.
Conclusion
This simple analysis confirms t h a t the process of magnetic monopole creation is possible in a laboratory, concurrently with low-energy nuclear reactions production. This possibility is new in the quest for "magnetic monopole hunting." In fact, to p u t the device into the proper condition, one would need "only" ionize a condensed medium and to initialize an LPS, to let electrons to crowd together. So particle physics could benefit from a low energy device of a condensed medium, with new experimental possibilities. References 1. G. A. Mesyats, Ectons processes at the cathode in a vacuum discharge, in Proceedings of the 17th International Symposium on Discharges and Electrical Insulation in Vacuum, 1996, pp. 720-731; G. A. Mesyats, Cathode Phenomena in a Vacuum Discharge (Nauka Publishers, Moscow, 2000); G. A. Mesyats, Explosive Electron Emission (URO Press, Ekaterinburg, 1998). 2. K. R. Shoulders, Ev - A Tale of Discovery (Austin, TX, 1987). A historical sketch of early EV work. Available from the author (PO Box 243, Bodega, CA 9492, E-mail [email protected]); K. R. Shoulders, U.S. Patent, 5,018,180 (1991), 5,054,046 (1991), 5,054,047 (1991), 5,123,039 (1992), 5,148,461 (1992); Ken Shoulders and Steve Shoulders, Observation on the role of charge clusters in nuclear cluster reactions, J. New Energy 1 (3) (1996). 3. Petr Beckmann, Electron clusters, Galilean Electrodynamics 1(3), 55-58 (1990). 4. M. Rambaut,Phys. Lett. A 164, 155-163 (1992); M. Rambaut, Frontiers of Cold Fusion, ICCF3 (Universal Academic Press Inc., Nagoya, October 21-25, 1993). 5. M. Rambaut, 'Accumulation d'electrons et vide quantique, Annales de la Fondation Louis De Broglie, 28(3-4), 465-483 (2003).
805 6. M. Rambaut, Electron clusters and nuclear fusion, in Colloquium: Is transmutation possible at energies of atomic levels (Paris, 26-27 November 2003). 7. L. I. Urutskoev, V. I. Liksonov, and V. G. Tsinoiev, Experimental detection of a strange radiation and of transmutation of chemical elements, J. Radioelectronics (3) (in Russian language) (2000). 8. N. G. Ivoilov, Effect of the strange radiation on the Fe Mossbauer spectrum, in Colloquium: Is transmutation possible at energies of atomic levels (Paris, 26-27 November 2003). 9. L. I. Urutskoev, Review of experimental results on low-energy transformation of nucleus, in Colloquium: Is transmutation possible at energies of atomic levels (Paris, 26-27 November 2003). 10. V. D. Kouznetzov and G. V. Myshinskii, Low level energy transmutations in chemical elements, in Colloquium: Is transmutation possible at energies of atomic levels (Paris, 26-27 November 2003). 11. D. V. Filippov, A. A. Rukhadze, and L. I. Urutskoev, Effect of atomic electrons on stability and radioactive decay, in Colloquium: Is transmutation possible at energies of atomic levels (Paris, 26-27 November 2003). 12. I. Dash, H. Kozima, I. Savvatimova, S. Frantz, and E. Weis, Effect of glow discharge with hydrogen isotope plasmas on radioactivity of Uranium, in Proceedings 6th International Conference on Cold Fusion, 2002. 13. T. Petrovsky and I. Prigogine, Poincare resonances and the extension of classical dynamics, Chaos Solitons Fractals 5 (1995); T. Petrovsky and I. Prigogine, Quantum chaos, complex spectral representations and time-symmetry breaking, Chaos Solitons Fractals 4, 311 (1994). 14. Steven Weinberg, The Quantum Theory of Fields (Cambridge University Press, Cambridge, 2000). 15. G. 't Hooft, Magnetic monopoles in unified gauge theories, Nuclear Phys. B 79, 276284 (1974); A. M. Polyakov, JETP Lett. 20, 194 (1974). 16. G. Lochak, The symmetry between electricity and magnetism and the problem of the existence of a magnetic monopole. Advanced Electromagnetism, foundations, theory and applications, in Terence Barret and Dale M. Grimes (Eds.) (World Scientific, Singapore, 1995). 17. M. Rambaut, Unpublished data.
EFFECTS OF ATOMIC ELECTRONS ON N U C L E A R STABILITY A N D RADIOACTIVE DECAY
D. V. FILIPPOV AND L. I. URUTSKOEV RECOM Russian research Center "Kurchatov Institute", Russia A. A. RUKHADZE General Physics Institute Russian Academy of Science, Russia
1. Intoduction (1) The only valid (necessary and sufficient) condition for /3-stability of a nucleus is the minimum value of the mass of the atom (not of the nucleus) on the isobar line (i.e., atomic weight = const.). This condition holds true for all known isotopes without exception. (2) The condition of nuclear stability and the decay schemes of unstable nuclei depend on the state of the electron shells. Atom ionization and other perturbations in electron shells (caused, e.g., by magnetic fields) not only changes the decay periods of unstable nuclei,1'2 but also alters decay schemes3 and modifies the stability condition. For example, the 163 Dy, 193 Ir, 205 T1 nuclei, which are stable in neutral atoms, become /3-active when atoms are completely ionized. This means that by affecting electron shells one can alter conditions of nuclear /^-stability and thus initiate nuclear transmutations by means of weak interactions. (3) We have developed a phenomenological model for the low-energy nuclear transmutation. According to the above observations, the probability of a nuclear reaction can significantly increase under the effects exerted on atomic electron shells. Without considering specific mechanisms of nuclear transformations, we have managed to determine the possible transformation products only using basic conservation laws (the energy and electric, baryon, and lepton charges). Amazingly, such a simple model yields results in qualitative agreement with experimental data.
2. Condition of Nuclear /3-stability The discussion of the conditions for /^-stability of nuclei began at the very dawn of nuclear physics. 4 ' 5 However, up to the 1950s, because there was not sufficient accuracy or experimental data on the masses of nuclear isotopes, it was not possible 806
807
to assess the correspondence between theoretical forecasts and experimental data. Inasmuch as at that time the accuracy of available experimental data did not always allow researchers to distinguish between nuclear masses and atomic masses, the conditions of the "minimum nuclear mass," "minimum atomic mass," and "maximum nuclear binding energy" on the isobar line seemed to be identical, while deviations from the assumed stability conditions were considered as exceptions. 4 ' 5 Nowadays, thanks to available data, 6 it is possible to formulate (and check) an accurate condition for nuclear stability. The analysis of the database has shown that the stability conditions such as "minimum nuclear mass" 7,8 or "maximum binding energy" 9 on the isobar line are not accurate. The only condition for /3-stability of the nucleus in a neutral atom, which is absolutely accurate, is the requirement that the atom mass attains its minimum on the isobar. 10 ' 11 Let us discuss this statement in more detail. Consider the stability of a nucleus with respect to processes not involving a change in the number of nucleons in the nucleus, that is, those occurring due to weak interactions, namely, the electron (/3~) or positron (/3+) /3-decay and the K-capture: 2 X ^ 2 + 1 Y + e - + P e + Qi, £ X - 2 _ 1 Y + e+ + i/e + Q2, %yL + e-->2_1Y + ve + Q3,
(1)
where ve and ve are the electronic neutrino and antineutrino, respectively, and X and Y are the nuclei with the atomic weight A and charge Z (in the electron charge units). It is well known 10 ' 11 that the energy produced (Q > 0) or absorbed (Q < 0) in such nuclear reactions can be determined using the mass difference between the initial nuclei and the reaction products:
Q = MN(AX,ZX)
- MN(AY,ZY)
T me,
(2)
where MN(A, Z) is the mass of the nucleus ^X, me is the electron rest mass; a "—" corresponds to /^-decay (Q\ and Q 2 ), and a "+" to the K-capture (Q3). As the K-capture always involves less energy than the positron /3+-decay (Q 3 -Q2 = 2m e ), the possibility of a positron /3+-decay does not alter the nuclear stability condition.
MN{A,Z)
= (A-Z)mn
+ Zmp-WN(A,Z),
(3)
where m p and m n are the rest masses of the proton and neutron, respectively. The binding energy Wjq is the energy that is to be "pumped" to the nucleus to separate it into constituent nucleons. Expression (2) is valid in the case where the nucleus has no electron shell. When a nucleus decays as a part of a neutral atom, the binding energy of electrons is to be taken into account. Since the first ionization potential is not over 25 eV, this energy can be neglected when compared to the accuracy to
808
which the nuclear binding energy is measured (~1 keV). In this approximation, the energy produced in the K-capture and electron j3~ -decay of a neutral atom equals: Q = MA(AX,ZX)
- MA(AY,ZY),
(4)
where MA(A, Z) = (A-Z)mn
+ Z(mp + me) - W(A,Z)
(5)
is the mass of the atom and W is the binding energy of the nucleus in the atom taking into account the full atom ionization energy I{Z): W{A,Z)
= WN(A,Z) + I(Z).
(6)
This is the energy needed to separate a neutral atom into the constituent protons, neutrons, and electrons. With an accuracy of ZIn (IH = 13.6eV is the hydrogen ionization potential), which for Z < 100 is not worse than the accuracy to which the nuclear binding energy is measured, the energy defined in this way is the same as the energy needed to separate the nucleus into neutrons and hydrogen atoms: MK(A,Z)
= (A-Z)ma
+ ZMH-W(A,Z),
(7)
where M H is the mass of the hydrogen atom. Historically, the nuclear binding energy was introduced for calculating the energy produced in nuclear reactions involving neutral atoms. Therefore, tables 6 quote these atomic energies W, which include the full ionization potential I(Z), rather than the nuclear WN values. For determining the energy of the nucleus, one can also use the mass defect AM, which is related to MA as follows:6 MA(A,Z)=Ama.e.m.+AM(A,Z),
(8)
where m a e m . « 931.5MeV is the atomic mass unit; for the mass defect, the normalization AM( 1 2 C) = 0 was chosen. It is well known 10 ' 11 that for a nucleus to be /3-stable, it is sufficient that all possible decay channels be closed for energy reasons (Q < 0). Hence, the sufficient condition for /3-stability of a nucleus can be formulated as the minimum atomic mass MA(A,Z) [which is equivalent to the minimum mass defect AM(A,Z)}, including all local minima on the isobar (A = const.). Note that this requirement involves the minimum atomic mass MA(Z) and not the minimum nuclear mass M^{Z) or the maximum binding energy W(Z) (these conditions are not the same!). The functions MA(Z), M^(Z), and W(Z) are related to each other in the following way: MN(Z) = MA(Z) + I(Z)-Z-me, -W{Z) = MA{Z) -A-mn + Z-m,
(] {
'
where m = mn — m p — m e = 782.3 keV. Since the functions MJSS(Z) and W(Z) differ from MA(Z) on the isobars (A = const.) by terms monotonic in Z (9), then, in qualitative terms, all of these three
809
functions (MA, M N , W) feature the same behavior, but the minima of M N (Z) may be shifted to larger Z and the binding energy W(Z) maxima may be shifted to smaller Z with respect to the minima of the M\{Z) function [the latter are the same as the minima of AM(Z)]. The dependence of the binding energy on the nuclear charge can be qualitatively described by the well-known semi-empirical Weizsacker formula:11
MA(A,Z)
= Amn - Zm - av A + as A2/3 + ac
+«SYM
(lz£T A
Z(Z — 1) /3 (10)
~I(Z),
ap^P
where o v = 15.75 MeV, as = 17.8 MeV, aG = 0.71 MeV, aSYM = 94.8 MeV and a P = 34 MeV are the coefficients of the nuclear energy: the volume, surface, Coulomb, symmetry, and coupling energy, respectively. The coefficient 6 describes the coupling effect: 5 = 0 for the nuclei with odd A, 6 = 1 for even-even nuclei (an even number of neutrons and an even number of protons), and 8 = — 1 for odd-odd nuclei. The exponent P in the last term (coupling) varies, depending on the author, from 1/3 to 1. Recall the well-known fact which follows from the Weizsacker formula (10): on isobars with odd A, MA(Z) is described by a parabola with one minimum (8 = 0) (Fig. la); on isobars with even A, MA(Z) is described by a broken line confined by two parabolas which correspond to even Z (S > 0) and to odd Z (S < 0) (Fig. lb, c). In the latter case, the function MA(Z) can develop (depending on A) one, two, or three minima. Figure l b illustrates the case when, for even A, the parabola minimum corresponds to even Z, and Fig. lc shows the parabola minimum corresponding to odd Z.
(b)
/]
M,
"/ 23Z
<^
1 J I /
1
Ma
•^•j\
^0
^0
Figure 1. Dependence of the atomic mass on the charge. ZQ is the parabola minimum, (a) For odd atomic mass A, (b) for even A and even Zn, and (c) for even A and odd ZQ.
810
A straightforward analysis of the database 6 shows that all stable isotopes without an exception correspond to minima of atomic masses MA{Z) on the isobars. Moreover, all /3-decay and K-capture processes that are energetically allowed are realized in nature (no other prohibitions are involved). Thus the following statement is correct. For a nucleus in a neutral atom to be /3-stable (stable with respect to single /J^-decay and K-capture processes), it isnecessary and sufficient that this isotope correspond to a minimum of the atomic mass on the isobar (A = const.). Note that all 12 natural isotopes that do not correspond to a minimum of MA(Z) are unstable. Even though they are long lived, nevertheless they are not stable (Table 1). On the other hand, there are no natural ^-stable isotopes with atomic mass 5 or 8, as they are unstable with respect to decay: 5 He —> 4 He + n, 8 Be —> 24He. For atomic masses A > 141, a-decay becomes energetically allowed, while for some isotopes with atomic masses in the 210 > A > 141 range, it is forbidden, and all isotopes with A > 209 are a-active. The isotope 1 8 0 Ta m , which is observed in nature, is a long-lived (1.2 x 10 15 years) isomeric excited state of the nucleus. The very long half-life time is due to the large difference of spins in the isomeric (9~) and ground (1 + ) states. Table 1.
Isotope
Natural abundance (%)
Channels of nuclear decay
Energy of nuclear transition (keV)
Half life (years)
1311 1505 278 1037 2208 283
1.277 x 10 9
40K
0.012
P-
48
0.187 0.25
P~ P-
Ca
50y
Unstable natural isotopes.
89.3 e(P+) 10.7 17
s(P+) 83 87
Rb Zr 113 Cd
96
115In 123Te 138
La
176
Lu Re
187
180Tam
27.85 2.8 12.22 95.77 0.9 0.09 2.59 62.6 0.012
PPPP~ £
P~+
33.6 66.4
316 496 53 1044 1738 1192 2.66 75.3
6 x 10 1 8 1.4 x 10 1 7 4.75 x 10 1 0 3.8 x 10 1 9 7.7 x 10 1 5 4.4 x 10 1 4 > 10 1 3 1.05 x 10 1 1 3.78 x 10 1 0 4.35 x 10 1 0 1.2 x 10 1 5
The analysis of the database shows that the assumption that the minimum nuclear mass M^(Z) as a sufficient condition for /3-stability is not accurate. For example, more than 30 isotopes that correspond to minima of the nuclear mass M N ( Z ) on the isobars are unstable with respect to the K-capture. The following example describes a typical situation: the minimum atomic mass for the isobar with the atomic weight 55 is attained on only one stable manganese isotope 55 Mn, while the nuclear mass attains its minimum on the unstable isotope 55 Fe (the decay period is 2.7years).
811
The
55
Mn nucleus is heavier than the
55
Fe nucleus:
M N ( 5 5 Mn) - M N ( 55 Fe) « 280keV, whereas the
55
Mn atom is lighter than the
55
Fe atom:
M A ( 55 Fe) - M A ( 5 5 Mn) » 231 keV. 3. The /3-stability of Ionized Atoms Further, we discuss how the changes in electron shells, that is, changes whose energies are much smaller than nuclear binding energies, can cause modifications to the nuclear stability condition. To determine the relation between the charge Z and the mass A of a stable isotope, let us find the minimum of the atomic mass MA{Z) on the isobar. The atomic mass can be represented in the form: MA(A, Z) = d(A)
+ C2(A) (z ~ Zo) ~ S(A, Z) aP A~p,
(11)
where Z0
A «SYM + ac A " 1 / 3
2
+ TO
asYM + ac A2/3
C2(A) = ^ + a c A - ^ , d{A)
= A(mn - av) + as A2'z - Zl C2(A) + aSYM~.
(12)
Inasmuch as Z can only be integer, the minimum of M\(Z) is attained at an integer Z nearest to ZQ. When the ionization potential of an electron shell changes (due to, e.g., the effect of a strong magnetic field), the stability condition has a similar form, but involves the following replacement TO —> rh + 0(me). With 0(me) -C asYM = 94.8 MeV, the difference between these two conditions seems to be negligible. However, in the cases when Z0 is close to a half-integer value, the perturbation, even as small as me/asYM, can change the integer nearest to ZQ by unity. This means that it is the nucleus of the neighboring isotope that will become stable. Using the Thomas-Fermi model for the atom ionization potential: 12 i"(Z) ^ 20.8 Z 7 / 3 eV
(13)
and the formula for the ionization potential of hydrogen-like atoms (consisting of a nucleus and a single electron): 12 / l e ( Z ) = 13.6Z 2 eV,
(14)
we deduce that the difference between ionization potentials of the neighboring elements I(Z+1) - I{Z) oc Z4/3
(15)
812
increases slower than the ionization potential of the hydrogen-like atom and that basically for all atoms (Z > 7): I(Z + 1) - I{Z) < Ile(Z)
< Ile(Z
+ 1).
(16)
Hence, the energy of the /3~-decay of a fully ionized nucleus to a bound state of the electron equals: Q = Q0 + I(Z) - I{Z + 1) + Ile(Z
+ 1) > Q0,
(17)
where Qo is the decay energy of the nucleus in the neutral atom. This means that when the nucleus is fully ionized, the /3~-dec&y to the bound state always yields more energy that the /3~-decay of the neutral atom. The analysis of the database shows that some stable nuclei of neutral atoms 163
Dy,
193
Ir,
205
T1
become unstable with respect to the j3" -decay to a bound state when they are fully ionized. This effect has been observed experimentally.1 When the atom is completely ionized, the nuclear stability condition always shifts to larger Z. For nuclei emitting delayed neutrons this results, in particular, in the increase of the fraction of delayed neutrons, as the nuclei become more neutronredundant upon ionization. 4. A Phenomenological Model of Nuclear Transformation We have shown that the conditions can be created (e.g., by application of a strong magnetic field) when the distortion of electron shells would result in a significant increase in the probability of nuclear processes involving weak interactions. Therefore, we consider the question whether the isotopic composition currently observed in nature is final and equilibrium. The changes in the isotopic composition of elements toward 56 Fe, due to fission and fusion reactions accompanied by great energy changes is known to be energetically favorable. Below we show that within a small (on the nuclear scale) energetic interval, a plethora of states can exist which are populated in nature in a very uneven way. Since the nuclear states being considered basically have the same energies (to within the accuracy of measurements), one nuclear state can transmute to another in a resonant transition without emission of a significant amount of energy (in the nuclear scale), which is without radioactivity. In standard nuclear reactions, the final nuclei are usually produced in excited states as a result of collisions between high-energy nuclei. Because of that usual nuclear reactions feature radioactivity phenomena. We consider non-standard nuclear transitions between initial and final states, which have the same nuclear energies. It should be stressed that we only discuss the question whether low-energy transitions are allowed by conservation laws, leaving aside the mechanisms underlying such transitions.
813
Consider hypothetical collective nuclear transformation processes involving weak interactions, which satisfy the following equation:
( 18 )
Y, tX* -> Y. z-YJ + ke~ + kV* + Q> *
3
where JQand Y) are the nuclei with the atomic weight Ai and charge Zi, respectively, a special case of which are neutrons (A = 1, Z = 0); k is the number of the electrons involved in the reaction; /scan be positive (in (3~-decay), negative (in K-capture), or equal to zero (in the case of strong interactions alone). Let us assume that generically some of the Xi (or Yi) nuclei may be identical. Define a set Sft of nuclear ensembles {X;}, that is, an ensemble of nuclei is an element of 3?. Then transformation is a transition between two elements of the set 3?. The development of the phenomenological model for such transformation reduces then to the following: in the set 5R of the ensembles of nuclei, it is necessary to find the ensembles {Yi}, the energies of which are closest to those of the initial ensemble {Xi} provided that the baryon charge (the number of nucleons), the electric charge and the lepton charge are conserved. Recall that neutrinos take away part of the released energy Q. However, the energy scale in the case being considered is significantly smaller than in usual noncollective reactions involving weak interactions: in the hypothetical collective process, a neutrino may have any small momentum. The first attempt to develop such phenomenological model of nuclear transformations was made by Russian researchers in Dubna (Kuznetsov's group). 13 Each ensemble of nuclei {Xi} is described by a set of integers {a,} = a, where ai is the number of nuclei Xi in the ensemble; the unit vector ^corresponds to an ensemble comprising only one nucleus Xi. In the set 9ft we define a norm:
Nl
=^2aiAiqi, i
(19) where W is the binding energy of the nucleus and Z is its charge rh = mn—mp—me = 782.3 keV. Using the data on isotopes, one can see readily that q(X) > 0 for all known isotopes (including unstable ones), and the maximum of q(X) is attained for 56 Fe. The introduced norm has the following physical meaning: it equals the energy needed to separate the atom into hydrogen atoms, i.e. to separate the nucleus into the constituent protons and neutrons with the subsequent transformation of all neutrons into protons: X% -> Ai JH + (At - Zi) e~ + (At - Zt) Pe-Q,
Q
Si
814
Actually, the ensemble consisting of hydrogen atoms is used as the origin (zero norm). When comparing the binding energies W of two nuclei, 3 He and 3 H (tritium), we determine that the binding energy of the stable nucleus 3 He is lower than that of the unstable one 3 H. This apparent contradiction (larger binding energy is expected to correspond to a more stable nucleus) is resolved when the considered norm is used: In this formulation, the problem of modelling the transformation process is reduced to a search for ensembles {bi} = b, whose norm is close to the initial one {a,} = a, i.e.: b — \\a\\ < e, e being small. One can check easily that the transition from the ensemble a to the ensemble b corresponds to a transformation of type of the following form: J2 ai zlx* ~> J2 i
bi
zlXi
+ N H iH + fee" + kve + Q,
(20)
i
where Nn = Y^i (ai ~ bi) Ai is the number of produced (A% > 0) or absorbed (NH < 0) protons, k = ^ i (a* — bi) (Ai — Z{) is the number of produced (fc > 0) or absorbed (k < 0) electrons, and Q = J2t (bi — a*) Ai qi is the produced (Q > 0) or absorbed (Q < 0) energy. The use of the proposed norm makes it possible to significantly simplify the task of selecting the nuclear ensembles, as actually, when selecting b, it is not necessary to check that the electric and baryon charge conservation laws are observed as these conservation laws are always observed owing to the specified conditions. The search for the nearest ensembles is reduced to an algebraic problem. Note that if one assumes that the binding energies and hence norms Qi = 5\ and Q2 = $2 of two nuclei X\ and X2 are exactly known and can be expressed as rational numbers, then the ratio Q1/Q2 can be expressed as a ratio of two integers N2/Ni. One can check easily that in this case two ensembles Ni Xi and N2X2 have equal energies. This implies that the transition Ni X\ —> N2 X2 + . . . can occur without changes in energy. However, the coefficients obtained in this case (the number of particles in each ensemble) can be so large that such a transformation will be of no practical interest. The quoted example only illustrates the theoretical possibility to find ensembles, which have very close energy values. In practice, the numerical selection of the ensembles is restricted by the accuracy to which the nuclear binding energy is measured (AQ ~ 1 keV). Taking into account huge nuclear binding energies, the discrete nature and the finite size of Mendeleev's table, it is not a priori obvious that it is possible to find different nuclear ensembles with the same number of nucleons and with nuclear energies differing by values of the order of the electron chemical binding energy. However, this is what we have succeeded in doing. When developing the transformation model, the initial nuclear ensemble is divided into groups called "clusters," and the search for ensembles with the nearest energy values is carried out separately for each cluster. The calculation model con-
815
tains a number of parameters: the range of considered energy changes in the cluster, the cluster's size, and the number of the nucleons transferred between the cluster's nuclei. The number of ways in which an initial cluster containing N nucleons can be "reshuffled" is ~ 2 W . Thus, it is so large that it is impossible to consider all configurations. It seems to be reasonable to assume that the number of nucleons in a cluster is limited by the closest geometrical neighbors, that is, it is not over 20. This approach makes it possible to significantly reduce the number of combinations involved in processing. The final calculation result is obtained by averaging all possible simplest transformations in clusters taking into account the statistical weight of each cluster in accordance with the initial distribution of nuclei. The final nuclear distribution shows what nuclei have appeared and what disappeared in the process of transformation. Note that the minimum number of cluster nuclei, for which a non-trivial solution can be found, equals to three. In order to determine the parameters of the phenomenological model that correspond to experimental data, we have modelled the transformation of titanium foil in water and glycerol in an argon atmosphere. In this case, the ensembles with the minimum energy differences |Q| < 1 keV (with energy changes smaller than the accuracy of the binding energy measurement) were as follows: 2 -f2 Ti + 4 -\ H -> 4 •* He + f9K + ^ T i + e + o(l keV), 23V + | | T i + l80 -+
5 7 2 6Fe
+ ??Na + HCl + e + o(l keV),
$ T i + 2 -ft Ar + leO -+ *5N + ??C1 + ?|Ar + igCr + o(l keV), 2 41 Ti + 2 i°s Ar + l2C -+ | 6 0 + ?|S + $ C a + 2 •« Sc + o(l keV), 5 -\6 O + 2 -l2 C + e -> J?Na + 2 •{ H + 2 -f N +
20
0Ne
+ f|Si + o(l keV),
6 -23 V + 3 -l3 C + 22Ti + 2°Ti - • ^ F e + 3 -f N + ^ C a + 6 -f2 Ti - e + o(l keV), 8 H Ti + 3 -| 6 O + 6 • e - • ^Be + \aO + 4 -f2 Ti + 2 -52°2 Ti + | | C r + f^Fe + o(l keV), l l - ^ T i + 2 - | 6 0 + 4 - e ->• ^He+ ^ 2 C+ f ? C l + 7 - ^ T i + f4Cx+ ^ M n + ^ F e + o ( l keV). Note that the nuclear energies of the left-hand side and right-hand side nuclear ensembles are the same (to within the accuracy to which the binding energy is measured). This means that the energy changes in such nuclear transformations are of the order of chemical energies. It should be stressed that when solving such a problem, a large number of combinations (10 5 -10 6 ) is processed, and the examples quoted above are nothing but illustrations. It would be incorrect to consider the quoted combinations as nuclear reactions where a large number of nuclei collide. These examples describe
816
transitions between states of nuclei, the mechanism of such transition being obscure as yet. One can only assume that some transition (possibly a resonant one) occurs due to effects of a new interaction. We have shown that there are nuclear ensembles consisting of stable nuclei, which have identical electric and baryon charges and the energy values that are very close to each other. Hence, transitions between such ensembles do not violate the known conservation laws and are not accompanied by radioactive emission of energy. We do not consider the transformation mechanisms, but note that in the resonance conditions, the probability of penetrating through a potential barrier does not depend on its height or width. This model needs detailed investigation by comparing experimental results with the results of modelling for different parameters. Such studies are currently in progress, but first it was necessary to find a qualitative effect predicted by the model, which could be checked experimentally. The numerical simulation of combinations, we have carried out, shows that when a sufficient amount of vanadium is transformed, the isotopic composition of iron should be distorted and shifted toward an increase in the 57 Fe isotope content. This feature is specific to vanadium and the result does not depend on the calculation parameters: the quantitative ratio of iron isotopes changed, but the amount of 57 Fe was always significantly larger than that in the natural mixture of iron isotopes. The proposed phenomenological model cannot make quantitative predictions for the content of 57 Fe. However, it predicts qualitatively an increase in the 57 Fe content as compared to that in the natural mixture of isotopes (2.2%), due to the transformation of V. The experiment, in which titanium foil was exploded using the electric charge in solutions of vanadium salts (VCI3 and NH4VO3), has shown that the content of 57 Fe in Fe shifts to larger values (to 3.7 ± 0.5%). We have shown that even without developing a specific model for low-energy nuclear transformation but using conservation laws alone, one can find examples of nuclear ensembles that differ only by chemical scale energies.
5. Conclusions (1) The only valid condition of /^-stability of a nucleus is the minimum value of the mass of the atom on the isobar. (2) The condition of nuclear stability and the decay schemes of unstable nuclei depend on the state of the electron shells. Atom ionization and other perturbations in electron shells (caused for example by magnetic field) • not only change the decay periods of unstable nuclei, • but also alter decay schemes • and modify the stability condition. (3) We have developed a phenomenological model for the low-energy nuclear transmutation.
817
References 1. M. Jung, F. Bosch, K. Beckert, et al, Phys. Rev. Lett. 69, 2164 (1992). 2. F. Bosch, et al. Phys. Rev. Lett. 77, 5190 (1996). 3. A.A. Rukhadze, L.I. Urutskoev, and D.V. Filippov, Bull. Lebedev Phys. Inst. # 1 (2004). 4. E. Fermi, Nuclear Physics (Chicago, 1950) [Translated into Russian (Moscow: IL, 1951)]. 5. J.M. Blatt and V.F. Weisskopf, Theoretical Nuclear Physics (New York: Wiley, 1952) [Translated into Russian (Moscow: IL, 1954)]. 6. G. Audi, A.H. Wapstra, Nuci. Phys. A 595, 409 (1995). 7. A. Bohr and B.R. Mottelson, Nuclear Structure, Vol. 1 (New York: Benjamin, 1969) [Translated into Russian (Moscow: Mir, 1971), p. 200]. 8. V.E. Kuz'michev, Zakony i Formuly Fiziki (Physics Laws and Formulas) (Kiev: Naukova Dumka, 1989), p. 645. 9. S. Glasstone, Sourcebook of Atomic Energy (New York: D. Van Nostrand Company, 1958) [Translated into Russian (Moscow: IL, 1961), p. 391]. 10. D.V. Sivukhin, Obshchii Kurs Fiziki T. 5 Atomnaya i Yadernaya Fizika (General Course of Physics. Vol. 5. Atomic and Nuclear Physics) (Moscow: Fizmatlit, 2002), p. 468. 11. K.N. Mukhin, Eksperimentalnaya Yadernaya Fizika (Experimental Nuclear Physics), Vol. 1 (Moscow: Atomizdat, 1974). 12. L.D. Landau and E.M. Lifshitz, Kvantovaya Mekhanika. Nerelyativists kaya Teoriya (Quantum Mechanics. Nonrelativistic Theory) (Moscow: Fizmatlit, 2001), p. 315. 13. V.D. Kunznetsov, G.V. Mishinsky, F.M. Penkov, et al., Ann. Fond. L de Broglie. 28, 173 (2003).
SEARCH FOR ERZION N U C L E A R CATALYSIS CHAINS FROM COSMIC R A Y ERZIONS S T O P P I N G I N O R G A N I C SCINTILLATOR
Yu. N. BAZHUTOV Institute of Terrestrial Magnetism, Ionosphere and Radiowave Propagation (RAS), 14-2092 Troitsk, Moscow Region, Russia E-mail: [email protected] E. V. PLETNIKOV State Technical University (MAI), Moscow, Russia In framework of Erzion model, charged cosmic ray Erzion intercepted in an organic substance should create Erzion nuclear catalysis chains with frequency of ~10-100MHz during ~10-100mks. If as an organic substance we use a plastic scintillator, we can observe a long and flat (10-100 mks) pulse of large amplitude (~100MeV). No elementary particle can imitate such pulses. It is expected that such pulses in a plastic scintillator with mass of 100 kg should appear at sea level every month, on average. Such pulses can be observed every day on the Spectrometric Scintillation Super-Telescope (SSTIS) in IZMIRAN for cosmic rays monitoring. In the framework of Erzion model 1 - 3 the following Erzion nuclear catalytic reactions may be run in condensed matter consisting of light stable isotopes: H1{3~,3°)n+
1.65MeV (100%)
(1)
H 2 ( 9 - , 3 N ) n +5.6MeV (0.016%)
(2)
H 2 ( 9 N , 9 ° ) H 3 + 0.1 MeV (0.016%)
(3)
H 2 (3°, B N J H 1 + 3.9 MeV (0.016%)
(4)
Li 6 (9 N ,9°)Li 7 + l.lMeV(7.5%)
(5)
Li 6 (3°,9 N )Li 5 + 0.48MeV (7.5%),
Li5 - • He 4 + H 1 + 1.7MeV
(6)
L i 6 ( 9 - , 9 N ) H e 5 + 3.2MeV(7.5%),
He 5 -> He 4 + n + 1.36MeV
(7)
Li 7 (9 N , 9~)Be 8 + 9.5 MeV (92.5%)Be8 -> 2 x He 4 + 4.8 MeV
(8)
C13(9N3°)C14+2.0MeV(l.l%)
(9)
818
819
C 1 3 (9°, 9 N )C 1 2 + 1.2MeV (1.1%)
(10)
C 1 4 ( 3 N , 9 " ) N 1 5 +2.4MeV (—)
(11)
N 1 4 ( 3 - , 9°)C 1 4 + 2.3 MeV (99.6%)
(12)
N 1 4 ( 3 ~ , 3N)C13 + 0.25MeV (99.6%)
(13)
N 1 4 ( 3 N , 9°)N 15 + 4.7MeV (99.6%)
(14)
N 1 5 ( 9 N , 9 - ) 0 1 6 + 4 . 3 M e V (0.37%)
(15)
0 1 7 ( 9 N , 9 ° ) 0 1 8 + 1.9MeV (0.038%)
(16)
0 1 7 ( 9 ° , 9 N ) 0 1 6 + 2.0 MeV (0.038%)
(17)
0 1 8 ( 9 N , 9 " ) F 1 9 + 0.2MeV (0.2%)
(18)
100
w
Figure 1.
50
Long and flat pulses shape, caused by Erzion catalysis chain in plastic scintillator.
If cosmic ray Erzion is stopped in organic substance (consisted of such chemical elements, as: H, C, N, and O), it begins to create Erzion nuclear catalysis chains [reactions (3, 4), (9, 10), and (16, 17)] with frequency of ^10-100 MHz in condensed matter during ~10-100mks. Then it is captured on "donor" isotopes (C 12 and O 16 ), or it goes out from this substance. If instead of an organic substance we use a plastic scintillator, we can observe long and flat (10-100 mks) pulses of large amplitude (~100MeV) (see Fig. 1). No elementary particle can imitate such pulses. It is expected that such pulses in plastic scintillator with mass of 100 kg must appear
820
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Figure 2.
View on "Doch-4m" installation in Kurchatov Institute.
at the sea level every month \{M x T ) ~ 3000 kg/day]. Few nuclear scientists have attempted such experimental techniques, and are in a position to observe such pulses. Very similar pulses were observed in MSU group. 4 The authors cannot explain their nature, but they suppose it may be a manifestation of extensive air
Bwa c6oKy Ha ycramiBKy CCTHC
B n a e a e p x y Ha ycTaHOBHy CCTHC
Figure 3.
View on new SSTIS installation in IZMIRAN.
821
showers. Fortunately, we have used such experimental technique of pulses shape observation in scintillator. Already, the Doch-4m installation at the Kurchatov Institute has been working for three years monitoring cosmic rays to search for Erzions. In this installation, the pulses shape of inorganic scintillations N a l & Csl is investigated. In the same Doch-4m installation we have a plastic organic scintillator ( ~ 3 0 k g ) used for anticoincidence purposes (see Fig. 2). To investigate the pulses shape in organic scintillator we changed master state of installation Doch-4m, and it worked for about m o n t h in this state. We received experimental exposition ( M x T) ~ 1000 kg/day, and we have examined about half the data, but until now we have not found the expected pulse shape. Soon, a very large new installation (SSTIS) (plastic scintillator with M ~ 800 kg, see Fig. 3) will operate in IZMIRAN. Such pulses can be observed almost every day on the Spectrometric Scintillation SuperTelescope (SSTIS) creating in IZMIRAN for cosmic rays monitoring and Erzion search.
References 1. Yu. N. Bazhutov and G. M. Vereshkov, New Stable Hadrons in Cosmic Rays, their Theoretical Interpretation & Possible Role in Catalysis of Cold Nuclear Fusion. Preprint No. 1, Central Research Institute of Machine Building, 1990. 2. Yu. N. Bazhutov, G. M. Vereshkov, and V. I. Kuksa, On a possibility of existing new stable hadrons-hypothetical catalyst of cold nuclear transmutation, in Proceeding of the 3rd Russian Conference On Cold Fusion & Nuclear Transmutation (Moscow, 1996), p. 157. 3. Yu. N. Bazhutov and G. M. Vereshkov, in Proceedings of the ICCF-4, Vol. 4 (Hawaii, 1993), pp. 8-1. 4. V. B. Atrashkevich, Yu. A. Fomin, G. K. Garipov, et ah, Temporal structure of scintillation detector pulse in EAS. J. Phys. G: Nucl. Part. Phys. 23, 237-247 (1997).
LOW-ENERGY NUCLEAR REACTIONS RESULTING AS P I C O M E T E R I N T E R A C T I O N S W I T H SIMILARITY TO K-SHELL ELECTRON CAPTURE
H. HORA University
of New South
Wales, Sydney
2052,
Australia
G. H. M I L E Y Fusion
Studies
Laboratory,
University
of Illinois,
Urbana, IL 61801,
USA
X. Z. LI Physics
Department,
Tsinghua
University,
Beijing
100084,
China
J. C. K E L L Y School of Physics,
Sydney
University,
Sydney
2006,
Australia
F. OSMAN University
of Western
Sydney,
Penrith-South,
NSW
1791,
Australia
Since the appeal by Brian Josephson at the meeting of the Nobel Laureates July 2004, it seems to be indicated to summarize the following serious, reproducible and confirmed observations on reactions of protons or deuterons incorporated in host metals such as palladium. Some reflections to Rutherford's discovery of nuclear physics, the Cockroft-Oliphant discovery of anomalous low-energy fusion reactions and the chemist Halm's discovery of fission had to be included. Using gaseous atmosphere or discharges between palladium targets, rather significant results were seen e.g. from the "life after death" heat production of such high values per host atom that only nuclear reactions can be involved. This supports the earlier evaluation of neutron generation in fully reversible experiments with gas discharges hinting that a reasonable screening effect - preferably in the swimming electron layer - may lead to reactions at nuclear distances d of picometers with reaction probability times U of about megaseconds similar to the K-shell capture radioactivity. Further electrolytic experiments led to low-energy nuclear reactions (LENR) where the involvement of pollution could be excluded from the appearance of very seldom rare earth elements. A basically new theory for DD cross-sections is used to confirm the picometer-megasecond reactions of cold fusion. Other theoretical aspects are given from measured heavy element distributions similar to the standard abundance distribution, SAD, in the Universe with consequences on endothermic heavy nuclei generation, magic numbers and to quark-gluon plasmas.
822
823
1. Prelude and Introduction The public opinion and the view of the media is still uncertain about the physics phenomenon of cold fusion or the low-energy nuclear reactions (LENR), which may occur by high concentration of protons or deuterons in host metals as palladium, nickel and others. There should be no doubt in physics in clarifying truth and only one truth, and even if non-physicists have different tools or views to address these questions, a strange situation has developed since 1989. For physicists, a list for clearly formulated questions has been presented by Brian Josephson 1 from which position at least a starting point for clarification should be possible. The problem may be that the phenomena were brought forward to physics by non-physicists. In this situation, it may be permitted to recapitulate what happened in similar cases before. When Becquerel discovered 1896 that the pitchblende from St. Joachimstal in Bohemia and other minerals containing uranium are emitting certain radiation blackening photographic plates, a wide range of people were speculating about this phenomenon. There were even papers explaining that some ghosts are involved. Ernest Rutherford after his undergraduate studies in New Zealand produced splendid results with his PhD in Cambridge where he before 1900 contributed to Marconi's detection of electromagnetic radiation by discovering very ingeniously the "radiomagnetic detectors". After becoming a professor at the McGill University in Montreal, he discovered that pitchblende emitted helium as demonstrated spectroscopically and found that another emission were energetic electrons, which were just recognized at this time. With this discovery of alphabeta- and gamma-radiation he became the founder of nuclear physics but his faculty was going to dismiss him because he was working in a field related to ghosts. He was saved in last minute by the offer of a professorship in England. After Rutherford discovered that the atoms are empty and there was only a very tiny nucleus in the center and that these nuclei could interact with others if they were bombarded with particles of several million electron volt energy to overcome the Coulomb repulsion, MeV accelerators were built and a broad field of nuclear reactions was studied. It was then the idea by Cockroft2 that he used his multi-MeV accelerator to bombard light nuclei with light nuclei at energies 50 times lower against all expectations and opinions how to overcome the Coulomb repulsion. And there were reactions e.g. of protons with 1 1 B. At this stage, Mark Oliphant who had come from South Australia for his PhD to Rutherford in Cambridge, used his very powerful 100 kV gas discharges for these nuclear bombardments and received the precise energy for the p-B(ll) reaction. 3 Then he tried to use the not long before discovered heavy hydrogen deuterium D instead of the protons in his discharge4 - produced by methods brought over by Paul Harteck from Germany - and found reactions with traces in the cloud chamber where even the grand master of this field, Lord Rutherford could not find an answer for several days. But then it was clear: the D-D reaction even working at 10 keV and less was producing the then not known superheavy hydrogen isotope tritium T and the very rare 3 He isotope with several branches of reactions unknown before.
824
This first nuclear fusion reaction in 1933/1934 is now a wide field for energy research. When few years before the deuterium was available in Berlin, Paneth tried to see what happens when this heavy hydrogen was used in the long known phenomenon of very high concentration (even above 1:1) absorbed in palladium at room temperature, it seemed that helium was emitted 2 - a strange analogy to the pitchblende. Physicist were sceptical and Paneth had to withdraw. 6 The incorporation of hydrogen or of its isotopes in palladium was indeed remarkable and this was used for transporting of protons or its isotopes through palladium layers which had to contain a small percentage of silver in vacuum techniques. The strong decrease of radioactivity when loading tritium T in Ti was noticed also in such a prestigious laboratory as that of Philips in Eindhoven 7 and neutron emission was reported from palladium compounds. 8 End of 1989 it was reported from the BARC (Bhabha Atomic Research Laboratory) where the Indians developed their nuclear weapons, that when moving D-Pd, tritium was appearing on the rare side as measured with their necessarily very sensible tritium detectors. M. Srinivasan reported that there were samples of Pd containing D stored for 15 years, which then showed tritium in dangerous quantities, which definitely had not been incorporated 15 years before. When Gopal Ayengar, Director of BARC, reported this to the top researchers at the Kurchatov institute in Moscow, they responded with icy tacite only. As a reaction to the reports on anomalous heat production from D loaded Pd April 1989 at the University of Utah 9 and neutron emission,10 the Kurtchatov institute like many other places liked to reproduce the reported anomalies but without success. S. Pismeny (Director of the Troitsk branch of the Kurtchatov Institute) mentioned that the money given to Fleischmann 9 was used mostly to rebuilt a large number of the initial electrolytic cells which could not demonstrate more than what was questionable in the beginning. Dozens of Million dollars were spent from Japan for research in a private laboratory in France and in a government laboratory in Sapporo. The latter one bought a large number of these electrolytic cells from France where its was claimed that these produced heat. When in Sapporo, no heat appeared even after Pons was there for several weeks working with the cells as M. Okamoto reported. Even physicists have examples where such failure in reproducing claimed observations do happen, before the complexity of a new situation in physics is clarified. The more sceptical are physicists when chemists or others are claiming anomalies in physics. Such a problem was between the chemist Otto Hahn and the radiation physicist Lise Meitner, a most prominent team e.g. with the discovery of the new element protactinium in 1918 where they - against the rules - did not receive the Nobel prize. Physicists expected the production of heavier nuclei when bombarding uranium with neutrons into which direction Meitner was looking when she left Berlin mid 1938 under unfavourable circumstances to Stockholm. Meitner meeting Hahn November 193811 still "objected to the most recent findings" of Hahn who then again with his world best techniques of chemical micro-analysis confirmed that
825
elements of middle weight were produced, proving that the neutrons were splitting the uranium nucleus. These results were reproduced very quickly in comparably easy experiments and the enormous consequences are known. In support of the arguments of Josephson 1 we are trying to report on reproducible results which physicists may consider worthwhile to re-examine. We are aware that the last 15 years produced more than 95% publications which cannot be accepted by physicists beginning with the theory that gravitation waves form far out galaxies cause cold fusion, not to talk about the ghosts with the Becquerel radiation. Since every cold-fusionist likes to get his own credit, nearly nobody is taking the work of colleagues serious or carefully reproduces the other's work. It is really the responsibility and duty of funding agencies like DOE or others to financially attract most carefully selected teams to reproduce the one or the other serious result as the very first step. Only after this clarifying progress on experiments, one may talk about any theory or model. 14 Nevertheless - indeed with all reservations - we are discussing some theoretical aspects in the following. Using the first complete theory about hot fusion cross sections 12 ' 13 based on a complex Schrodinger potential, we show direct agreement with the results of the picometer-megasecond nuclear reaction model which was concluded earlier from experimental results.
2. Experimental Facts Most of the reported observations of heat generation or radiation emission from deuterium loaded palladium are occurring not regularly, are pulsating statistically and not reproducible. This was summarized by Yamaguchi et al.15 and distinguished from the few reproducible observations of neutron and gamma emission where the palladium was in a gaseous environment and where gas discharges were used and complications with electrolytic procedures were avoided. One of the reproducible results were that by Prelas et al.16 In this case, it was noted that the standard cleaning of the palladium surface by an argon pre-discharge was essential and the interaction with air stopped the neutron emission indicating that the surface conditions of the palladium are important. The generation of heat was indeed in the focus of interest. Experiments were performed in gaseous atmosphere at different pressures and temperatures placing Pd wires in deuterium gas 17 but observing also effects if not deuterium but light hydrogen is loaded into the palladium. 18 Long time repeated experiments with Pd wires in hydrogen atmosphere showed "heat after death": heat was generated after the gas loading discharge had been stopped and the gas was evacuated. For the following 43 h, the wires produced 3.6 kW/cm 3 heat or 13 keV per palladium atom. Such energy cannot be produced by chemical processes. Since any heat generating process will not be due to every average Pd atom but to specific ones only, reactions with the well-known MeV can be concluded as expected from nuclear reactions. This experiment 18 was repeated at different places and witnessed by experts from the MIT.
826
If such nuclear reactions occure - even if without emission of alphas, betas, neutrons or not resulting in radioactive reaction products - the MeV recoil of daughter nuclei should produce X-rays in the few keV range and the MeV daughter nuclei should appear as traces in CR39 foils. Both has been detected, 19 the in situ Xrays and the charged particles using the evaluation of the CR39 foils at the Dubna Nuclear Research Center. Before it was shown20 that the CR39 traces differ considerably from that of alpha traces, being larger due to the larger MeV nuclear reaction products. A proof that the produced new elements after reaction of hydrogen or deuterium in Pd are not contamination from walls, etc., can be seen from the fact, that rarest of rare earths nuclei were generated, e.g. terbium 21 as detected uniquely from the K-shell X-ray spectrum. There are many more experimental results, which however, need more careful repetition or more accurate measurement before convincing arguments can be established. In the following sections some results are compared with some modelling or consistency proofs as examples how further research may be directed. 3. Modelling Nuclear Interactions at Picometer Distance Although the DD reaction in palladium is not fully explored experimentally by not fully clarified weighting of branches leading to tritium, neutron production and directly to 4 He, the reproducible results of the continuous generation of neutrons (in contrast to stochastic bursts 15 ) as measured from Pd when loaded with deuterium in gas discharges16 were used for estimations for fusion reactions. The details of the measurements with argon discharge cleaning of the Pd surface, stopping of neutron production when air was let into the reaction chamber and re-establishing of the reaction after argon discharge and deuterium loading discharges in a fully reproducible way, gave confidence to assume transparent physics conditions. 16 The starting point 22 was the mentioned large distance anomaly of the reaction of light nuclei as discovered as an unexpected phenomenon by Cockroft2 and further clarified by Oliphant et al.3 leading to the discovery of the very anomalous DD and DT hot fusion reactions 4 with their more than 1000 times larger cross sections than the usual nuclear reactions having mbarn cross sections. The fusion reactions appeared at central collision distance d with energies E: d = e2/E = 1.43 x 10~15/E
(cm) (E in eV)
(1)
at E of 10 keV or even much less. The distance d is then 143 fm or larger. This is about 100 times larger than the diameter of the deuterons! Expecting that these hot fusion reactions happen within the usual 10~ 20 s, and taking the well-known reaction time U for muonic fusion,23 and furthermore, taking the estimated reaction time U for deuterons in a heavy hydrogen molecule,24 a plot of Fig. 1 resulted in a relation 22 U = 8.139 x 10 4 d 3 4 8 (s) (dgiven in picometer, pm).
(2)
827
/ Fusion in hydrogen molecule2'
10,70 c o o to
10:50
c o 'to 3
10',30
to
10 10
10°
_
LENR
E 10-io
Hot fusion
10
-30
10-1
10°
101
10 2
103
Distance between D-D (pm)
Figure 1. Measured reaction times U and nuclear distance d in picometers. Points from the left: hot fusion, myonic catalysed fusion and calculated fusion of DD in a D2 moleule. 22
The protons or deuterons in the palladium are assumed to be in a state of a Maxwellian gas with a screening S reducing the Coulomb repulsion as for central collisions to distances d of d=(l/S)e2/E
(3)
the question is still open whether such a strong screening is within the bulk of the Pd or only near the surface due to the well-known swimming electron layer.25 For the interior of high temperature plasma, screenings of S — 5 are well known26 and for solid Pd higher values in the interior or especially near the electron layer at the surface may well be possible. When evaluating the reproducible continuos neutron emission from the surface of D loaded Pd, 16 a screening S = 14 was estimated. 22 The reaction distance of the deuterons is then in the pm range and rather smaller than that of central collision of about 3 pm. Following Eq. (2) and Fig. 1, the reactions are then occurring in the range of picometers and with reaction times U of about megaseconds. It should be noted that these times are similar to the measured half life of radioactivity at K-shell electron capture where the Bohr radius is in the similar range of pm.
828
I 0.11
4. CO
c g o a
0.01 1 + ENDFdata
• CO CO
o o c o
-
;
Selective resonant tunneling
4
1E-3-:
to
D LL
•
+ T3
1E-4-g
,4s
\
^ + 1E-5- I
10
,
r—- T — " !
1—ITT\
'
1
1
1
100
1—|"-|-'fT"[
'
1000
Deuteron energy (Lab.) keV Figure 2. section. 1
Comparison between experimental and theoretical calculation for d + d fusion cross-
The picometer reaction distance is in some agreement also with other models 22 for cold fusion. It should be noted that the Debye length for the protons or deuterons at 1:1 loading in Pd at room temperature is 4.8 pm what may permit the assumption that these ions are moving around within the Pd nuclei and their electron clouds like neutral particles whose electric charge is cut off a these pm distances permitting the nuclear reactions with any heavy nuclei within the long times of orders of magnitudes of megaseconds. 4. Comparison with N e w Cross-Section Calculations The agreement with the measured neutron emission16 and the screening for picometer DD reactions was possible only for the energetic tail of the Maxwellian distribution of the deuterons in the Pd host metal. It was necessary that the deuterons had to have at least an energy of about 2.4 eV for the reaction. The screening 5" = 14 corresponded then to protons in unscreened low-density high temperature plasma of 470 eV where even for DD a certain very low reaction probability can be expected.
829
We compare this now with the new theory for the fusion cross sections using a complex Schrodinger potential for light nuclei. All other models for cross sections were numerical fitting of experimental values, e.g. with five constants. 2 7 The new theory uses only the two reasonable parameters of physics, the resonance energy and the width of the resonance distribution. T h e model uses a square well nuclear potential and calculates the selective resonant tunnelling. T h e imaginary p a r t of the potential accounts for the absorption insided the nuclear well. This optical nuclear model was used before for heavy nuclei only. T h e resonant tunnelling is usually treated as a tow-step process with decay independent tunnelling b u t this is not true in the case of light nuclear fusion. T h e wave function will reflect back and forth inside the nuclear well. T h e surprisingly good agreement between the theoretical calculation of fusion cross sections with experimental d a t a implies t h a t the compound nucleus model might not be applicable for the light-nuclei sub-barrier fusion. Instead the selective resonant tunnelling model is used. This provides a new approach toward nuclear fusion energy with no strong nuclear radiation for the sub-barrier fusion nuclear physics. T h e good agreement between cross D D fusion section measurements and t h e t h e o r y 1 2 ' 1 3 is shown in Fig. 2. Any measurement of a DD fusion cross section for 470 eV is far beyond the present experimental possibilities. We refer e.g. to the only theoretically concluded p - p weak force cross section which was not yet experimentally confirmed but its estimation fully explains 2 8 why the burning of protons at about 15 mK in the centre of all the 10 2 2 stars in the Universe takes few billion years. T h e theory 1 3 for D T at 470 eV results in a fusion cross section of a = 3.6761 x 10~ 2 6 barn,
(4)
which value is few orders of magnitude smaller t h a n the estimated p - p weak interaction cross section near 1.5 keV. From the theory we can then conclude t h a t the fusion reaction time of U = 10 5 s for the p m distance DD reactions is comparable to the concluded 10 2 5 times longer reaction time of the hot fusion DD reactions in fair agreement with the conclusion of the preceding section and of Ref. 22. 5. C o n s i s t e n c y V i e w s In this section is comparing some experimental results of nuclear transmutations, fission and combined nuclear reactions induced by protons incorporated mostly in palladium and nickel multi-layers as L E N R . We underline t h a t these consideration may be taken as consistency proofs only and may support the existence of cold fusion and L E N R only in a wider view t h a n a direct proof would need. Following the creation of a large range of elements during several weeks of interaction in a fully reproducible way with 18 runs in electrolytic experiments, 2 9 ' 3 0 there appeared a distribution of endothermic (nucleon number A = 60 lager t h a n iron) generation of nuclei with maxima close to the magic numbers (see Fig. 3). These production rates were given from the evaluation of secondary ion mass
830 10' 10 1
t
I
-*
———l
i
r _
JSb-Si OJ
| 10 16 o <. — o> -|o 15 ~
-
Al O
/cu\
s< CI
c
4 \
™
AccT\,
JoFe I
f 1014
.V
"
se °Co
S
k§L< J7 r
LTe
10 r — 101:
""\
Au
S I T " * - —
P&\ i
r .
I 20
40
60
80
100
Atomic number (Z)
Figure 3. Elements produced in palladium at very high concentrations of protons within several weeks of interactions by LENR. 2 9
spectrometry (SIMS) measurements of the element distribution in the Pd-Ni layers before the electrolytic treatment (Fig. 4) and after the treatment (Fig. 5). Despite an accurate analysis that the observed additional elements in the layers are not due to contamination from the electrolytic cell, the scepticism against all
1.E + 00
100 Mass (amu) Figure 4.
Element distribution from SIMS for Ni-Pd layers before reactions. 2 9
831
1.E + 00 100 Mass (amu) Figure 5.
SIMS mass spectrum after reactions. 2 9
these kind of experiments is still there despite the reproducible results from 18 runs. We mentioned before the fact that rarest of rare elements (terbium) were uniquely measured 21 in other experiments which definitely could not come from pollution. The question was discussed30 why these transmutation are not showing neutron, alpha or gamma emission and why not radioactive nuclei are produced via compound nuclear reactions for achieving the endothermic generation of heavy nuclei. The reason is that these reactions are slowly and there is time to find the most energetic branches in the compound reactions resulting in stable products different to the fast fission of heavy nuclei where one of the two daughter nuclei is radioactive. The fact that MeV energies of daughter nuclei are produced was seen from the larger than alpha traces in CR39 19 ' 20 and the emitted X-rays in the keV range correspond to the bremsstrahlung of the daughter nuclei.20 As proof in support of the reality of the LENR results, we show in this section how the results of Fig. 3 are consistent with general knowledge from other fields in physics.
5.1. Endothermic
Production
of Nuclei and Magic
Numbers
Drawing a line through the maxima of the measure element distribution depending on the nuclear charge Z in Fig. 3, we find a Boltzmann-like probability distribution for the production rate N(Z)
N{Z)=N'exp(-Z/Z'),
(5)
832
where the best fit is with the decrement Z' = 10. This agrees with the element distribution in the Universe, Fig. 6, again with using the plot for the proton number Z in the nuclei based on the same Z' = 10. The problem of the endothermic production of nuclei with Z above 26 (iron) is one of the unsolved important problems in astrophysics. 31 ' 32 It should be noted that the distribution (5) only with Z' = 10 fits an interesting relation for the magic numbers of nuclei. We discuss here what consequences it has due to the fact that the drawn curve in Fig. 3 - fitting with the empirical astrophysical observations of the SAD - results in a Z' = 10 in Eq. (5) or values nearby. This is now related to the nuclear shell model where we derive an alternative foundation of the magic numbers compared to the usual explanation by spin and spin-orbit properties of nuclei. The magic numbers of the nuclear shell model are the sequence magic numbers : Mx 6 2, 8, 20, 28, 50, 82, 126
(6)
for protons Z in nuclides as well as for neutrons N = A - Z with the measured well known maxima of binding energies. We now calculate the ratios R(n) for the astrophysical 30 SAD-Boltzmann probabilities from Eq. (5) R(n) = [N(Zn + l)/N(Zn)]
- 1 = exp[(Z n + 1 - Zn)/Z%
(7)
where the magic numbers Zn of the protons are taken with the following indices n (0,1,2,3,...) ZQ = 2, Z2 = 28,
Z\ = 8,
Z3 = 50,
Z2 = 20
Z4 = 82,
for relation up to the magic number 20, Z5 = 126
(8)
for the magic numbers above 20. (9)
As seen from Table 1 for Z = 10 in Eq. (5), the ratios R, Eq. (7) results in values very close to R(n) = 3" (10)
(10)
shown in Fig. 7. The good fit with Z' = 10 compared with other numbers can be seen for the magic number 81 at n = 4. Instead of R — 81.45 (being very close to 3 4 for Z1 = 10) we find R = 224.69 for Z' = 8; R = 132.80 for Z' = 9, R = 54.598 for Z' = 11. Extending the procedure with the 3"-law (10) to higher magic numbers - see the extension of the fully drawn line by the dashed line in Fig. 7 (Ref. 37) - one arrives at the following higher magic numbers indicated by open circles as closest values to the line. The result is that for n = 6 one arrives at a magic number 180, for n= 7 at 246 and for n = 8 at 324: new magic numbers : 180, 246, 324
(11)
shown by circles in Fig. 7. This can be compared with the earlier predicted magic numbers 33 114, 184 and 228 (crosses in Fig. 7), which by far do not fit so well the relation (10).
833 100o
0.001
60
80
100
120
140
160
180
200
220
240
Mass number (A) Figure 6. Measured standard abundance distribution of the elements (SAD) 3 0 in the Universe where the line follows the exponential Boltzmann dependence of Eq. (5) with Z' = 10.
Table 1. Sequence n = 0, 1, 2 , . . . of magic numbers with the values exp(Zn/Z') and R(n) = e x p [ ( Z n + i -Zn)/Z'\ of Eq. (7) with Z1 = 10 from Eq. (5) as measured. N 0 1 2 (as n + 1 in (8)) 2 (as n in (8)) 3 4 5
Magic number 2 8 20 28 50 82 126
exp(Z/Z') 1.221 2.2225 7.389 12.1824 148.413 3640.95 296558.5
R(n) 1.822 3.321
3" 1 3
-
-
9.025 24.53 81.45
9 27 81
The first conclusion of these results derived from this fitting of the Boltzmann probability (5) with the standard abundance distribution of the heavier elements observed in the Universe, Fig. 6, refers to the curious jumping procedure with the magic numbers 20 and 28 in Table 1. This is exactly what was necessary to be explained when the magic numbers were discovered numerologically by Bagge. 34 ' 35 In order to explain the maximum binding energy of some nuclei, which cannot be explained so easily as, e.g. the electron shells in atoms from the Schrodinger equation with the well known 2n 2 -relation (n = 1, 2, 3,...) for the electron shells, other estimates were needed. It is most remarkable that a purely speculative combination
834
1000 -
2
4
6
Sequence of magic numbers (n)
Figure 7. Values R{n) = exp[(Z n +i — Zn)/Z'] for the sequence of magic numbers n with specially defined exception of 20 and with the fitting value Z' = 10 (dots) compared with the 3"-relation (Eq. 10) straight line. 3 7 Circles are for derivation of new magic numbers (180, 246, and 324), Eq. (11) and crosses for earlier considered 30 numbers 114, 184 and 228.
of the sequences 2, 3, 4, 5, 6,... and of the sequences 1, 2, 3, 4, 5,... and their combinations 35 led Bagge 34 to the result of the following sequences (12) and (13) for the magic numbers. In the first case taking the sequences 2, 3, 4, 5, 6,... as differences to produce 1, 3, 6, 10, 15, 2 1 , . . . and then taking them as differences, one arrives at 0, 1, 4, 10, 20, 25, 56,... and doubling these values: M 2 e 2, 8, 20, 40, 70, 112.
(12)
Beginning with the sequences 1, 2, 3, 4, 5, 6,... as the differences one arrives at 1, 2, 4, 7, 11, 16, 22,... and again using these as differences leads to 0, 1, 3, 7, 14, 25, 41, 63,... which elements doubled leads to M 3 e 2, 6, 14, 28, 50, 82, 126.
(13)
Bagge's question was why did the bold numbers fit the observed magic numbers and how to explain the jump from the Bagge sequence (13) and (14) after the first three elements. A well-known explanation was given by Jensen and Maria GoeppertMayer35 who noted that there is a difference in the spin and orbit configurations in the nuclei preferring in the one case the lower numbers of Eq. (12) and in the other case the higher numbers of Eq. (13). In contrast to this explanation, we see now that the jump between the magic numbers 20 and 28 results systematically
835 from the procedure of Table 1 without any need of a physical explanation of the spin, etc. If our explanation for a quark structure of the nuclear shells is the reason, this would be well different form the spin model and one has to learn again from a co-existence of basically different properties for the phenomena of the nucleus. Vice versa one may find an explanation of the spin-orbit phenomenon related to the threefold multiplicity of Eq. (10) concluding t h a t the stable nuclear shells are combined each with three quark links of the higher shell t o one quark in the low shell. This consideration of t h e magic numbers was involved also t o t h e generalization of the Debye length and the subsequent surface energy in laser produced plasmas to the degenerate electrons in a m e t a l 2 5 with a subsequent q u a n t u m theory of surface tension of metals in agreement with measurements. Only instead of the temperature, the Fermi-Dirac energy had to be used. Generalizing this furthermore to the Fermi energy of nucleons (protons and neutrons) the q u a n t u m surface energy is just compensating the internal energy - dominated by t h e Fermi energy - of the nucleons in a nucleus resulting at the measured size of nuclei. This is a new access to Bohr's droplet model of nuclei as it successfully explained the fission of u r a n i u m 3 6 - however - now on a basically new basis of t h e Debye lengths. 3 8 ' 3 9 One further result is t h a t at about six times higher t h a n nuclear density, the change of the Fermi energy into its relativistic branch makes any nucleation impossible and results in a soup of particles where the mass is eliminated explaining t h e n the quark gluon state. W h e n expanding at the big bang from higher density to t h a t of nuclei, the nucleation begins and the Boltzmann equilibrium permits the generation of nuclei including the endothermic nuclei, however only u p t o the atomic number of about qq
uranium. All these results are to some extend related to the reported measurements of L E N R 2 9 and may indirectly link to a confirmation of work initiated by the cold fusion 9 whatever the motivations or some confusions to these initial developments had been. References 1. B. Josephson, Pathological Disbelief, Lecture given at the Nobel Laureate Meeting, Lindau, June 30, 2004 (Edited version, revised Aug. 20th, 2004). 2. J. Cockroft and A. Walton, Proc. Roy. Soc. Lond. A137, 229 (1933). 3. M.L.E. Oliphant and L. Rutherford, Proc. Roy. Soc. Lond. A141, 259 (1933). 4. M.L.E. Oliphant, P. Harteck, and Lord Rutherford, Proc. Roy. Soc. Lond. A144, 692 (1934). 5. F. Paneth, Naturwissenschaften 14, 958 (1926). 6. F. Paneth, Nature 119, 728 (1927). 7. O. Reifenschweiler, Internal Report Philips Research Laboratories 1961; see Phys. Lett. A 184, 149 (1994). 8. B.V. Derjaguin, et al., Colloid J. USSR 48, 8 (1986). 9. M. Fleischmann, S. Pons, J. Electroanalyt. Chem. 261, 301 (1989); M. McKubre, in Xing Zhong Li (Ed.), Proceedings of the 9th International Conference on Cold Fusion, Beijing, May 2002 (Tsinghua University Press, Beijing, 2003), p. xviii
836 10. 11. 12. 13. 14.
15.
16. 17. 18. 19.
20. 21.
22. 23. 24. 25. 26. 27. 28. 29.
30.
31. 32. 33.
S.E. Jones, Nature 338, 737 (1989). E. Crawford, R. Lewin Sime, and M. Walker, Phys. Today 50 (9), 26 (1997). X.Z. Li, J.T. Tian, M.Y. Mei, C.X. Li, Phys. Rev. C 024610 (2000) X.Z. Li, B. liu, Q.M. Wei, and H. Hora, Laser Particle Beams 22 (4), (2004). H. Hora, Summary about Theory, in Xing Zhong Li (Ed.), Proceedings of the 9th International Conference on Cold Fusion, Beijing, May 2002 (Tsinghua University Press, Beijing 2003), p. xxi E. Yamaguchi and T. Nishioka, Nuclear fusion induced by the controlled out-transport of" deuterions in palladium, in Proceedings Third International Conference on Cold Fusion, Nagoya, October 1992. M. Prelas, F. Boody, W. Gallaher, E. Leal-Quiros, D. Mencin, and S. Taylor, J. Fusion Energy 9, 309 (1990). X.Z. Li, Bin Liu, Z. Ren, et al, in X.Z. Li (Ed.), Proceedings of the 9th International Conference on Cold Fusion, Beijing, 2002 (Tsinghua University Press, 2003), p. 197. J. Tian, B. Liu, X.Z. Li, et al, X.Z. Li (Ed.), Proceedings of the 9th International Conference on Cold Fusion, Beijing, 2002 (Tsinghua University Press, 2003), p. 360. A.G. Lipson, A.S. Roussetski, G.H. Miley, and C.H. Castano, in X.Z. Li (Ed.), Proceedings of the 9th International Conference on Cold Fusion, Beijing, 2002 (Tsinghua University Press, 2003), p. 218. Y. Deng and X.Z. Li, Conference Three Gorges, 6 October 1998. X.Z. Li, S. Guang, Xiu M. Qiao, et al, in W.F.M. Collins and R. George (Eds.), Proceedings of the Asti Meeting, October 1999, Conference Proceedings (Italian Physical Society, Bologna, 2000), p. 102. H. Hora, J.C. Kelly, J.U. Patel, M.A. Prelas, G.H. Miley, and J.W. Tompkins, Phys. Lett. A175, 138 (1993). Z. Hennis, S. Eliezer, and A. Ziegler, J. Phys. G15, L219 (1989). J. Rafelski, M. Sawitzki, et al, Fusion Technol. 19, 136 (1991). H. Hora, Gu Min, S. Eliezer, P. Lalousis, R.S. Pease, and H. Szichman, IEEE Trans. Plasma Sci. PS-17, 290 (1989). S. Ichimaru, Rev. Mod. Phys. 65, 255 (1994). R.G. Clark, H. Hora, P.S. Ray, and Sir Ernest Titterton, Phys. Rev. C18, 1127 (1978). R. Kippenhahn and A. Weigert, Stellar Structure and Evolution (Springer, Heidelberg, 1990). G.H. Miley, G. name, M.J. Williams, J.A. Patterson, J. Nix, C. Cravens, and H. Hora, in M. Okamoto (Ed.), Progress in New Hydrogen Energy (New Energy and Industrial Technology, Tokyo, 1997), p. 627. H. Hora, G. Miley, and J. Kelly, in E. Panarella (Ed.), Current Trends in International Fusion Research - Proceedings of the Third Symposium (NRC Press, National Research Council of Canada, Ottawa, ON, Canada, 2002), p. 527. Michael Turner, see P. Gwynne, Phys. World 14 (2), 6 (2001). Spencer Abraham, APS News 12 (11), 8 (2003). M. Brack, P. Quentin, and D. Vautherin, in M.A.K. Lodla (Ed.), Proceedings of the International Symposium on Superheavy Elements, Lubbock, Texas (Pergamon, New York, 1978), p. 309; A. Sobieczewski, Phys. Scr. 10A, 47 (1974); M. Schadel, et al, Nature 388, 55 (1977); M. Schadel and J.V. Kratz, Physikalische Blatter 53, 865 (1997); P. Armbruster, in P. Blasi and R. Ricchi (Eds.), Proceedings International Conference on Nuclear Physics, Florence/Italy 1983 (Tipografia Compositori, Bologna, Italy, 1984), p. 343, see also the agreement with the new magic numbers (12): K. Rutz, M. Bender, T. Burenich, T. Schilling, P.G. Reinhard, J.A. Maruhn, and W. Greiner, Nuovo Cimento 110A, 1237 (1997).
34. E. Bagge, Naturwissenschaften
35, 376 (1948).
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35. 36. 37. 38.
0 . Haxel, J.H.D. Jensen, and H.E. Suess, Zeitschr.f. Physik 128, 295 (1950). L. Meitner and O. Frisch, Nature 143, 239 (1939). H. Hora, Czechoslovak J. Phys. 48, 321 (1998). H. Hora, Plasma Model for Surface Tension of Nuclei and the Phase Transition to the Quark Plasma, Report CERN-PS/DL-Note-91/05, August 1991, see also H. Hora, Laser Interaction and Related Plasma Phenomena, Vol. 10 (Plenum Press, NY, 1992), p. 19. 39. H. Hora, G. Miley, F. Osman, and P. Hammerling, in C.R. Phipps (Ed.), High Power Laser Ablation V, SPIE Proceedings No. 5448, 2004, p. 119.
ON T H E POSSIBLE M A G N E T I C M E C H A N I S M OF SHORTENING T H E RUNAWAY OF RBMK-1000 R E A C T O R AT C H E R N O B Y L NUCLEAR POWER PLANT
D. V. F I L I P P O V A N D L. I. U R U T S K O E V RECOM,
Russian
Research
Center
"Kurchatov
Institute,"
Russia
G. L O C H A K Fondation
Louis de Broglie,
France
A. A. R U K H A D Z E General Physics
Institute,
Russian
Academy
of Science,
Russia
The official conclusion about the origin of the explosion at the Chernobyl Nuclear Power Plant (CNPP) is shown to contradict significantly the experimental facts available from the accident. The period of reactor runaway in the accident is shown to be unexplainable in the framework of the existing physical models of nuclear fission reactor. A hypothesis is suggested for a possible magnetic mechanism, which may be responsible for the rise-up of the reactor reactivity coefficient at the fourth power generating unit of C N P P in the course of testing the turbine generator by letting it run under its own momentum.
1. The Questions not Answered The present paper is aimed at clarifying the physical mechanism of RBMK-1000 reactor explosion. The official conclusion does not seem to be satisfactory: First, many questions, as shown below, have not been answered; Second, the official conclusion is based on a numerical simulation whose results do not agree with the experimental facts and analytic estimations. Here a hypothesis is suggested that the accident was caused by the change, in the course of testing the turbine generator by running it under its own momentum, of decay of the nuclei emitting delayed neutrons. Despite what seems at first glance to be the low plausibility of such a hypothesis, it provides a simple and logical interpretation of the variety of experimental facts that have not been explained previously. In the authors' opinion, a number of experimental facts observed during the Chernobyl accident have not been explained convincingly. These include: • • • •
the integrity of structures in the reactor cavity, the impossibility of locating a considerable amount of fuel, two detonations 1-2 s apart, an unnatural bright glow above the reactor cavity after the explosion, 838
839
• a distortion of the isotopic ratio in the fuel samples studied, including the isotopic shift toward 2 3 5 U, 1 , 2 • the attraction of electrical cables to steam pipes, • and most important: the very mechanism of reactor's runaway. How could the reactor with a high rate of fuel consumption (up to 20 MW day/kg), and spoiled with xenon, be accelerated within 10 s from 200 MW power level (i.e., 6% of nominal power) to the level exceeding the nominal one by a factor of several dozen? Why did the safety rods fail to stop the runaway? According to the reactor design, the rod lowering rate was sufficient to compensate for any possible accidental runaway which, if driven by the delayed neutrons, could happen with a typical time of ~10s (i.e., with the lifetime of the nuclei emitting delayed neutrons). The runaway, however, proceeded three times faster. The power level of 530 MW was registered by the instruments at the third second; the sixth second brought the signal from the AZ controller which had been tuned at the 1600 MW power level. Afterwards, the runaway proceeded presumably much faster - no detailed information is available. Thus, within the first 6 s the power was increasing by a factor e each 3 s. The above facts do not agree with the official version 3-6 in which the analysis of the origin and evolution of the accident was based on a numerical simulation. The authors of 3-6 suggested the following main sources of the accident: • As the reactor was spoiled before the accident, the operative reactivity margin was limited to 6-8 safety rods only, with the minimal allowable number equal to 30 rods; of course, a decrease of the operative reactivity margin by itself does not lead to a runaway, but it is dangerous because it produces an unstable state. • Development of a strong of energy release (i.e., neutron density) inhomogeneity in vertical direction in the reactor, caused by the downward motion of the safety rods, led - under the condition of the decreased operative reactivity margin - to the reactor's runaway. • The high positive value of the steam reactivity coefficient (compared to the designers' specifications) resulted in a substantial shortening of the instability development time. The steam reactivity coefficient av is defined as a ratio of the rate of excess reactivity variation to the rate of specific steam content variation in the coolant. Let us evaluate the possibility of altering the reactor runaway time in the frame of the official accident model. The intensity of neutron breeding in the reactor core is described by the neutron-breeding coefficient K\>, which is the ratio of the neutron number of a certain generation to a similar number in the preceding generation. The excess reactivity p is defined as (K^-l)/K\>. For p = 0 the reactor is in a steady-state regime, for p < 0 and p > 0 the reactor is, respectively, slowing down and accelerating. In the process of nucleus decay a small fraction /3 of neutrons is
840
emitted by the daughter nuclei; they do it with a large enough delay of ~10s (these neutrons are called delayed). For various types of reactors the (5 value varies in the range from 0.2 to 0.7%. For the given RBMK-1000 (high-power channel-type reactor), before the accident the /3 value was equal to 0.45%. The reactor state is well known to be described by the following kinetic equations: 7 dn p-P y-^ dCi fan i
where C,, Aj, and fa are, respectively, the density, the inverse lifetime, and the fraction of nuclei emitting delayed ith group neutrons (/? is the value averaged over all the fa values); T = 1 0 _ 3 s is the lifetime of one generation of neutrons. For the estimation one can use the wide-spread one-group approximation for delayed neutrons, taking A = 0 . 1 s - 1 (Ref. 7) and, hence, the condition AT -c fa For a constant value of reactivity p, it is not difficult to find the eigenfunctions of the linear system of differential equations, Eq. (1). Analyzing the eigenvalues of the increment k of the respective characteristic equation, it is easy to notice that it is the presence of delayed neutrons that makes it possible to regulate the reactor operation. Indeed, for small p (namely, 0 < (fap) ~ fa), one obtains from Eq. (1): k = Xp/(fa-p), i.e., the reactor speeds up with a characteristic time of ~10 s, which is the lifetime of nuclei emitting delayed neutrons. For large values of reactivity, p > fa, one obtains k = (p-/3)/T, i.e., the runaway is due to instantaneous neutrons, with characteristic time less than 0.1s. Of course, the function k(p) is continuous for any reactivity and, for a certain p value, may become k ~ 3A ~ (3 s ) - 1 . In such a transient region, p < fa, the function k(p), however, goes up very fast - therefore, the phase volume of initial conditions for such a solution is small. In other words, the solution with k ~ 3A is unstable in the sense that for a small reactivity change as in the course of turbine generator test, this solution has to change its time increment to a substantially different value. In the accident, however, the power rise proceeded, during two periods (i.e., 6s), with a constant increment, which obviously suggests that the observed runaway should have been a stable one. The excess reactivity depends on parameters of the medium, including the coolant density 7. As regards the cause of the runaway, it was claimed i n 3 - 6 that upon decrease of the coolant density one has to observe a strong rise of excess reactivity up to 5/3 (where (3 is the fraction of delayed neutrons) - see curve "a" in Fig. 1 taken from Ref. 4. The authors presented the dependence, which was calculated at the stage of design (see curve "6") and appeared to agree with the experimental results obtained in the course of testing the RBMK-1000. It is seen that these curves differ substantially for low values of 7. The calculated curve "6" in Fig. 1 is confirmed by the results of experimental tests, whereas curve "a" is based on a single event that took place in 1986 at the fourth unit of the Chernobyl Nuclear Power Plant (CNPP). From the scientific viewpoint, curve "6" in Fig. 1 has a larger credit. Note that for an excess reactivity p > fa, the reactor runaway is driven by
841
instantaneous neutrons. Therefore, the validity of the curve p{"i) given in Ref. 4 would imply that the reactor may have been accelerated by merely a complete coolant withdrawal. Such a trivial disaster in water supply must lead to a runaway driven by the instantaneous neutrons with period less than 0.1 s (in such a case, the reactor turns to be an "atomic bomb"). Were it so, a further exploitation of such type reactors would be inadmissible. We hope anyway that curve "6" in Fig. 1 is more realistic as it was obtained by the designers who accurately and with much responsibility both calculated and experimentally tested all the main parameters of the system at various stages of fuel burning.
y kg/m3
Figure 1. Excess reactivity, in the units of /3, as a function of the coolant density 7: "a" — the calculation after the a c c i d e n t ; 3 - 6 "b" - the design curve (i.e., the one calculated before the accident).
According to the official version, 3-6 the accident developed as follows: a localized power rise under condition of diminished level of the operative reactivity margin (6/8 safety rods instead of minimally required 30 rods) caused a localized overheating of the coolant. This resulted in a decrease of the coolant density, which, in turn, induced an increase of excess reactivity - see curve "a" (Fig. 1). The rise of reactivity heightened the reaction rate and the power (note that the heat release power is proportional to the neutron density) resulted in the development of instability in the time behavior of neutron density. Below, the time of such an instability development is shown to substantially exceed the actual time of the reactor runaway observed during the accident even if one takes, as input data, the disputable curve "a" (Fig. 1) for the dependence of the excess reactivity coefficient on the coolant density. Note that beside the steam reactivity coefficient, also the temperature and power coefficients may influence the dynamics of instability, by diminishing the rate of the reactivity rise.8 It has been shown9 that the runaway of the reactor RBMK-1000 of the Chernobyl NPP fourth power-generating unit was during the accident driven by delayed neutrons. This conclusion9 was based on the instrument readings that indicated that the power rise during the first 6 s had been developing at a constant value
842
of the excess reactivity, p ~ 0.5/3, and the power had changed with time approximately by the law N = 200e*/ 3 MW, i.e., with a period of 3s. Further on, the runaway became probably faster: after the next 4 s, a signal pointing to a sharp increase in the gas pressure in the reactor graphite stack was detected. Thus, in accordance with the available data, the runaway of the reactor power lasted on the whole t > 10 s. Based on this fact, it was reasonably concluded9 that the reactor runaway had proceeded with a participation of delayed neutrons because with instantaneous neutrons the process would have been approximately 100 times as fast and absolutely uncontrolled by instruments at the control panel. The irrelevance of the runaway driven by instantaneous neutrons is supported indirectly by the absence of visual damages of the reactor wall (the so-called casing). This fact was established in 1990 by the staff of the "Complex Expedition" of the Kurchatov Institute: drilling wells made it possible to survey the reactor's internal surface with the help of a periscope. The reactor cavity was found to be fully empty, i.e., the reactor itself had completely disappeared. No visual deformations or damages of the internal surface of the casing were observed and, moreover, even the paint coating was well preserved. Visual inspection revealed some signs of soot only in the southeast area of casing's internal surface. This cast doubt on the hypothesis of fire in the reactor and a subsequent melting of the fuel. The experts who investigated the fragments of the fuel arrived at the same conclusion.10 The above arguments suggest a conclusion that the scenario of the accident 3 ' 4 widely accepted to date not only fails to explain the facts, it directly contradicts them. 2. Analysis of the Widely Accepted Mechanism According to the official version, the rise of reactivity was caused by large steam coefficient values. In this approach, however, the rate of the reactivity rise is proportional to the neutron density, and therefore the neutron flux has to grow much slower compared with the case of a sudden change of reactivity considered in Ref. 7. We will show that even for the overestimated values of the calculated function p(^) - curve "a" in Fig. 1 - the e-times rise of the power from 200 to 530 MW would require not less than 20 s, whereas the actual rise took 3 s. Given the validity of the overestimated version of the dependence p(j) (curve "a" in Fig. 1), one can obtain the following restriction on the steam coefficient av:
because, as follows from the data 8 (page 34), in the reactor which attains the steadystate regime of fuel reload, (3 = 0.0045. Note that the officially reported value3 is even smaller: av = 2 x 10~ 4 %~ 1 . According to the reactor design,8 the steam capacitance of the reactor with nominal power operation amounts to 1.5 T/s, while the average outlet value of 7 is equal to 15% and the amount of coolant inside the reactor is not less than 30 T; the
843
rate of the coolant density (specific steam content) variation in time is proportional to the power (i.e., to the neutron density). The coolant is pumped through the reactor by eight Main Circulation Pumps (MCP). The schedule of the tests of the fourth CNPP power-generating unit assumed four of these pumps to be fed by the electric circuit of the 3rd CNPP unit. Therefore, these four pumps must have been sufficient for the reactor cooling at least up to 50% of nominal power, whereas the reactor runaway started from 6% of the nominal power. Even if the coolant circulation had stopped completely, which could not have happened, the rate of the reactivity rise would not have exceeded the value: dp_dpd7 di ~ d7"dT
<
6/3 1.5T/sW 0 075 30T W^'
where WQ = 200 MW is the initial reactor power for the runaway process, and WB = 3200 MW is the nominal power. Hence, for the maximum p(t) growth rate, one has the equation: dp nn -£=a0—, di no
2
where a < 0.025 s _ 1 , n and no are the neutron density and its initial value. Note that Eq. (2) is valid locally because we have restricted ourselves to the assumption that the coolant confined in a closed space is evaporated at the expense of released heat. Solving the system of Eqs. (1) and (2) in the approximation of single effective group of delayed neutrons and allowing for the initial conditions p(0) = 0, p' t (0) = a/3, and p' t t (0) = a/3n' t (0) = 0 as far as the runaway started from the steady state, we arrive at the equation: T \ d2p
(T\
\ dp
p dp
Ap2
In the approximation considered here (TA
For t
(5)
Thus, in the frame of adopted initial conditions, the power rise during the first 10 s cannot significantly exceed a factor of 1.5. This agrees with the solutions 7 because in our case at the first stage the excess reactivity increases linearly at the rate a. During the accident the reactor increased its power e times each 3 s, so it follows that even the steam reactivity coefficient as high as taken in Refs. 3 and 4 (see
844
curve "a" in Fig. 1) could not have been the cause of reactor runaway upon the coolant overheating. The multi-group model for the description of delayed neutrons will not change major results: the e—times power increase from 200 to 530 MW cannot have been attained faster than within 20 s, whereas actual rise took 3 s. The numerical models suggested in Refs. 3-6 fail to explain the rate of reactor power runaway. This casts doubt on the validity of the calculated dependence of the excess reactivity on the coolant density (curve "a" in Fig. 1), which seems to be too high compared to the respective designed values (curve "6"). 8 Let us consider the statement 3 concerning the role of spatial inhomogeneity of energy release (i.e., neutron density) in the reactor runaway. First, note that the bursting depressurization of reactor and flying reactor's away apart indicated, most probably, on rather homogeneous increase of neutron density. 11 Moreover, already in the pioneering papers by Fermi, 12 the allowance for spatial inhomogeneity under condition of a small positive excess reactivity was shown to suppress high spatial harmonics. For a high enough reactivity, the high spatial harmonics grow up, at least, slower that the fundamental one. Indeed, the first equation in (1) takes, with allowing for spatial inhomogeneity, the following form Ref. 12:
^=DAn+^-n
,
+
£xiCi,
(6)
i
where D = L2/T is the coefficient of neutron diffusion, T, as above, is the lifetime of one generation of instantaneous neutrons, and L is the diffusion length. The diffusion length is L ~ 50 cm for graphite and ~3cm for water. Seeking solutions of Eq. (6) in the form n(t) = ip(x,y,z)f(t) under conditions n = 0 at the reactor boundary, we find: Aip = ~Q2f: p-(qL)2-
dn
"dT
=
T
-0 n •
(7)
7 y A,Ci, i
where q is the wave vector. It is seen that the inhomogeneity decreases the reactivity by a value {2-KL/O)2, where a is the wavelength of spatial harmonic of the perturbation. In other words, spatial inhomogeneity of the neutron distribution gives rise to a diffusion term in the reactor kinetic equations. This term "washes out" the fluctuations of neutron spatial distribution. We can summarize the above considerations as follows. (1) The official versions of the accident contradict the available facts and contemporary physics at the following points. • The dependence of reactivity on coolant density is overestimated with respect to the designed data.
845
• The increment of the instability growth calculated analytically from the equations analyzed exceeds by far - even for the overestimated reactivity - the respective results of numerical simulation. 3 ~ 6 • The claim of a strong inhomogeneity of neutron density is not compatible with the explosion; anyway, a strong inhomogeneity may result in an increase of the runaway time rather than its decrease. (2) The cause of the CNPP accident has not yet been convincingly explained and the contemporary state of science does not seem to be able to provide such an explanation. (3) To interpret such a high rate of the reactor runaway, we think one should assume the existence of a new physical phenomenon (or even a number of such phenomena). Below we suggest a possible mechanism of the reactor runaway which does not contradict the above-mentioned facts. 3. The Bound-State /3-Decay Despite the common belief that the energy-space-time scales of nuclear processes differ considerably from those of atomic ones, many examples of a strong coupling of atomic and nuclear phenomena are known to physics. A theory of /3-decay into a bound state (i.e., a decay in which the /3-electron does not escape from the atom and is captured into an unoccupied bound state in the atom) was developed in Refs. 13-16. The bound-state /3-decay was shown 17 to additionally increase the phase volume of final states and, hence, to increase the probability of /3-decay. The ratio of the decay constants (i.e. decay probabilities) into the bound, Ab , and free states, Ac , was calculated in Refs. 15 and 16. For the low energy /3-decay of fully ionized heavy atoms, the ratio Ab/Ac can be as large as 103 to 104. Thus, the presence of unoccupied electron states may result in a thousands of times increase of /3-decay probability. The theory of the bound-state /3-decay was successfully verified in experiments. 18 ' 19 Interestingly, for 187 Re (Ref. 19) the complete ionization decreased the half-lifetime by a factor of 109 (specifically, to 33 years for a bare nucleus vs. 4.3 x 1010 years for a neutral atom). The calculation of the ratio of probabilities of /3-decay into bound and free states is similar to a conventional calculation of the ratio of probabilities of K-capture and positronic /3+-decay.20 Relying on the results, 15 ' 16 ' 20 we can formulate the following significant statement: for every allowed nuclear transition the appearance of an unoccupied electron state in the atom increases A, the constant of /3-decay, by a value 5X (in atomic units H = c = me = 1): 6\_n\ye(R)\2(E-lf A 2 f(Z,E)
~
2K{aZf(E-lf N*f(Z,E) '
l ]
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where ^e(R) is the value of the electron wave function at the point of nucleus location, E the energy of nuclear transition, Z the nuclear electric charge, and f(Z,E) is the Fermi integral function: E
f(Z,E) = J' F{Z,s)e^^i{E-e)2de,
(9)
1
a = 1/137 is the fine structure constant, and iV is principal quantum number of the unoccupied state of electron in the atom. The second relation in Eq. (8) is derived within the approximation of hydrogen-like atomic state of electron. According to the well-known approximation, 20 the function f(Z,E) of Eq. (9) rises with increasing energy faster than E2 (for E 3> 1 one can use the approximation / ~ £ l 5 /30). This enables us to find from Eq. (8) for TV = 1 the value of SX:
%-«*(§)'•
m
It is seen that SX/X is larger for nuclear transitions with a lower transition energy E, i.e., for transitions to upper-lying (excited) levels in the daughter nucleus. The /3-decay to the bound state opened owing to the atom ionization was considered in Refs. 13-19. There are, however, other ways to produce unoccupied electron states. Kadomtsev 21,22 turned to the problem of transformation of electron states in an atom in a strong magnetic field. It was shown 21 that electrons, in heavy atoms in a strong magnetic field, do not tend to occupy the lowest energy levels. This means that the atom will be in an excited state and the lowest unoccupied atomic levels will be opened for the /3-decay into the bound state. This implies that the application of a strong enough magnetic field opens the bound-state /3-decay channel. The presence of a strong magnetic field in the accident is suggested by the observed ejection of electric cables from the wall. The probable origin of such a strong magnetic field is discussed below. We shall now turn to the problem of how the bound-state /3-decay can influence the fraction of delayed neutrons in the nuclear reactor. 4. The impact of disturbed rate of decay of nuclei emitting delayed neutrons upon the reactivity The decay of 235 U gives a large number of daughter nuclei of atomic weight in the range from A = 72 to 160. The distributions of daughter nuclei in their mass and electric charge have been investigated in the literature in detail. The majority of daughter nuclei are unstable because of an excess of neutrons. 23,24 A part of these nuclei (~50 nuclei) are capable of emitting delayed neutrons. The scheme of their decay in which they are the mother nucleus is shown in Fig. 2. 24 The /3-decay of mother nucleus (i.e., emitter of a delayed neutron) via the channel with a lower /3-transition energy gives an intermediate nucleus in an excited nuclear state. If the excitation energy exceeds Qn (the binding energy of the neutron),
847
OR * i
,
Qn Daughter nucleus Z+1./V-2
ii Mother nucleus Z, N
Intermediate nucleus Z+1./V-1
Figure 2. The scheme of decay of a nucleus emitting delayed neutron. Qt, is the maximum energy of /3-decay, and Qu is the binding energy of the neutron in the intermediate nucleus.
the intermediate nucleus emits a neutron. This emission takes place practically instantaneously, and so the delay time is fully determined by the lifetime of the mother nucleus. Note that the fraction of delayed neutrons is determined by the /?decays with small transition energy, and their fraction for all the emitters of delayed neutrons does not exceed 10%. 24 For the majority of intermediate nuclei, the energy of neutron escape amounts to the value Qn ~ 5 to 7MeV. As far as the energy (Qp - Qn) of /3-decay with a neutron yield is much smaller than Qp, it follows from Eq. (10) that if the channel of the bound-state /3-decay is open, the ratio SXn/Xn for the neutron channel with a small energy E has to exceed considerably the value of 5Xp/Xp for a neutronless decay to lower-lying levels: 5Xn Xn
SXp Xp
(11)
The fraction of delayed neutrons is proportional to the ratio: /3oc
An An + A/3
The relative change of fraction of delayed neutrons cab easily be derived to give: SP _ Xp f5Xn P
X \ A,
where A = An + A^ + (5An + 5Xp. Hence,
5Xp* >o, X,
the appearance of an unoccupied electron state in an atom, capable of emitting a delayed neutron, leads to an increase of the fraction of delayed neutrons. Equation (6) allows for the densities of only those nuclei emitting delayed neutrons that underwent /3-decay via the neutron channel, while the daughter nuclei which underwent the /3-decay without neutron emission are thought of as lost to the chain reaction. In fact, the neutrons, which caused the production of daughter nuclei undergoing a neutronless /?-decay are taken into account in the growth of the energy loss, i.e., in the decrease of the reactor excess reactivity p. As is known, 24 the number of decays with neutron release is less than vn ~ 10% of the total number of /J-decays of nuclei emitting delayed neutrons. In the steady-state regime of reactor operation the fraction of delayed neutrons is j3 ~ 5 x 10~ 3 , the decay constant for nuclei-emitters is A ~ 0.1s" 1 , and the lifetime of instantaneous neutrons is T ~ 10 _ 3 s; Eq. (1) gives the concentration of all the nuclei emitting delayed neutrons (including also those nuclei whose decay does not release the neutron): C = t'nT7^ n ~ J / n 50n~ 500n, A1 i.e., the number of nuclei emitting delayed neutrons exceeds the number of instantaneous neutrons by more than two orders of magnitude. A huge number of daughter nuclei capable of emitting neutrons are always present in the reactor. Therefore, the distortions of the mechanism of decay of emitters of delayed neutrons may cause a considerable change of the neutron density. To analyze the behavior of the reactor upon changes of the /3-decay constant A, we consider the kinetic Eq. (1) in the single-group approximation for delayed neutrons with allowance for all the nuclei emitting delayed neutrons (including also those nuclei whose decay does not release the neutron):
where n is the neutron density, p the excess reactivity of reactor, /3 the fraction of delayed neutrons, T = 1 0 - 3 s the lifetime of one generation of instantaneous neutrons, N the density of nuclei emitting delayed neutrons, including nuclei whose /3-decay does not release the neutron; An the constant of /3-decay with release of neutrons, \p the constant of /3-decay without release of neutrons, and /3t = /3(An + A/g)/An is the fraction of all the nuclei emitting delayed neutrons. Let us consider a reactor in a steady-state regime, i.e., with reactivity p = 0, the reactivity caused by the instantaneous neutrons being constant, pi nst = - Pb (/3b is the initial value of the fraction of delayed neutrons). Consider the variations -V ~^ ('V3 + ^Z 5 ) a n d ^n -> (An + <^n) which obey Eq. (11). Assuming the above variations to occur instantaneously (i.e., in a time interval
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following relation from Eq. (12):
f +A
dn
/?(,
8\j3 = 0
8Xn-
(13)
An
(here A = (An + A^ + 5Xn + 5Xp) ) which, in the first order in SX, describes an instability with the following increment:
As is known, 24 the major contribution to the production of delayed neutrons stems from daughter nuclei Z ~ 35 to 37. For the neutronless channel the transition energy is estimated to be Ep 3> En ~ 1 (in units of the electron rest mass). Using a rough estimate of Eq. (10) and allowing for the inequality TX A+<5A, the respective relative increase of probability of neutron-releasing decays into excited nuclear states, SXn/Xn , substantially exceeds the value 5Xp/Xp for decays without neutron release, hence, the fraction of delayed neutrons, /3, increases, in an active media, this leads to the runaway of the reactor. Thus, in contrast with the official version,3 it is not the reactivity that increases to the value 5/3 (see curve "a" in Fig. 1), but the value of (3 itself, i.e., the fraction of delayed neutrons. k
5. Probable Role of Magnetic Monopole in the Accident This brings about reasonable questions: What could be the source of magnetic monopoles at the fourth unit of the Chernobyl power plant? How could they get into the reactor? The idea of invoking magnetic charge as a mechanism of the Chernobyl accident has arisen during a study of the physical properties of the "strange" radiation observed in Ref. 25. In experiments dealing with electric discharge on metallic foils in fluids26 for nuclear emulsions and film detectors located at distances of up to 2 m from the setup axis, abnormally broad tracks similar to a caterpillar's track appeared regularly. Since the sizes of the tracks did not allow one to explain their origin in terms of known kinds of radiation (a, (3, 7), the existence of a new
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type of radiation, conventionally referred to as "strange", was assumed. When a weak magnetic field, Hz ~ 20 Oe, was applied to the setup along the Z-axis, the pattern of the tracks changed. This circumstance suggested a magnetic nature for the detected radiation and provided grounds for regarding the radiation as a flux of magnetic particles. 27 ' 28 The current source used in the described experiments 26 was a discharge of a capacitor bank. In the tests done on April 26, 1986, the eighth turbine generator was disconnected from the substation and served as a power source for the purposes of only the fourth unit of the Chernobyl Power Plant. It is noteworthy that the initial power of the running under it's own momentum turbine generator was 40 MW and the run lasted for ~40s; hence, an occasional short in the electric circuit could have created conditions similar to those used in experiments in Ref. 25. This analogy is largely intuitive but it complies well with evidence given by the operating personnel. Tregub, the supervisor of the previous shift at the fourth unit told the following. "First, I heard a characteristic noise of a shutting-down turbine generator. About 6 s later there was a stroke. I thought that the turbine blades were broken. Then another stroke followed. I looked at the upper floor and felt that it was going to fall down. I moved away to the safety shield. The instruments displayed a terrible emergency. I ran out of the building . . . a floodlight shone from the "Romashka" roof but some glow was also seen above the fourth unit." 29 Davletbayev, deputy supervisor of the turbine department said: "After several seconds, a low-pitched sound was heard from the turbine building, the floor and the walls were severely shaken, the dust and small-sized chips fell down from the ceiling, the fluorescent lighting died out, and there became darkish. A hollow stroke accompanied by thunder-like bursts was immediately heard. Then the lighting appeared again." Dyatlov, the deputy chief engineer at the second tail of the Chernobyl Power Plant said: "I heard the first stroke from the turbine building. It was heavy but not as heavy as the next one, which was heard several seconds later. This was perceived as either one long stroke or two strokes following one another. The second one was more intensive." 30 Thus, contrary to the generally accepted opinion, this hypothesis suggests that the development of the accident started at the turbine building and that pressing the emergency button AZ-5 incidentally coincided in time, and by no means could have prevented the disaster. The initial suggestion of the formation of magnetic monopoles at the moment of turbine generator run under its own momentum can be advanced to form some scenario of the accident development. The magnetic monopoles, which have presumably formed in the vicinity of turbine generators, could get into steam pipes. Since oxygen is paramagnetic, magnetic particles should form so-called "bound states" with oxygen and move along the steam pipes, together with the steam, as in wave-guides. A "magnetic current" should have flown in the steam pipes. The electric wires located near such a field should be attracted to the magnetic current formed by the monopoles moving along the steam pipes. This
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can be really observed when one passes along the steam pipe route; moreover, some of the distribution boards were torn off together with the fastening fittings and fragments of partitions (near the separator department). In the separator buildings, even the partitions were ruined. The magnetic charges, having got into the main circulation pumps should, caused a failure in the electric motor operations. Apparently, this fact is responsible for the failure of power supply for four main circulation pumps (two north and two south ones). The failure took place exactly in those pumps that were supplied from the running under it's own momentum turbine generator No. 8. The other four main circulation pumps were supplied from the third unit and these pumps remained intact. After entering the reactor, the magnetic monopoles should have interacted both with the 238 U nuclei and the nuclei emitting the delayed neutrons, which resulted in the growth of reactivity and hence, rise up of the power and the steam explosion. The probable production of a huge amount of hydrogen as resulted from nuclear transmutation may have caused a hydrogen explosion as well. The two successive explosions in the region of the reactor at the moment of the accident 30 can be consistently explained within the framework of the mechanism we consider if one takes into account the difference between the pipeline lengths from the turbine building to the north and south separators. Based on experimental results, 26 it can be claimed that not only 238 U nuclei but also some other nuclei, for example, 1 2 C, could be transformed under certain conditions under the action of magnetic monopoles. Thus, it can be suggested that once magnetic monopoles have got into the reactor, the reactor graphite should also undergo a transformation. In a study of the elemental composition of the post-accident fragments of graphite blocks from the fourth unit of the Power Plant, considerable islets of Al, Si, Na, and U were found within the graphite depth, although it is well known that highly pure graphite is used in reactors. This fact can serve as indirect evidence supporting the assumption about partial transformation of graphite. A number of eyewitnesses including the members of the Government Commission have noted that the glow observed above the ruined reactor during the first days after the accident was unnaturally colored.29 This fact can be easily explained within the framework of interaction of magnetic monopoles with excited atoms, which shifts the electronic levels of optical transitions, 32 ' 33 giving rise to a color spectrum unusual for the human eye.
6. Conclusions The author is aware of the fact that his hypothesis may provoke quite understandable skepticism among professionals. However, any hypothesis is admissible if it is able to explain some of the facts that do not fit in the framework of the existing views, and predicts some other facts that can be verified experimentally. The following studies are proposed for verifying the hypothesis in question:
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(1) A thorough determination of the isotopic composition of uranium in the fuel-containing masses (FCM). (2) Determination of the isotopic composition of the graphite units and carbon contained in the F C M (certainly, with allowance for the conducted campaign). (3) It is quite probable t h a t radionuclides not characteristic of a uranium fuel cycle will be detected, because some 2 3 8 U should have split under the action of the monopoles. (4) Fresh fuel assemblies were left in the central room and remained tight. If magnetic monopoles did actually participate in the accident, some of these could get into the fresh fuel and thus distort the initial isotope ratio toward 235TJ
(5) Finally, a direct experiment can be carried out, because magnetic monopoles should be stable particles such as electrons a n d one could a t t e m p t to detect t h e m using nuclear emulsions. T h e tracks of magnetic charges are rather typical 2 6 and can be easily identified. T h e monopoles themselves can be "pulled out" by means of a current coil.
References 1. I.E. Kuz'mina and Yu. N. Lobach, Nuclear fuel and peculiar features of aerosols in the installation "Shelter", Atomic Energy 82 (1), 39 (1997). 2. E.V. Sobotovich and S.I. Chebanenko, Isotope contents of uranium in soils of the near zone of Chernobyl Nuclear Power Plant, Phys. Doklady 885 (1990). 3. Information on the accident at the Chernobyl Nuclear Power Plant and its implications, submitted to IAEA, Atomic Energy 61 (5), 302 (1986). 4. E.O. Adamov, V.V. Vasinger, V.P. Vasilevskii, et al, An estimate of qualitative effects of probable perturbations during the accident at CNPP, in The First International Workshop on Severe Accidents and their Implications (Nauka, Moscow, 1990). 5. E.O. Adamov, V.P. Vasilevskii, A.I. Ionov, et al. Analysis of first stage of the accident at the 4-th unit of Chernobyl Nuclear Power Plant, Atomic Energy 64 (1), 24 (1988). 6. A. A. Afanasieva, A.M. Fedosov, R. Donderer, et al, Analysis of the accident at Chernobyl Nuclear Power Plant with allowance for the damage of the reactor core, Atomic Energy 77 (2), 87 (1994). 7. M.A. Shultz, Control of Nuclear Reactors and Power Plants (Westinghouse Electric Corporation, Pittsburgh, 1955); in the book translated to Russian by "Publishers of the Foreign Literature", Moscow, 1957, pp. 29-70. 8. N.A. Dollezhal and I.Ya. Yemel'yanov, Channel Nuclear Power Reactor (Atomizdat, Moscow, 1980), pp. 22-23, 34, 50, 96-97 (in Russian). 9. G.N. Kruzhilin, On the features of explosion of RBMK-1000 reactor at Chernobyl Nuclear Power Plant, Physics Doklady 354 (3), 331 (1997). 10. E.B. Anderson, B.E. Burakov, and Z.M. Pazukhin, Did the fuel of the 4-th unit of Chernobyl Nuclear Power Plant melt? Radiochemistry (5), 155 (1992). 11. A.N. Kiselev, A.I. Surin, and K.P. Checherov, Post-accident survey of the reactor at the 4-th unit of Chernobyl Nuclear Power Plant, Atomic Energy 80 (4), 240 (1996). 12. E. Fermi, Research Papers, Vol. 2 (Nauka, Moscow, 1972), pp. 316-326 (in Russian). 13. J.N. Bahcall, Theory of bound-state beta decay, Phys. Rev. 124 (2), 495 (1961).
853 14. K. Takahashi and K. Yokoi, Nuclear /3-decays of highly ionized heavy atoms in stellar interiors, Nucl. Phys. A404, 578 (1983). 15. K. Takahashi, R.N. Boyd, G.J. Mathews, and K. Yokoi, Bound-state beta decay of highly ionized atoms, Phys. Rev. C36 (4), 1522 (1987). 16. I.S. Batkin, On the problem of /3-decay into bound states, Izvestiya AN SSSR, Ser. Phys. 40 (6), 1279 1976 (USSR Acad. Sci. Reports; in Russian). 17. F.A. Gareev and Yu. L. Ratis, Capture of virtual positrons by the nuclei of highly ionized atoms as a new type of natural radioactivity, Estestvoznanie, Ekonomika, Upravlenie (Natural sciences, Economics, Management; in Russian) Samara (3), 103 (2002). 18. M. Jung, F. Bosch, K. Beckert, et al., First observation of bound-state /3-decay, Phys. Rev. Lett. 69 (15), 2164 (1992). 19. F. Bosch, T. Faestermann, J. Friese, et al., Observation of bound-state /?-decay of fully ionized 1 8 7 Re: 1 8 7 Re- 1 8 7 Os cosmochronometry, Phys. Rev. Lett. 77 (26), 5190 (1996). 20. M. Preston, Physics of Nucleus (Moscow, Mir, 1964), pp. 388-403 (in Russian). 21. B.B. Kadomstev, Heavy atom in a superstrong magnetic field, Zh. Exp. Theor. Fiz. (Sov. Phys. JETP) 58 (5), 1765 (1970). 22. B.B. Kadomstev and V.S. Kudryavtsev, The matter in a superstrong magnetic field, Zh. Exp. Teor. Fiz. (Sov. Phys. JETP) 62 (1), 144 (1972). 23. Physical quantities, in I.S. Grigoriev and E.Z. Meilikhov (Eds.), Handbook (Energoatomizdat, Moscow, 1991) (in Russian). 24. Yu.P. Gangrskii, B. Dalkhsuren, and B.N. Markov, The Products of Nuclear Splitting (Energoatomizdat, Moscow, 1986) (in Russian). 25. A.G. Volkovich, A.P. Govorun, A.A. Gulyaev, S.V. Zhukov, V.L. Kuznetsov, A.A. Rukhadze, A.V. Steblevskii, and L.I. Urutskoev, Experimental observation of the distortion of the uranium isotopic relationship and violation of the thorium-234 secular equilibrium upon electric explosion, Bull. Lebedev Phys. Inst. (8), (2002). 26. L.I. Urutskoev, V.I. Liksonov, and V.G. Tsinoev, Observation of transformation of chemical elements during an electric discharge, Ann. Fond. L. de Broglie 27, 701 (2002). 27. G. Lochak, in T.W. Barrett and D.M. Grimes (Ed.), Advanced Electromagnetism (Foundations, Theory and Applications) (World Scientific Publishing Company, Singapore, 1995). 28. G. Lochak, Ann. Fond. L. de Broglie 8 (1983) 345, 9 (1984) 5. International Journal of Theoretical Physics, A. Blaquiere, S. Diner, and G. Lochak (Eds.) (Springer, Wien, NY, 1987). 29. Chernobyl's Reporting (Planeta, Moscow, 1988) (in Russian). 30. A.S. Dyatlov, Chernobyl. As it was (NauchTechlzdat, Moscow, 2000) (in Russian). 31. V.M. Dorovskoi, L.A. Elesin, D.V. Filippov, A.V. Steblevskii, V.L. Stolyarov, and L.I. Urutskoev, Electron microscopy study of the transformation products, Ann. Fond. L. de Broglie (to be published). 32. S.D. Drell, N.M. KroU, M.T. Mueller, S.J. Parke, and M.A. Ruderman, nergy loss if slowly moving magnetic monopoles in matter, Phys. Rev. Lett. 50 (9), 644-649. 33. D. Lynden-Bell and M. Nouri-Zonoz, Classical monopoles: Newton, NTU space, gravitation lens and atom specters, Rev. Modern Phys. 70 (2), 421-445 (1998).
COLD F U S I O N IN T H E C O N T E X T OF A SCIENTIFIC REVOLUTION IN PHYSICS: HISTORY A N D ECONOMIC RAMIFICATIONS
EDWARD LEWIS P.O. Box 2013, Champaign, IL 61825, www.scientificrevolutions.com
USA
Scientific revolutions have occurred in an approximately 80 year periodicity since 1500. Economic depressions have occurred at an approximately 40-50 year periodicity since 1790, and the economic depressions are a result of the scientific revolutions. The field of cold fusion is a part of a scientific revolution in physics. Understanding cold fusion phenomena in the broader historical context is helpful for understanding the development of the field and the significance of the phenomena technologically and economically. This paper includes a short history of science and of the recent scientific revolution, and includes predictions about the economic consequences of the development of the paradigm.
1. Introduction: Seven Paradigm Shifts The cold fusion phenomena are several of a larger group of anomalies in physics. These anomalies are discerned because they are contradictions of the basic ideas of Quantum Mechanics (QM) and Relativity theory. The present development of the field of cold fusion and the elucidation of these anomalies are a part of a scientific revolution in the field of physics. This is not the first time the basic ideas of an established paradigm have been contradicted. There have been similar revolutions in the field of physics of the kind described by Thomas Kuhn every 80 years since 1506 when there was the beginning of the Copernican Revolution. Understanding cold fusion and the CF field in the broader historical context is helpful for understanding the development of the field and the significance of the phenomena technologically and economicly. There have been seven "crisis periods" and "paradigm shifts" in physics since 1500. Kuhn wrote about both of these features in his book. There was such a shift recently. The various kinds of phenomena now collectively termed "cold fusion" are a part of a "crisis period" in physics. In The Structure of Scientific Revolutions, Kuhn 1 described crisis periods as 10 or 20-year periods of time during which the fundamental ideas of an established paradigm are challenged by the discovery of anomalies which are phenomena that contradict the hypotheses. The current revolution is following the pattern of the past revolutions that was described in his book. 854
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Scientific revolutions have occurred in an approximately 80 year periodicity since 1500. All the important theories in physics can be grouped according to the following seven paradigms. The basic beliefs of the founders of the paradigms were more or less the basic ideas of their followers, though there were often small variations among their followers in basic assumptions. Some scientists such as Tycho Brahe and Priestley (b. 1733) stand out as having physical views that can be described as selective combinations of the hypotheses of two paradigms. In Priestley's case, for example, this was a combination of Faraday's and Newton's ideas (Fig. 1).
Scientific revolutions of theory premise formulation (paradigm formulation)
1500
1700
1800
1900
V 2000 O CT>
CD
I
o J9
Figure 1.
Chart of scientific revolutions in physics after 1500.
Since Copernicus was telling people that the Earth revolves around the Sun in 1506, he had to convince people by explaining why they all did not just fall off the round Earth. He explained his own way of thinking which was that everything on the Earth had a proper position to which it strived - the people, the chairs. This striving was called Impetus. So that the reason a person came down to the Earth when he jumped up was because his body strove to go back to its proper position. Likewise for the planets; Copernicus thought that they also strove to maintain their positions. So his explanation for gravity was impetus. Galileo, Kepler and Gilbert taught that the reason we and other things stick to the earth is because of magnetism. They thought that everything was magnetic and that the parts of the earth, the rocks, etc. stuck together magnetically. Gilbert in particular also emphasized that electricity had a role in the Earth's cohesion and in meteorological processes, but among the followers of this paradigm, gravity was mainly thought to be magnetism. In 1590s, Kepler and Galileo corresponded and
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shared ideas, and about 1600, they wrote that they agreed with Gilbert's theory in his book. Newton did not believe this. He talked about a force that he called gravity. He thought that atoms had an intrinsic force called gravity that drew them together. This was his explanation for both the positions of the planets and for why people stuck to the Earth. So Galileo and others with that idea talked about one main magnetic force that kept everything together, and Newton and his followers talked of two forces, gravity and magnetism. Franklin kept Newton's understanding of atoms and their force of gravity, but added the ideas that electricity was a fluid and that heat was a fluid and each of these fluids had certain intrinsic behaviors. So to the two forces discussed by Newton, Franklin added two new forces. A characteristic of these two forces was that they were conserved in systems, and this idea was important for the development of heat and electrical technology during the Industrial Revolution which followed a few decades later. He seems to have thought that magnetism was a fluid also, and Aepinus developed this idea. Faraday did not agree with Newton and Franklin that atoms were hard and compact, but thought that atoms were point atoms. A way to think about this is that he thought that forces around an atom had a point of highest intensity at the center of an atom. He thought of heat as the vibration or motion of atoms, and he thought of electricity and magnetism as being aspects of the lines of force from atoms. He tried to show that gravity could be explained in this way, but was not able to. He wanted to show the interconversion of the known forces, magnetism, electricity, and gravity, and of heat and motion. Maxwell followed up on his work by writing a mathematical theory of fields that was internally consistent. But again, he failed in the area of explaining gravity with these ideas. They had the notion that energy and mass were distinct things. Einstein explained that the mass in atoms changed the time and space around atoms to make them fall together. This was his explanation for gravity. He thought that the entire mass of everything like atoms might convert to energy. This was different than Maxwell and Faraday. He also explained that light and other forms of energy was not just a wave phenomena, but was quantized, somewhat particle-like. But he also could not explain both gravity and the forces with the same general idea. Somewhere along the way, physicists postulated that the entire mass of atoms can't convert entirely to energy, but only a small fraction of the mass could do so. Einstein probably had to intuit this idea even though he believed that mass converts to energy, because atoms and his surroundings seemed stable, and there was no known example of atoms converting to energy in entirety. A new paradigm that is being proposed takes all phenomena to be variations of the same basic thing: plasmoid. Galaxies, stars, atoms and particles are plasmoids of different sizes and kinds. Plasmoids have typical behavior. A broad class of plasmoids has been called ball lightning, and the existence of microscopic plasmoids points to the development of a new atomic physics, with the basic assumption that
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both atoms and atomic processes are plasmodal so that atoms may convert entirely to light or electricity given the right circumstances. Understanding matter this way helps to understand atomic and plasmoid object interactions. However, these assumptions must be tested and experiments done to elucidate plasmoid behaviors, especially concerning time and motion change associated with plasmoid behavior.
2. Broad Overview of the History of Physics' Periodicity After Copernicus conceptualized both a new astronomy and a new physics explaining natural phenomena from a heliocentric standpoint in 1506, there have been revolutions in physics every 80 years: the Galilean, about 1593; the Newtonian, 1664; the Fluid paradigm about 1745 that was originally formulated by Franklin; the Classical Field theory, 1820 that was rudimentarily formulated by Faraday and developed by Maxwell; the Quantum Mechanics and Relativity theories, about 1905; and the Plasmoid theory, about 1992. From 1506 to now, physics developed in an 80 years, three-generation pattern. In Generation 1, individuals formulate a paradigm's basic premise which is comprised of a handful of basic and simple hypotheses which are axioms for the theory. Later generations may reject or modify basic hypotheses, but the basic framework of theories of the same paradigm are recognizably similar. In Generation 2, people who were born about the time when the theory was formulated and learned about the anomalies and perhaps also about the founder's new theory while young continue the development of the theory to the point when it can be said that the theoretical development had matured. An example of this process is Schwinger, Tomonaga, and Freeman's development of QED when they matured in their scientific careers about 1945. They were born about 1905, when Einstein published his seminal papers. In Generation 3, people who grew up learning about the well developed theories as they were growing up invent important technologies that are applicable to experimental research and perform experiments that both support and contradict their own theories of physics. People in this generation also develop technology and invent products that enable industrial revolution. Theoretical formulators like Einstein usually do their basic paradigm formulation work when they are in their 20s. Franklin and Gilbert were older, but as Thomas Kuhn described they were relatively new to the field and inexperienced. Copernicus was born in 1473 and while young he learned about the anomalies and the problems of the established physical theories of his time. In 1506, when he was 33, he started to circulate letters describing his heliocentric ideas. He described a general theory to explain the known phenomena of planetary motion, meteorological phenomena, lodestones and rubbed amber, and the fall of objects. The young people who accepted his ideas developed the Copernican paradigm in the two routes of astronomy and earth-based physics when they reached middle age (about 1546). Some younger theorists, including Rheticus (b. 1514) and Reinhold (b. 1511), focused on studying Copernican astronomy. Both men were impressed by his ideas
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and contributed their best work in their 40s. Rheticus published Narratio Prima, which was about De Revolutionibus, in 1540 when he was 26. In 1551, when he was 40, Reinhold published a set of astronomical tables that were computed by the mathematical methods developed by Copernicus. By the early 1550s, other theoreticians of their generation developed much of the physics of earth motions of that paradigm. For example, Benedetti (b. 1530) developed a physics of motion on the earth and statics according to Copernican-type ideas. He published Demonstratio in 1554. So about 40 years after the inception of the Copernican paradigm, Copernican theory was well developed in its two major fields. Consistently, over the past 500 years, the time between formulation of the basic hypotheses of a premise and the general physics theory's development has been 40 years. About another 20 years is required before a crisis period begins, and then about another 20 before the time of the next theoretical formulation. Men of the next generation performed the important experiments that tested the theory. Most of these men were Copernicans, though one of these men, Tycho Brahe (b. 1546), was not a Copernican. He espoused a theory that was a mixture of Copernican ideas and earlier ideas. His theory could be regarded as a mixture of two or more sets of postulates. Brahe used the tables that Reinhold published as a guide or template for testing Copernicus's theory to discern several important anomalies, such as the extra-lunar orbit of comets and the incorrect predictions about planetary motion. Simon Stevin (b. 1548) believed and taught Copernican theory and verified Benedetti's prediction that objects of the same substance but of different weights would fall at the same rate in vacuum. Sarpi (b. 1552), along with many others who in the late 1500s accepted Copernican ideas, believed that the earth was a magnet, based on their study of magnets and the discovery of the magnetic dip by Norman (date of birth unknown) as described in 1581 in The New Attractive and by Georg Hartmann (b. 1489). They understood that magnetism originated in the earth, that the earth drew objects, and that the reason for the orientation of compasses was not extraterrestrial. These ideas contradicted Copernicus's idea of impetus. There was thus a crisis period in physics during the late 1500s, extending from about 1575 to 1795. In the late 1500s, Gilbert, Galileo, and Kepler formulated similar sets of hypotheses based on the experimental work of the preceding generation of experimenters. Galileo and Kepler were enthusiastic about Gilbert's theory when they read the De Magnete, which was published in 1600. Gilbert (b. 1544) formulated his premise in about 1582. In the preface to the De Magnete, Edmund Wright wrote that Gilbert had held back his magnetic philosophy for almost 18 years. Gilbert postulated what he called magnetic form and electrical effluvia. In 1589, at age 25, Galileo (b. 1564) formulated his first postulates of motion. He laid a foundation of a physics of motion of that time, but Descartes and others completed this theory. Later, after a series of experiments, he believed that objects tended to remain in their state of motion. But initially, people who formulated this paradigm believed that objects had a tendency to rest.
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Kepler (b. 1571) attended the University of Tubingen where Maestlin, who taught a theory similar to Copernicus's, taught and performed experiments. Around the year 1595, Kepler formulated a heliocentric theory for astronomy. Later, he understood that the planets follow elliptical orbits. There is evidence that he hypothesized that planets had a tendency to rest about 1604 or 1605.2 He thought that objects on the earth had a tendency to rest as well. By 1600 he thought that the sun emanated a magnetic vigor that caused the planetary rotations. He idealized outside force, the tendency of bodies to rest, and fall as a magnetic phenomenon. Those of the next generation who developed similar theories of this genre include Gassendi (b. 1592), Mersenne (b. 1588), Desargues (b. 1591), Descartes (b. 1596), Roberval (b. 1602), Etienne Pascal (b. 1588), Castelli (b. 1578), and Cavalieri (b. 1598). They defined gravity as magnetic effluvia or form, or electric effluvia, or as a vortex of particles. Descartes developed a highly influential philosophical physics that was nearly impossible to test and published his ideas in the early 1640s. Experimenters of the next generation such as Torricelli (b. 1606), Boyle (b. 1627), Hooke (b. 1635), Von Guericke (b. 1602), and Blaise Pascal (b. 1623) found some important anomalies during the crisis period of 1640-1664. Von Guericke put Descartes' "plenist" theory, which denied the existence of the vacuum, to the test. He devised and constructed various models of pumps to produce a vacuum. The anomalies to the early paradigm that were discovered, such as the property of the vacuum and that sound did not travel through a vacuum, were important for Newton's formulation of new hypotheses about the nature of matter and motion. Their contemporaries in the mid-1600s, such as Borelli (b. 1608) and Huygens (b. 1629), tried to comprehend the anomalies according to the older GalileoDescartes paradigm that they already accepted, but it was Newton who formulated the set of postulates for the next paradigm. But the development of theories of this earlier genre did not end with Newton. In Continental Europe, scientists such as Leibniz, the Bernoullis, Euler, Nollet, and Dufay continued development of ideas based on theories similar to those of Galileo and Descartes. These theorists described gravity, electricity, and magnetism as vortices, the mechanical motion of tiny invisible objects, following Descrates. Most educated Continental Europeans accepted a theory of this genre until the mid-1700s, but the Newtonian paradigm was accepted mainly in Britain. There was a similar divergence in thinking in the mid-1800s among theoreticians in Britain and the Continent as is described in this article. In 1664, at the age of 22, Newton (b. 1642) formulated the basic premise of his theory. He attempted to lay a uniform theoretical foundation for the whole of known phenomena. His work proved successful for mechanics and gravitation. After 1664, there followed a two-generation process that required about 80 years to complete. People of the next generation who developed the theories of the paradigm include Boerhaave (b. 1668), Hauksbee (b. 1666), Gravesande (b. 1688), Stephen Gray (b. 1666), and Desaguliers (b. 1683). When they reached middle age in the early 1700s, they taught others who verified predictions of Newtonian theory or
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found anomalies in this paradigm. Boerhaave was born in the Netherlands. He was born about the time that Newton first formulated his theory. He learned about the important experiments of Hooke and Boyle, and believed Newton's basic ideas. Like Newton, he thought that light was corpuscular and that the corpuscles of light were different sizes. During the crisis period of 1725-1745, Martine (b. 1702), Van Musschenbroek (b. 1692), and Von Kleist (b. 1700) made discoveries of electrical and heat anomalies that led to Franklin's fundamental theoretical formulation. George Martine showed experimental anomalies of the Newtonian premise concerning heat. In 1745 and 1746, Von Kleist and Van Musschenbroek independently produced the anomalous Leyden jar to store electricity generated from Hauksbee-type machines. Some of the researchers were Newtonians and others accepted the earlier paradigm. When he formulated is premise in the middle of the 1700s, Franklin (b. 1706) was among the oldest of the formulators of premises. He may have been as old as 39-years old when he formulated his theory. According to Constraint I described later, he was able to formulate a novel premise because he was inexperienced and had not apprehended an earlier general theory when he understood the anomalies. Kuhn wrote the same thing about Franklin in his book. Sometime about 1745, maybe even before he learned about the Leyden jar in 1745, Franklin originated novel hypotheses about what he called the "matter of heat" and the "matter of electricity." Before the year 1745, he conducted scientific research on heat and the effect of the sun on warming different color materials and also invented an efficient kind of furnace design that was called the Franklin stove that he wrote was 50 or 66% more efficient of firewood. Because of this earlier, innovative work on heat, it is. uncertain when he had developed this general premise. The fourth paradigm was developed and contradicted by the next two generations. The ideas about the particulate nature of the fluid of heat and about their mutual repulsion, tendency to reach equilibrium in matter, and the permeability of matter to this fluid is the basic caloric theory that Lavoisier, Cleghorn, and other scientists of the second generation espoused. Caloric is the French term for the fluid of heat. He postulated that atoms had an affinity for the particles of heat. The ideas in his description of the basic chemistry involved in the evaporation of salt-water were the basis for caloric chemistry. Franklin's ideas on the indestructibility of the particles of electricity and heat meant that these fluids were conserved in systems, which is the basis for the conception of latent and specific heats. The properties of these hypothetical fluids to flow and to reach equilibrium in bodies are the basic ideas behind the innovations in steam engine technology by Watt and others, and some writers like Cardwell have emphasized how the caloric theory of heat was very different in basic concepts from Boerhaave's theory of heat. Aepinus (b. 1724) was among the first of the second generation physicists to help develop the paradigm to its full form. He began the theoretical development work of describing the new theory mathematically near the time of his middle-age. In this work he proposed primarily a theory of magnetism that held postulates
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very similar to the postulates of Franklin's electrical theory. In fact, he listed his postulates one by one and showed how each one matched a postulate of Franklin's premise. Coulomb (b. 1736), LaPlace (b. 1749), Hauy (b. 1743), Lavoisier, and many other French people who apprehended a theory similar to Franklin's began to perform electrical, magnetic, chemical and heat experiments and develop the premise of the paradigm further. Gay-Lussac, Biot (b. 1774), Carnot, Ampere (b. 1775), Savant (b. 1791), Arago (b. 1786), Berthollet, Poisson (b. 1781), and Fourier (b. 1768) were among the scientists of the third generation who accepted and extended the new paradigm. Thomas Young verified Franklin's description of light as a wave during the period 1801-1804. When the third generation scientists learned about the electromagnetic effect and Faraday's experiments, they began to change their physics of fluids to fit the evidence. Meanwhile, others of their generation, notably Davy (b. 1778), Thompson (b. 1753), and Oersted began to discover major anomalies in the crisis period that started about 1800 and lasted until about 1820. Davy hypothesized that atoms were point atoms. Both Davy and Benjamin Thompson hypothesized that a body's heat was due to the motion of its particles and tested this idea experimentally. Then in 1820, Oersted (b. 1777) startled the world by discovering the electromagnetic effect. Scientists had sought for a relationship for decades. Davy and Thompson formed the Royal Institution where Faraday was hired and worked for Davy when he was very young. There they taught their new hypotheses about point atoms and heat to Faraday. When in 1820 he learned about the electromagnetic effect, he understood both electricity and magnetism as properties of an idealized kind of phenomena he called lines of force, understood atoms as point-atoms, and heat as the motion of the point-atoms. He formulated the basic postulates of his theory in 1820. His new understanding enabled him to invent two of the important technologies of the 19th and 20th centuries, the electric motor and the electric generator. He wrote the fundamental laws of electrochemistry. As he experimented with metals according to his theory of point atoms, he invented several types of industrially important steel alloys, and laid the basis of scientific metallurgy. His new conception enabled him to conceive how forces propagate and how material is organized, so that he could conceive and produce electromagnetic devices, invent important industrial steel alloys, chemicals, organic chemicals such as benzene, and several kinds of glass. People who accepted his theory when they were young included Maxwell and perhaps Thomson (b. 1824). Maxwell developed the Field theory when he matured, about 1864, 44 years after the initial formulation by Faraday. Because of Limitation 2, the theorists did not test their theories by themselves or develop most of their new inventions to the point that they started important industries. The men and women of the third generation started to introduce the economically important new inventions and to discover major anomalies around 1880. Some of them were Curie, Alexander Bell, Thomas Edison, Lenard, Thomson, and Michelson.
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In 1905, Einstein laid the basis for both the theories of Quantum Mechanics (QM) and Relativity. His basic framework of hypotheses included the concept of quanta of energy; mass-energy equivalence; his concepts on time, space, gravity, mass, and inertia; and other basic concepts of early 20th century physics. Einstein is recognized as being the first to think of quanta of radiation as something real, not just a mathematically useful construct. Because of Limitation 1 described later, those of the next generation developed his ideas when they were in their 30s and 40s. Some of these people were Bohr (b. 1885), de Broglie (b. 1892), Dirac (b. 1902), Heisenberg (b. 1901), Pauli (b. 1900), and Schrodinger (b. 1887). Schrodinger and de Broglie developed a premise for physics that differed from that premise developed by those of the Heisenberg school. The QM was almost fully developed in 1948 through the work of Tomonaga (b. 1906), Schwinger (b. 1918), and other physicists who developed QED theory. Because of Limitation 2, the theoreticians who developed the theories could not produce new industries and economically important inventions or disprove their own theories by experimentally finding major anomalies. It was mainly middle-aged experimenters born about the time of the development of the paradigm in the 1940s who validated important experimental predictions and ideas of the Einstein paradigm and contradicted it. During the crisis period of the 1970s and 1980s, they used newly invented technologies based on QM theory such as atomic clocks, lasers, and various types of electronic microscopes. In conclusion, it seems that in the history of science we may find these general principles that were described by Kuhn: (1) that scientists who accept a general paradigm never become fluently functional in developing a new paradigm and (2) that the best experimental physicists who find major anomalies are not in the forefront of the theoretical development of a paradigm. A theory can be constructed using these that the development of a paradigm in physics is a three-generation process working through two constraints.
3. General History of the Recent Crisis Period Since the 1970s, experimental physicists who work according to quantum mechanics have been discovering anomalies to quantum mechanics. There are ball lightning, cavitation and sonoluminescence phenomena, water memory, superconductivity, and astrophysical anomalies. Some of the leaders of this research have been Andre Lipson (b. 1956), Pons and Fleischmann, Matsumoto, Ken Shoulders, and Deryaguin. Atoms show anomalous changeability and motion. They show the anomalous ability to not only fuse and break up at slight changes in condition, but also anomalous relative motion, so that atoms in solids move around as if they are transparent to each other or as if they are a fluid or a gas. What is happening is that the atoms change state from what has been regarded as their normal stable state in a solid or fluid or gas, and behave like BL. This is why atoms may pass through each other and move around as if in fluid flow.
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In 1992, it was apparent that BL-like objects were emitted from CF experiments. It was hypothesized that materials converted to microscopic BL in electrodes used for CF research and that these caused the markings in the plastic sheets found by Matsumoto. Matsumoto read this idea, and started researching the relationship between BL and CF. In 1992, the structure of BL was speculated to be an example of the structure of atoms, and research was begun to determine whether all phenomena including astrophysical and meteorological phenomena are the same thing, called "plasmoids," the term used by Winston Bostick. It was determined that tornadoes and ball lighting can be identified as kinds of the same basic phenomena, and this supported the assumption that weather could be described in terms of plasmoid behavior. In 1996, while performing microscopic investigation of Miley's Run # 8 , a researcher found markings like those of microscopic BL. The "strange" radiations reported by Urutskoev leave markings on detectors much like the BL reported by Matsumoto. These objects can be classified as a kind of microscopic BL. In nature, BL and whirlwinds may leave ditches or areas of discoloration on the ground. A series of international BL conferences started in 1986. Egely researched the excess energy and anomalous properties of natural BL. Dijhkuis researched radioactivity and particle emission from BL, and conducted experiments on BL-like discharge objects. Egon Bach's UFO's from the Volcanoes provides evidence of BL generation during geological process. In the late 1990s, the BL and CF fields merged in Russia. At the last international conference on BL in St. Louis in 2001, George Miley and Dan Chicea sent abstracts, and microscopic BL in CF was a scheduled topic of discussion and lecture. In 1983, Lipson suspected the acceleration of deuterons by the electric fields in cracks generated by the fracture of deuterated dielectric crystals such as LiD. He published about this in 1986 in the journal Soviet Physics Technical Physics. According to Lipson3 this work followed the discovery of X-ray emission during mechanical fracture, which followed Deryaguin's discovery of fast electron emission from fractured solids in 1953. In the early 1990s, Lipson began research on neutron emission from HTSCs, and discovered the effect that the superconducting phase transition coincided with neutron emission. In 1996 he suspected that palladium and other materials may contain cores with high hydrogen density and superconducting properties even at high temperatures, and CF reactions due to high energy phonons and phase transitions. Both HTSC work and CF started about the same time, so both Celani and Lipson and his group were prepared to start research on the relationship simulteanously. Mueller (b. 1927, same as Fleischmann) and Bednorz (b. 1950) discovered superconductivity of 33 K in a layered, ceramic material. Recently, working with Carlos Castano and others working with George Miley, Lipson has shown that a hydrogen cycled PdH x [x = 4.0 x 10~4) single crystal showed evidence of superconductivity below 30 K. They suspect finding minute amounts of the diamagnetic phase of condensed hydrogen or superstoichiometric hydride ( I > 1 ) inside the dislocation nanotubes, a quasi-metallic metastable hydrogen phase at room temperature,
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like that predicted recently by Ashcroft. By using small-angle neutron scattering (SANS), Heuser discovered that dislocation cores caused by H2 gas cycling Pd films are sites of high hydrogen absorption and concentration. The two fields are merging. Fleischmann (b. 1927) and Pons (b. 1943) began research on the fusion of atoms in metal electrodes in 1986. They had known about prior research in this area dating from early in the century such as the work of Bridgman in the 1930s, and Fleischmann followed up on certain anomalous phenomena he had observed in the course of this research as an experimental chemist. In 1960s, Deryaguin (b. 1902) and others started a controversy about the strange properties of water. They said that water had polymer-like qualities, and used the word "Polywater." He claimed this water had been discovered by another Soviet scientist, N. N. Fedyakin. Much like CF, most scientists around the world did not accept the existence of this anomaly. But lately, like CF, the subject is again gaining in general popularity, as shown by Josephson's recent lectures. Lipson studied the association of cavitation and cold fusion in the early 1990s. In the 1950s, Winston Bostick researched plasmoids that were emitted from electrodes during discharge. He wrote important and widely read articles on this topic, such as the article called "Plasmoids" that was published in Scientific American4 • Some astronomers adopted this way of looking at the universe and researched the astrophysical objects as plasmoids. It was known early on that electrical discharges to produce plasmoids were associated with a low level of deuterium fusion reactions, and in the 1960s this topic and the topic of exploding wires in general were studied by researchers for the militaries of the US and USSR. Ken Shoulders studied the plasmoids and determined a number of anomalous phenomena associated with them, such as their high energy density, life-span, method of production, and their effects in interaction with materials. Shoulders wrote that he and Bostick had a working relationship, and that he (Shoulders) determined that plasmoids contain smaller things he called by various names such as EVs, NEVs and charged clusters. The objects behave like BL in many ways. It is evident that there is no longer a reason to think of matter and energy in terms of nuclei bound together in the center of atoms, since it is obvious that BLlike phenomena are compact and like matter in many ways, and yet may convert entirely to electricity and light, as far as it is known. The microscopic BL produced by Matsumoto passed through materials to reach the plastic sheets, as did those produced by Savvatimova. At the basic level of analysis, the structure of plasmoids may be thought of as energy, since some BL converts entirely to electricity and light. This paradigm is unlike QM that describes that certain basic particles are basically inert, "hadrons," and gravity and light by distinct hypotheses. What needs to be researched further is the relationship between the presence of BL-like plasmoids and atomic reactions and time.
865 4. P a r a d i g m C h a n g e a n d Economic R e s u l t s Paradigm changes in physics have led to similar patterns of productivity growth, industrial revolutions, and economic depressions. The productivity grew at an 80 years periodicity in the most advanced industrial economies, with productivity growth lows during the industrial revolutions and productivity growth increasing (accelerating) the fastest about 30 years after the dips in the 1820s and 1830s and the 1920s and the 1930s. During these "technological acceleration" times there were major economic depressions in the most technologically advanced economies, and another depression would be expected in the next few years if the past pattern holds. During the industrial revolutions, there were less severe depressions or recessions in the most advanced economies. The past pattern helps us to understand how the new science will impact technology and economics (Fig. 2). c q
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Figure 2. The three industrial revolutions resulted in an 80-year periodicity of productivity growth in the United States. Growth dips happened around 1800, 1895, and 1975. Growth accelerations started in 1830, 1920, and 2000. The growth accelerations were associated with technological acceleration depressions. The growth dips were associated with industrial revolution depressions. Statistics for this chart come from Paul Romer 5 , 6 and estimates for productivity growth after 1980. Paul Romer's chart in the working paper shows a gradually increasing trend of per capita GDP from 1800 onward until after 1830.
Recently published statistics on the productivity acceleration in Britain show that at the beginning of the 1st Industrial Revolution, 1760-1830, output per capita grew 0.5% per year on average.7 By comparison, per capita output increased at an average rate of nearly 2% per year from 1830 to 1870. As Crafts wrote, 8 the acceleration of growth of output in Britain from the late 1700s until about 1820 was a gradual process. But in the 1820s and afterward, Britain achieved growth in real
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output of 2% per year. Romer's graphs showed a jump in American productivity starting about 1840, rapid acceleration around 1850, and a dip lasting from about 1890 to 1905. Jesus willing, once a generation of researchers who are now teenagers who were born sometime about 1992 reach their middle age, the most productive time of their careers, they will help to complete the development of the new paradigm. This would be sometime about 2032. By then, there may be practical and profitable manufacture of plasmoid-type equipment. It is not possible to know when most scientists will accept the plasmoid theory. But if the past pattern continues, it will not be until the third generation of people who accept the new paradigm matures sometime about 2052 that the important industries of the paradigm will begin. The maturation of experimental scientists and the availability of technology designed according to the principles of the new paradigm will lead to the discovery of basic anomalies to the theory; and around 2072, when a young or inexperienced person might understand the anomalies in a new way, there will be the eighth scientific revolution, Jesus willing. If the past pattern plays out, there may be an industrial revolution depression about 2062 because of the combined effects of the depletion of the technological potential of the QM paradigm, the small size of the highly productive Plasmoid theory industries, trade competition against the most advanced economies due to the trade competition from follower countries that will have the chance to catch up because of the lack of innovation in the mature industries, and the transfer of labor and resources from the old to the new industries. All of these played a role in the depressionary periods in the advanced economies in 1900 and 1980. There may be another depression associated with this new science about 2102. During the times of technological acceleration in the dominant industries of advanced economies, there have been severe depressionary periods. In Great Britain, this depressionary period lasted about 20 years or so, from about the late 1820s to 1844s. Since the US was catching up technologically, the depression was less severe, and much shorter, and happened mainly during the 1840s. However, when the US was technological leader during the 1930s, there was an 11-year or 12-year long depression period that only ended with American entry into the World War. By comparison, Britain's depressionary period in the 1930s was less severe, because it was the technological follower in that paradigm. In Technological Acceleration and the Great Depression, Waters 9 explained how the increase of the rate of technical progress from 1% per year to 2% per year during the 1920s, figures he obtained from widely accepted prior research, led to the conditions of the 1920s and the 1930s of high investment and high and increasing business and consumer debt, and the shift to higher consumption due to the availability of new products. He thought that the connection between productivity growth and the Great Depression was mainly the financial consequences of what he called a "technological acceleration". But the labor displacement and unemployment due to automation and the labor efficiencies arising from the establishment
867 of oligopolies in each of the industries probably played the major role. This drop in labor employment meant a shift in consumption and non-payment of debt. T h e decrease of introduction of new kinds of products in the late 1920s and the 1930s meant a decrease in consumption as well, since once people had acquired the standard products of the times, such as automobiles or radios, they had satiated their demand somewhat.
5.
Conclusion
T h e past p a t t e r n of history shows t h a t the field of cold fusion is a p a r t of a scientific revolution in physics, and t h a t most of the major inventions of this paradigm may only h a p p e n after about 40 more years, and the IR may be associated with an economic depression. T h e theory of this paradigm may be well developed about 2032 when the younger generation of theorists m a t u r e . T h e "technological acceleration" periods and the industrial revolution periods have been the economic depressionary troughs in the most advanced economies. T h e p a t t e r n of scientific and industrial revolution is the cause of the Kondratiev p a t t e r n of economic depressions. During the last few years, the fields of cold fusion, superconductivity, ball lightning, and cavitation have been merging. Simple hypotheses for a new paradigm have been formulated, b u t there is a need for tests and the experimental determination of relationships.
References 1. T. Kuhn, The Structure of Scientific Revolutions (Chicago, University of Chicago Press, 1970). 2. M. Casper, Kepler, C D . Hellman, Trans, and Ed. (London, Abelard-Schuman, 1959). 3. Andre Lipson, personal conversation, January 2005. 4. W. Bostick, "Plasmoids," Scientific Am. 197, 87 (1957). 5. P. Romer, Increasing Returns and Long Run Growth, manuscript article, 1985. 6. P. Romer, "Capital accumulation in the theory of long-run growth," in R.J. Barro, ed., Modern Business Cycle Theory (Cambridge, Harvard University Press, 1989). 7. K. Kliesen and D. Wheelock, "Heavyweights of productivity: does the microchip match up?" Reg. Econ. 1, 4-9 (2001). 8. N. Crafts, British Economic Growth During the Industrial Revolution (New York, Oxford University Press, 1985). 9. J. Waters, Technological Acceleration and the Great Depression (New York, Arno Press, 1977).
T H E NUCLEOVOLTAIC CELL
DAVID D. MOON Minneapolis, MN, USA
Described in this paper is a cold fusion device that is conceptually designed to convert the energy release, from deuteron to deuteron fusion, directly to electricity at an efficiency worthy of commercial development. The working element is an N-type semiconductor, which has been coated with a thin film (a few 100 A) of hydrogen-active metal, e.g., palladium, and which is joined to a P-type semiconductor at the PN-junction. The working element is not an "electrode," as such, but an "electron pump." During operation, deuterium gas is absorbed into the interface between the thin metallic layer and the N-type semiconductor. Excess electrical energy and voltage result from the d + d fusion reaction, as electrons in the N-type semiconductor are promoted to higher energy from the valence band to the conduction band. This new phenomenon of converting nuclear energy directly to electricity is termed "the nucleo-electric effect." The electronic schematic of a possible commercial nucleovoltaic cell is shown on the next page. Of course, the first proof-of-concept experiments will emphasize fabrication and design of the semi-conductors used in the cell core. 1. Cell Design Pressure-strong inner vessel (1) contains D2 (or H2) gas. A P-type semiconductor (2) has an NP-j unction (3) with the N-type semiconductor (4) that has been coated with a thin film of hydrogen-active metal (e.g., Pd, Ti, or Ni). Electrical contacts (5) connect the semiconductors to the external load (6) as well as to a rechargeable battery or energizer (7), in series with two-ohm resistors (8,9), and a parallel circuit consisting of a heating coil (10). Deuterium or hydrogen gas is admitted to the evacuated vessel (1) through valve (11). The gas pressure will be made above atmospheric. During the startup phase of cell operation, the internal switch (12) is closed, while the external switch (13) is open. The energizer (7) provides a forward-biased voltage across the NP-j unction (3) greater than the contact potential set up in the reverse direction (P-N). A certain current is generated through the energizer circuit - from point A-N to P-B, and is limited by the total resistance, R7 + R8 + RNP + R9. A larger current is passing through the solenoid, which is intended to heat the hydrogen gas (to help gas absorption into the N-type) and create magnetic lines of 868
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force along the NP-core, which will assist alignment of deuteron or proton chains. (Chains of deuterons or protons are the "reacting species" in my cold fusion theory, called Mechanisms of a Disobedient Science - see Infinite Energy, 28, 1999.) During startup, a PN-type rectifier (14) assures electron flow in the direction indicated, avoiding any "electron backup" going from N to D to B. Also, during this phase, parameters of gas temperature and pressure will have to be made sufficient to enable D or H to absorb into the interface between the thin metallic film and surface of the N-type semiconductor. There, deuteron-deuteron fusions (or protonproton-electron fusions) energize electrons in the N-type, driving them across the junction to fill electron holes in the P-type. Thus, the N-type becomes more and more positively charged and the P-type more negatively charged.
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2. Cell Output Phase As fusion reactions occur during the startup phase, eventually voltage across NP (where P is negative and N is positive) increases until V (at C) > V (at A). At point C, electron current divides, with some e~ flow going to point A, and, when switch (13) is closed, to the external negative terminal (15) fitted on the outer housing (16), then through load (6) to the positive terminal (17) of the device. Concerning the internal circuit during the cell output phase, electron flow from C to A will divide into three parallel branches at point A: from A through R8 to N,
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from A through solenoid to B through R14 to D to N, and from A through R7 to B to R14 to D then to N. The latter is the recharging cycle for the battery or energizer (7). Resistor (8) is needed in the circuit to limit a "bleeding off" of electrons from P to C to A to N, allowing more current to pass from A to R7 to B to D to N. Also during operation, current through the solenoid branch, i.e., from P to C to A through coil to B to R14 to D to N, is now limited by R14. During cell operation, some excess heat undoubtedly will come from the fusion reactions (i.e., not 100% conversion to electricity) so less electron flow through the heating coil is desired. One additional circuit is noted during cell output: from P to R9 to B, then through R14 to D to N. I believe resistor (9) is needed to guarantee a voltage drop from P to B, so that V (at B) is less than V (at A) - a necessary condition for proper electron flow through the internal circuits during cell output phase. If it happens that reactions in the N-type semiconductor fall below the minimum operational rate, then V (at C) becomes less than V (at A), and battery (7) re-energizes the cell. Choosing the correct components for the Nucleovoltaic cell, including the best ohm rating for resistors (8) and (9), can lead to a reliable, a rugged, self-sustaining and long-lasting source of direct current for many applications.
i n d i v i d u a l cells might produce varying direct current, but cells in combination should generate a steady current, and current of increased amperage.
I N T R O D U C I N G T H E BOOK "COLD F U S I O N A N D T H E F U T U R E "
JED ROTHWELL
"Cold Fusion and the Future" is the title of a new book by this author. In December 2004, it was uploaded and distributed for free on our web site, LENR-CANR.org. This paper discusses a few of the topics in the book. 1. The Ideal Source of Energy Cold fusion has been called the ideal source of energy: it does not pollute; the fuel is inexhaustible; it is potentially thousands of times cheaper than conventional energy. Cold fusion reactors will be compact and lightweight, like gasoline engines, because they do not require heavy shielding. Like all nuclear power, the energy density is roughly a million times greater than gasoline or other chemical fuel. Cold fusion has such a remarkable list of advantages, people feel it must be "too good to be true." But putting aside theoretical objections, strictly from an engineering point of view, it has no unique virtues. Every advantage in Table 1 is shared by other energy sources. Cold fusion is desirable because it has all of these advantages bundled together in one single energy source. (1) Fission reactors produce no pollution during operation, but uranium mining does, and the disposal of radioactive waste (radwaste) and spent fuel are serious and expensive problems. High level radwaste and spent fuel might be used in a terrorist attack. (2) According to a Los Alamos study, plasma fusion reactors would produce about the same amount of nuclear waste that conventional, present-day fission reactors do, they would not be commercially competitive with advanced fission reactors, and they would not have significant environmental, safety and health (ES&H) advantages over advanced fission. Krakowski et al, Lessons Learned from the Tokamak Advanced Reactor Innovation and Evaluation Study (ARIES), Los Alamos National Laboratory and U.S. Department of Energy, Office of Fusion Energy (3) Fission reactors are located far from cities because there is some risk they will fail catastrophically, and plasma fusion reactors would probably produce large amounts of dangerous radwaste, so it would not be prudent to locate them near population centers. (4) "Works 24/7" means the energy source is available on demand, and it is available at night, unlike solar energy. Solar or wind energy might converted 871
872 Table 1.
Pollution free Fossil fuel Hydroelectric Wind Solar Uranium fission Plasma fusion Cold fusion
Very safe
Comparison chart for different energy sources.
Inexhaustible
Unlimited
Low fuel cost
Low reactor cost
Compact
Locate anywhere
Works (4)
Ready now
Y
Y
Y
Y
Y
Y
Y
Y Y Y Y
Y
Y
Y
Y
Y Y (1)
Y Y
Y Y Y
Y
Y Y Y
Y
(3)
Y
Y
Y
Y
Y
(3)
Y
Y
Y
Y
Y
Y
Y
(2) Y
Y
Y
to hydrogen and stored for times when they are not available, but this would increase cost. Hydroelectric power has to be reduced during droughts. Any energy system must be turned off periodically for maintenance. One aspect of cold fusion may seem impossible to members of the public: it is an intense nuclear power source, yet it does not produce dangerous radiation. Plutonium-238 nuclear fuel is similar. Like cold fusion, it emits alpha particles that can be easily shielded. Figure 1 shows a NASA radioisotope thermoelectric generator. A conventional nuclear reactor requires heavy shielding; if this were a fission or hot fusion reactor, the woman in the photo would be killed. Commercial plutonium-238 pacemaker batteries have been implanted in patients. They last 1020 years. Obviously, this relatively benign isotope does not reduce the overall risk from radioactive materials; it merely leaves the dangerous materials behind, to be dealt with later. Cold fusion will create no dangerous radioactive material, and when the cold fusion reaction stops, and the alpha emissions will stop.
2. The Transition from Fossil Fuel will be Rapid A few cold fusion cells have achieved temperatures and power density that would suitable for nearly any practical purpose. Mizuno's 1991 cell was a dramatic example. 1 It produced palpable heat after death at over 100 W initially. It did not boil because it was pressurized. Fleischmann and Pons demonstrated boiling cells that ran continuously for months. 2 Mizuno's cell was disconnected from the power supply and placed in a bucket of water to cool. The next day the water in the bucket had evaporated, so it was replenished, and it evaporated again. Altogether the cell evaporated 37.51 of water over an 11-day period before finally cooling down, which requires at least 84 MJ in principle, and much more in practice because the bucket was not insulated and the cell was left exposed to air for hours at a time.
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X RTG Mounting ' „.,. „ Midspan heat flange Multi-foil Silicon-Germanium source support insulation (Si-Ge) unicouple
Figure 1. The NASA cassini mission general purpose heat source radioisotope thermoelectric generator (GPHS-RTG).
Once the mechanism is understood, we should be able to make any cell do what Mizuno's cell did - only we will have complete on/off control. If something can happen once in one laboratory, even by accident, eventually we ought to be able to make it happen on demand. From that point on, commercial development should be straightforward. From 1948 to 1952, transistors existed only as rare, delicate, expensive laboratory devices that were very difficult to replicate. One scientist recalled that, "in the very early days the performance of a transistor was apt to
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change if someone slammed a door." 3 By 1955, millions of transistors were in use, and any of these later mass produced devices was far more reliable than the best laboratory prototype of 1952. Mass-produced cold fusion cells should cost roughly as much as today's batteries. The materials will be inexpensive, unless platinum group metals are needed. Production lines may resemble those used to make batteries; the extraordinary, expensive, clean room standards of a semiconductor production line should not be necessary. Mizuno's cell was made by hand in a room with normal levels of contamination, yet it generated commercially useful levels of heat. Thousands of corporations have the capital and expertise to manufacture things like batteries, and many of them will compete to make cold fusion devices, quickly driving down prices. Cold fusion appears to be safe. No significant ionizing radiation has been detected. Researchers exposed to working cells have not suffered from adverse effects. Because the fuel cost will be virtually zero, and assuming the devices will be inexpensive and safe, cold fusion will rapidly supplant all conventional energy sources. After the effect becomes fully reproducible and controllable, engineering development will begin. It will be a few years before production lines are set up. In the meanwhile, regulatory, health and safety agencies will make sure the devices are safe. Small machines are easier to develop and cheaper to manufacture than big machines, so the small ones will come first: water heaters, space heaters, small heat engines for pumps, and rugged, simple thermal refrigerators and air-conditioners. NASA, the military, and the telephone companies will be quick to develop cold fusion thermoelectric generators for critical applications in hard-to-reach places. Ten years after the first commercial devices, cold fusion powered automobiles should become available, along with the small electric power co-generator, suitable for houses or apartments. Toyota and Honda took about 5 years to design and begin selling hybrid gasoline automobiles. Large and complex machines such as aerospace engines will take much longer to redesign. However, in the aggregate, small, shortlived machines consume more energy than the big ones do. When most automobiles and water heaters use cold fusion, it will have captured most of the energy market. The very first commercial cold fusion water heaters will be expensive novelties. But the tank, the insulation and most other components will be the same as in a gasfired heater. Based on the power density of the Mizuno cell, a cold fusion cell should have high enough power density to fit in where the gas burners are now located. To reiterate, because Mizuno's cell did not require extraordinary manufacturing techniques, we can predict the cell will be reasonably cheap, around $100. After a few years, competition will drive the cost of the whole water heater down to $300, the same as gas or electric models. The transition away from fossil fuels will occur in the time it takes for all water heaters, automobiles and air-conditions to wear out and be replaced, which is about 15 years. This is how long it took to go from minicomputers to microcomputers, and from black and white television to color television. Market forces will accelerate
875
the last stages of the transition. After about a third of the automobiles on the road have been replaced by cold fusion models most gas stations will go out of business, and it will become increasingly difficult to operate a gasoline powered model. The holdout motorists will be forced to replace the rest of the fleet prematurely, before it wears out. Similarly, when half the people in your city have home generators, the electric power company will go out of business, forcing everyone else to buy home generators. 3. Revolutionary Technology The first cold fusion commercial products will be ordinary, small machines: pumps, motors, electric lights, cooking stoves, refrigerators. People in first world nations already have these small machines in abundance, but a third of the human race - two billion people - does not have enough of them, and this causes appalling human suffering and ecological damage. If cold fusion only succeeds in bringing 19th century Western levels of sanitation and illumination to the rest of humanity, it will be the most revolutionary and beneficial breakthrough in history. But it will probably accomplish far more than that. It will usher in revolutionary technology. One obvious application for cold fusion is already performed with fossil fuel and nuclear fission: desalination, the production of fresh drinking water from ocean water. It is widely used in arid places such as Los Angeles and Saudi Arabia. Worldwide, roughly 5-10 km 3 of drinking water is produced every year. This is done with fossil fuel, and in one case with fission. Desalinated water is cheap enough to drink, but too expensive for irrigation. Energy is a major cost component. Efficiency is much improved in modern designs, but the point is, energy is still the limiting factor to production, and it still dictates the design of the plants. The total amount of water we could extract from the ocean is limited by the amount of energy we can produce, and by the pollution that energy would cause. Modern desalination plants use reverse osmosis (RO). The technique is expensive but energy efficient. With cold fusion it would be better to revert to an older method, multi-stage flash (MSF), in which you boil the water and collect the distillate. This takes 4-30 times more energy, but with cold fusion that will not matter. The MSF has other advantages: it is rugged, simple, easier to maintain, the equipment costs less, and it removes more of the salt from the water. 4 The goal would be to eradicate food shortages, supply millions of people with drinking water, and reverse global warming, with a profitable, self-sustaining development project. We accomplish all this by irrigating a third of the Sahara and Gobi deserts, leaving two-thirds as a wildlife preserve. This would undo the damage caused by people over the centuries. We create as much farmland as there is in the US: 3.9 million km 2 , bringing verdant land, food and water to the poorest parts of the world. We use subsurface drip irrigation and other advanced techniques. The details are spelled out in the book. To summarize, we would need 312 times more desalination plant capacity than now exists, or approximately 9400 of the large-scale desalination
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plants in Saudi Arabia. Nine thousand factories built along the edges of the world's largest deserts would not take up inordinate amounts of space, or materials, or time to construct. The project might take 50 years. The factories would cost $8.4 trillion at the price Saudi Arabia pays today, but the cost will fall dramatically because cold fusion will simplify the engineering, and lower the cost of construction, operation and maintenance. Half the cost would be eliminated because the Saudi plants are cogenerators and we will not need the electricity. Cheap energy will drastically lower the cost of aluminum, steel, copper and other building materials. It will lower the cost of transporting the building materials to the site, and operating bulldozers and pipeline pumps. All machines use energy, and energy is the one design parameter that affects every other aspect of economics and engineering. Cold fusion will quickly end most carbon emissions, but there will still be billions of tons of carbon left in the atmosphere from the 20th century. After the desalination project is well under way, forests will recover. Assuming half of the land is devoted to forests, they will grow to sequester 30 billion tons of carbon, or 4.5 years of present carbon emissions. If we harvest the timber and bury it deep underground, we can eventually remove all of the excess carbon now in the atmosphere. If that does not work, the book describes some other methods of removing carbon from the atmosphere. The desalination plants would have additional benefits. Magnesium and sulfur can be extracted from the enriched brine at desalination plants, as shown in Table 2. This is not a new idea. Commercial production of bromine from seawater began in 1924. Most magnesium production during World War II was from seawater. After decades of building desalination plants, extraction techniques will improve until it becomes economical to selectively extract other dissolved elements such as iodine, but not, unfortunately, palladium. This project might cost $10 billion per year for 50 years, but soon after it began it would generate a profit from agriculture, increasing land values, and improved health. Small cold fusion powered robots with artificial intelligence can attack invasive species or find fugitive terrorists. Both tasks call for small, autonomous robots, like the "roboinsects" now being developed by NASA. The book describes with roughly as much intelligence as chickens, equipped with small parallel processors. Chickens put our best supercomputers to shame. They fly through threedimensional space with pinpoint accuracy; they can distinguish between shadows and objects; and they are amazingly good at spotting, running down and eating insects. Eventually, we will learn how to make computers this good. The Asian longhorned beetle is an invasive insect that is destroying trees in the US. If we dispatch 100,000 robot chickens to go after these beetles, while we also employ pheromones and other conventional techniques, we would probably soon eradicate the beetles, or reduce their numbers so drastically that native species can reoccupy the niches. We have driven other species into extinction using cruder methods, without even trying to, or wanting to.
877 Table 2. Elements and compounds in 1000 km 3 of seawater, enough to supply half to two-thirds of the desalination mega project.
Element or compound Salt (NaCl) Magnesium (Mg) Sulfur (S) Potassium (K)* Bromine (Br) Iodine (I) Molybdenum (Mo) Vanadium (V) Palladium (Pd)
Present world consumption (metric tons) 210,000,000 3,360,000 59,000,000 23,000,000 570,000 21,400 127,000 60,000 171
Amount dissolved in seawater (metric tons) 30,215,827,338 1,280,000,000 898,000,000 399,000,000 67,000,000 58,000 10,000 2,000 0.06
Multiple of consumption 144 381 15 17 118 3 0 0 0
*The USGS shows world production is 27,400,000 tons of potash, K 2 0 , which is 83% potassium by weight. Sources Consumption: U.S. Geological Survey http://minerals.usgs.gov/minerals. Elements in seawater: Nozaki, A fresh look at element distribution in the North Pacific, Ocean Research Institute, University of Tokyo, http://www.agu.org/eos_elec/97025e-table.html.
Researchers in the UK are working on an autonomous pest-control robot that captures slugs. The limits of electric batteries constrain every aspect of the design. A conventionally powered robot would be far too heavy to fly. It would have to recharge every day. A cold fusion powered model could go for years without recharging, it could have sophisticated high-powered electronics, and range would be unlimited. The legs and wings would be driven by artificial muscles [electroactive polymers (EAP)], not by mechanical motors and gears, giving it the same range and power as an animal has. Just as ordinary birds can migrate thousands of kilometers, the robot chickens could fly from the factory to their assigned destinations. Chickens can easily identify individual people, and they have sharp vision. The robot chickens could not only find insects, they could look for individual people in crowds, or fugitive terrorists and lost hikers in the wilderness. 4. Public Support is Essential Some people feel it is pointless to speculate about how cold fusion may shape the future when there is no funding, and when cold fusion cells have seldom produced more than a few watts of power. Some may feel this book oversells the prospects for the technology. But I believe we must have broad public support in the political battle to fund this research. The public will not act until we inspire. When the voters in a democratic society become aware of a problem, and they demand action, their power is irresistible. Samuel Florman wrote: 5 Sir Hugh E. C. Beaver, addressing the First International Congress on Air Pollution in 1955, traced the 700-year long campaign against air pollution in England. Complaint after complaint, committee after committee, report after report - all were
878 ineffectual... Finally t h e London Smog of 1952, with its horrendous 4000 deaths, set the scene for a new investigating committee, which was chaired by Sir Hugh. T h e committee's report was well received, said Beaver, and led to effective action, not because the report was exceptional in any way, but because the public was, at long last, receptive. T h e lesson to be learned, according to Beaver, is t h a t "on public opinion, and on it alone, finally rests the issue."
References 1. T. Mizuno, Nuclear Transmutation: The Reality of Cold Fusion (Infinite Energy Press, Concord, NH, 1998). 2. T. Roulette, J. Roulette, and S. Pons, Results of ICARUS 9 experiments run at IMRA Europe, in Proceedings of the Sixth International Conference on Cold Fusion, Progress in New Hydrogen Energy (Lake Toya, Hokkaido, Japan, 1996); New Energy and Industrial Technology Development Organization (Tokyo Institute of Technology, Tokyo, Japan, 1996). 3. M. Riordan and L. Hoddeson, Crystal Fire, the Birth of the Information Age (W. W. Norton & Company, NY, USA, 1997). 4. California Coastal Commission, Seawater Desalination in California, http://www.coastal.ca.gov/desalrpt/dchapl.html. 5. S. Florman, The Existential Pleasures of Engineering (St. Martin's Griffin, USA, 1996).
R E C E N T COLD F U S I O N CLAIMS: A R E T H E Y VALID?
LUDWIK KOWALSKI Department of Mathematical Sciences, Montclair State University Upper Montclair, NJ 07043, USA
1. What is Cold Fusion? Cold fusion (CF) is a mixture of several claims that may or may not be related. Some of them belong to the realm of basic science while others belong to the area of patents. And some seem to be science fiction. From the point of view of history the CF episode, described in several books 1 - 7 and articles, 8 ' 9 is highly unusual. It is a situation in which the validity of research in one particular field has been officially questioned, at least in the USA. According to many scientists, the CF claims are in conflict with basic principles of physics and chemistry. That is why most researchers are no longer interested in CF. Surprisingly, however, the field still attracts a large number of investigators with excellent credentials. Once a year they meet at international conferences and publish papers, most often in conference proceedings and over the Internet. 10 As a nuclear physicist, and a physics teacher, I examined some of these publications and attended one CF conference.11 My goal here is to describe the main CF claims: (a) unexpected neutrons and protons, (b) unexplained excess heat, and the most extraordinary, (c) transmutation of chemical elements. The first claim resulted from the work of a physicist, Steven Jones, who wrote about his CF work in the early 1980s. The second resulted from the work of a world class electrochemist, Martin Fleischmann; he kept the CF investigations secret up to the 1989 press release. And the third claim can be traced to the 1990s observations of another chemist, John Bockris. For the sake of brevity each claim will be described in terms of its origin and in terms of recent reports with which I am familiar. The task of writing a systematic review of hundreds of investigations conducted by top scientists in the last 10 years is beyond my capabilities; I am not a CF researcher.
2. The Claim of Unexpected Neutrons and Protons Steven Jones, working at the Los Alamos National Laboratory, was exploring muonic atoms of hydrogen and the unstable molecules they form.12 Such molecules are about 200 times smaller than their stable electronic counterparts. According to a well-verified theory of the so-called "tunneling effect," the proximity of hydro879
880
gen atoms in muonic molecules increases the probability of nuclear fusion by many orders of magnitude. This is associated with the release of energy, as in stellar interiors and hydrogen bombs. For nearly a decade the work on muonic atoms was supported by the US government as a possible path toward a new source of energy. The grant, however, was not renewed after it became clear that practical applications, if any, would not materialize in the immediate future. These investigations led to the idea that CF might be occurring at very high pressures inside planets, as described in. 13 ' 14 The notion that guides Jones, of a large electron screening effect in the D-D fusion reaction for deuterons embedded in metals, has been independently confirmed by other experimental physicists. 15 Can screening be responsible for lowering of the D-D coulomb barrier in a metal? Recent observations of rare neutrons and charged particles, reported by Jones, 16 give credence to such speculations. The rates of observed emission are usually very low but significantly higher than the background; in one experiment the rate of proton emission was 400 times higher than the background. The particles, identified as 3 MeV protons, were emitted from spots inside thin titanium foils loaded with deuterium. To load hydrogen ions into the foils Jones placed them (for several hours) into a cylinder filled with the deuterium gas at elevated temperature (500° C) and pressure (40psi). Emission of nuclear particles was subsequently recorded with scintillation and silicon detectors in the low-noise environment. An aluminum foil of 19 /jm helped to identify charged particles as protons. Coincidences between protons and other charged particles (tentatively assumed to be 3 H) were observed with a set of two silicon detectors. Let me add that protons and alpha particles have also been reported by Lipson,17 Oriani, 18 and Karabut. 19 These researchers worked independently of each other; their methods of loading metals with ions, and their methods of particle detection, were very different from those used by Jones. The process of emission of such particles remains to be interpreted. For the time being Jones favors the model according to which the 2.45 MeV neutrons and the 3.02 MeV protons are accompanied by 0.82 MeV 3 He and by 1.01 MeV 3 H, respectively, as in well-known thermonuclear reactions. The probability of emission of these particles in a metallic environment, however, is much higher than expected. A recent paper, published by a large team of German scientists, 15 does show that the cross section of the D(d,p)t reaction, at very low energies (down to 5 keV), is about one order of magnitude larger in the deuterated Ta than in a gas target. Similar observations were made earlier in Japan. 20 Very recently, a team of researchers from Russian Academy of Science,21 found a unique way of observing protons (presumably from the same reaction) down to the energy of 0.8 keV. The observed rate of emission, at the lowest energy, turned out to be nine orders of magnitude higher than predicted by an accepted theory. This seems to indicate that the theory which agrees with experimental data above the energy of 10 keV fails to account for what happens to the embedded ions in titanium at much lower energies. But arguments about a model (screening vs. other possible explanations) should
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not be confused with arguments about the validity of experimental data (observing unexpected neutrons and protons).
3. The Claim of Excess Heat The claim of excess heat was first made in a famous press conference, on 23 March 1989. That event, and its consequences are described in several books about C F . 1 - 5 Two scientists, Fleischmann and Pons, announced that they had been conducting research on highly unusual electrochemical cells for several years. These cells were said to be outputting more thermal energy than received in the form of electric energy. The authors wrote that chemical contributions to excess heat were found to be insignificant. On that basis they tentatively concluded that the origin of excess heat was nuclear. Rejecting this hypothesis the critics pointed out that rates of nuclear reactions accompanying excess heat, if the origin of that heat were nuclear, would be many orders of magnitude higher than what was observed. The path of Fleischmann toward CF research was prompted by a theoretical consideration. In an article published in 2000,22 he wrote: "Realization that models of electrolyte solutions had to be based on the QED paradigm inevitably focused my attention again on the Pd/H and Pd/D systems. I had realized since the end of 1947 that these were the most extraordinary examples of electrolytes... The question of whether one could induce nuclear reactions became more clearly defined at the end of that decade (1960s). Work on the isotopic separation of H and D showed that it was necessary to assume that the H and D present had to be modeled as many-body systems in order to explain the macroscopic behavior... In the early 1980s Stan Pons and I started a number of collaborative projects... We decided that the project not only had to have a 'hidden agenda,' it had to be totally hidden. This was all the more necessary because the military applications of any positive outcome of the research were not at all clear... The overall structure of the problem had become reasonably clear by the summer of 1988. We were observing the generation of heat in excess of the enthalpy input to the cells, and far above that commensurate with the generation of tritium and neutrons predicted by measurements on 'hot fusion.' Moreover, the excess enthalpy was far beyond that which could be attributed to any parasitic chemical reactions." Subsequent work in the area is described in two books 6 ' 7 and in many papers, such as Refs. 23 and 24. The authors of these references describe experiments in which excess heat was presumably generated. But they do not always provide enough data to rule out the possibility that a large fraction of excess heat can be due to parasitic chemical reactions, or other non-nuclear processes. Furthermore, according to Shanahan, 25 the excess heat claims are due to calibration errors. It is difficult for me to accept this accusation because similar results have been reported by a large number of highly qualified scientists in several countries. On the other hand, I do not ignore the possibility of experimental bias, mutual self-deception, or
882
even fraud. The best evidence that the excess heat is nuclear would be to show the commensurate accumulation of byproducts of nuclear reactions, such as 4 He. This will be discussed in Section 4. The most recent contribution, in the area of excess heat, belongs to a group of Chinese scientists. 26 Li, a veteran of CF research, did not use electrochemistry to load palladium with deuterium. The excess heat was generated when compressed gas was allowed to diffuse through a thin palladium wall. According to the authors that heat could not be explained by the well known Joule-Thomson effect or by chemical reactions. They write: "this experiment has been repeated six times already in various configurations. The 'excess power' density in the Pd disk is more than 100 W/cm 3 , which is about the power density in a fuel rod of a thermal neutron fission reactor." Reproducible results on generation of excess heat, in a glow discharge chamber (another non-electrolytic method of loading metals with D + ions), were also reported by Russian scientists. 19 Generation of excess heat without producing radioactive material would certainly be desirable. But how can nuclear energy be released without commensurate amounts of radioactivity? According to some theoretical considerations, 27 deuterium ions embedded in crystals might be influenced by a large number of atoms able to supply and to remove energy "in unison." Theoretical modeling of natural phenomena, however, and attempts to validate these phenomena experimentally, are two different things. Arguments for or against models do not resolve disputes about validity of experimental data. 4. The Alchemy Claim Attempts to change one chemical element into another are usually referred to as alchemy. Such transformations are believed to be impossible unless nuclear reactions are involved. A nuclear fusion of two deuterons (2H + 2 H), for example, nearly always results in production of either 3 He or 3 H (associated with the emission of neutrons and protons, respectively). Turning atoms of one element into atoms of another element, such as 2 H into 3 He, by means of nuclear reactions, is usually called transmutation. Atomic nuclei repel each other and for that reason they are not expected to fuse spontaneously at temperatures below tens of millions of degrees. That is why the claim of nuclear origin of excess heat was not taken seriously when it was first made in 1989. But several years later Bockris reported 28 accumulation of 4 He, and other atoms, in the electrodes of CF cells. Some of his early claims were later withdrawn 29 due to irreproducibilities. Progressive accumulation of 4 He, however, was later observed by other investigators. 30,31 They reported that helium generated via CF is mainly 4 He; the 3 H and 3 He atoms are produced much less frequently. The situation is dramatically different from what happens in thermonuclear reactions taking place in ionized gasses. In these reactions the probability of the 2 D + 2 D —>4He (releasing about 24MeV of energy) is 10~ 6 while the probabilities of reactions producing 3 H and 3 He (releasing about 3MeV of energy) are roughly 0.5 each. How can this difference be
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explained? That is one of the many unanswered theoretical questions. At present, however, the main issue is experimental rather than theoretical. Is the accumulation of 4 He, at the rate of about one atom per 24MeV of excess heat, real or apparent? It is natural to suspect that helium comes from the surrounding air and not from a totally unexpected nuclear reaction. The authors of the above-mentioned reports, however, addressed this issue and ruled out the possibility of atmospheric contamination. If confirmed, such findings could become very significant. They would indicate that 4 He is the main "ash" of the mysterious CF burning, at least in some cases. A connection between the excess heat and alchemy would be established. Observation of alpha particles emitted from metallic foils loaded with deuterium, reported by two Russian teams, 16 ' 19 might also be linked with the accumulation of helium. It is significant, however, that the reported rates of alpha particle emission are not commensurate with the rate of generation of excess heat. Production of elements heavier that helium, first reported and then withdrawn by Bockris, was later heralded by some investigators. 6 ' 19 ' 32 Results from a very extensive study are summarized in Ref. 33. The most recent report in this disputed area was presented by Iwamura, from Advanced Technology Research Center, Mitsubishi Heavy Industries Ltd., Japan. Addressing the 10th International CF Conference (August 2003) Iwamura described a fascinating setup 34 in which cesium was turned into praseodymium and strontium was turned into molybdenum. The paper describing these experiments 35 had already been published in the prestigious Japanese Journal of Applied Physics (JJAP). Was I the only one whose first reaction, during Iwamura's conference presentation, was to think about pseudo-scientists? Imagine a 0.1 mm membrane, mostly Pd, forming a window of a container filled with deuterium. The gas diffuses slowly through the membrane and enters a vacuum chamber (from which it is constantly removed by a pump). On the deuterium side the membrane is covered, either electrolytically or by the ion injection method, with a material to be transformed. Using highly sophisticated analytical tools the researchers were able to show that the amount of deposited material, such as purified Cs or Sr, decreases, while the amount of new material, such as Pr and Mo, increases at the same rate. Comparing this situation with a typical nuclear reaction setup (a target and a beam from an accelerator) the authors write: "analysis of the depth profile of Pr indicated that a very thin surface region up to 100 A was the active transmutation zone. Many experimental results showed that the quantity of Pr was proportional to the deuterium flux through the Pd complex. The cross section of transmutation of Cs into Pr can be roughly estimated at one barn if we consider the deuterium flux as an ultra-low-energy deuteron beam." The view of the membrane in Fig. 1 (of their paper), shows that it is essentially a 0.1mm Pd foil coated with several alternating thin layers of CaO and Pd. The first layer encoutered by deuterium, as it enters the membrane, consists of Pd; it is 400Athin. Pure Cs or Sr were deposited on that layer. As indicated in another
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figure, it took nearly 100h to turn all atoms of Cs (about 1.3 x 1015) into atoms of Pr; transformation of an equal amount of Sr into Mo took about 300 h. The Cs —> Pr experiment was performed two times while the Sr —> Mo experiment was performed three times; the results were shown to be reasonably reproducible. I find it highly significant that the isotopic composition of Mo, produced from Sr, is drastically different from that found in nature. This seems to rule out the possibility of contamination (redistribution of impurities). On the other hand, I recognize the exotic nature of the suggested mechanism (see below) and the small amount of products (fractions of microgram). Low-energy transmutations in condensed matter, reported by Iwamura, have recently been repeated by scientists from Osaka University.36 Here is a quote from their brief description: "as a result, we confirmed that the nuclear transmutation reaction from 133 Cs to 1 4 1 Pr occurred. This transmutation suggests that the mass number and the atomic number increase by 8 and 4, respectively. The model of multi-body resonance fusion of deuterons, proposed by Takahashi, can explain this mass-8 and charge-4 increased transmutation as follows: (Primary reaction): (Secondary reaction):
8D -> 133
16
0 * - • 8 Be* + 8Be* + 95.2 MeV,
Cs + 8 Be(47.6MeV) - •
141
Pr* (50.47MeV),
or 8
Be* - • 4 He + 4 He.
If the phenomena occur according to this model then 4 He should also be produced. So we are trying to detect 4 He." I am puzzled by some aspects of the suggested model. For example, I do not understand the nature of the "multi-body resonance" process by which eight deuterons fuse to form a highly excited (109.8 MeV) oxygen nucleus. If the 1 4 1 p r * nuclei are excited, as indicated by the asterisk, then characteristic gamma rays would be emitted. But why should this influence my attitude toward experimental data? It is interesting that radioactive byproducts (of presumed nuclear reactions) are not mentioned in Ref. 33 or in Ref. 34. Most radioactive byproducts would be much easier to identify, in small quantities, than their stable counterparts. Confirmed absence of radioactive byproducts would indicate that nuclear reactions in condensed matter (presumably responsible for exotic transmutations), are totally different from common nuclear reactions. This has already been suggested by those who investigated generation of helium.
5. Final Comments The CF is not taken seriously by most scientists. But, according to my own informal survey, the opinion of many is still based on what was known in 1989 and not on
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recent publications. I think that the often repeated labels, such as "pseudoscience" and "fiasco of the century" were justifiable in 1989, when the Energy Research Advisory Board (ERAB) report was published. The ERAB, 37 was a team of American experts appointed to evaluate the CF claims. But are such labels justifiable today? Most of us are not equipped to answer this question through laboratory investigations. That is why another official evaluation, for example, by teams of experts appointed by the US National Academy of Sciences, is desirable. Each of the three claims should be investigated independently; finding that something is wrong with one does not necessairely mean the other two claims are not valid. Are the credentials of CF scientists doubtful or not? Are their ways of validation consistent with scientific methodologies? Is there any evidence of deliberate deception? Answers to such questions should help us decide what to think about the controversial field, and what to tell students when they ask questions about it. For the time being I tell them that CF is nothing more, and nothing less, than an area of investigation that has to be explored because a large number of competent scientists are working in it. The degree of support, as in any other area of basic research, should depend on results at hand, on available means, and on the rate of progress. I also tell students that claims conflicting with what is known about natural phenomena should not be accepted without extraordinary evidence. Let me end this essay by quoting from an e-mail message received from a recognized authority in the area of nuclear chemistry. "The whole atmosphere around CF has been filled with poisonous material, some valid and some emotional. One must be very careful, on entry into such an atmosphere, to be protected by a useful theoretical proposal or at least a plausible explanation that can be subjected to experimental tests. On the basic level there are two obvious questions: (1) how could hydrogen atoms fuse at such a low temperature? (2) If they do fuse, how is the energy released (if not in gamma rays, then how) i.e., what reaction occurred? If one has no proposed answer or proposed experiment to get an answer, then one is in a state of massive weakness... I infer that the major skepticism in the mainstream nuclear science community stems from the silence on the basic two questions above... Such skepticism seems to me to be justified until something reasonable is proposed or, better yet, demonstrated. Until then, essentially all responses will be 'impurities or errors'." Yes, these two theoretical questions are very important. But, as indicated above, arguments about models should not be confused with arguments about the validity of experimental data. No theoretical model existed when excess heat from radium was discovered by Pierre Curie. On the other hand, experimental findings conflicting with confirmed theories, as in the case of CF, should be scutinized very carefully before being accepted. That is why many of us would benefit from another formal investigation of the main CF claims by experts.
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References 1. F.D. Peat, Cold Fusion (Contemporary Books, Chicago, 1989). 2. F. Close, Too Hot to Handle: The Race for Cold Fusion (Princeton University Press, Princeton, NJ, USA, 1991). 3. E.F. Mallove, Fire from Ice: Searching for Truth Behind the Cold Fusion Furror (Wiley, NY, USA, 1991). 4. G. Taubes, Bad Acience: The Short Life and Weird Times of Cold Fusion (Random House, NY, USA, 1993). 5. J.R. Huizenga, Cold Fusion: The Scientific Fiasco of the Century, 2nd edn. (Oxford University Press, Oxford, 1993). 6. T. Mizuno, Nuclear Transmutations: The Reality of Cold Fusion (Oak Grow Press, Concord, NH, USA, 1998). 7. C. Beaudette, Excess Heat. Why Cold Fusion Research Prevailed (Concord, NH, USA, 2000). 8. G.H. Miley, Some personal reflections on scientific ethics and the cold fusion episode, Account. Res. 8, 121 (2000). 9. D.J. Nagel, Cold fusion and philosophy, Account. Res. 8, (2000). 10. A large number of cold fusion papers is downloadable over the Internet, in the form of pdf files, from the library section at http://www.lenr-canr.org. 11. Proceedings of the 10th International Conference on Cold Fusion was held in Cambridge, MA, USA, 24-29 August 2003. In the form of pdf files, can be downloaded from the Internet site at http://www.lenr-canr.org/iccflO/iccflO.htm. 12. S.E. Jones et al, Phys. Rev. Lett. 5 1 , 1757 (1983). 13. S.E. Jones et al, Phys. Rev. Lett. 56, 588 (1986). 14. S.E. Jones et al, Cold Nuclear Fusion (Scientific American, 1987) p. 7. 15. F. Raiola et al, Enhanced electron screening in d(d,p)t for deuterated Ta, Eur. Phys. J. A 13, 377-382 (2002). 16. S.E. Jones et al, See three papers presented at the 10th International Cold Fusion Conference, August 2003 (see Ref. 11). 17. A. Lipson et al, See his paper presented at the 10th International Conference on Cold Fusion, August 2003 (see Ref. 11). 18. R. Oriani et al, See his paper presented at the 10th International Cold Fusion Conference, August 2003 (see Ref. 11). 19. A. B. Karabut et al, Nuclear product ratio for glow discharge in deuterium, Phys. Let. A 170, 265 (1992). (A much more detailed report, based on recent data, was presented at the 9th International Cold Fusion Conference in China (2002) (see Ref. 10). 20. J. Kasagi et al, Anomalously enhanced D(d,p)T Reaction in Pd and PdO observed at very-low-energy bombardments. This 1998 paper is available over the Internet (see Ref. 10). 21. A. Lipson et al, Enhancement of DD-reaction accompanied by X-ray generation in a pulsed low voltage high-current deuterium glow discharge with a Ti-cathode. This 2003 paper is available over the Internet (see Ref. 11). 22. M. Fleischmann, Reflections on the sociology of science and social responsibility in science, in relationship to cold fusion, Account. Res. 8, 19 (2000). 23. M. McKubre, This paper, presented at the 10th International Cold Fusion Conference, is available over the Internet (see Ref. 1). 24. E. Storms, Excess power production from platinum cathodes using the PonsFleischmann effect, in Proceedings of the 8th International Conference on Cold Fusion (Lerici (La Spezia), Italy, 2000). This paper is available over the Internet (see Ref. 11). 25. K. Shanahan, A systematic error in mass flow calorimetry demonstrated, Thermochim. Acta 387, 95-100 (2002). This article is available over the Internet (see Ref. 11).
887 26. X.Z. Li et al, Correlation between abnormal deuterium flux and heat flow in a D/Pd system, J. Phys, D: Appl. Phys. 36, 3095-3097 (2003). This article is available over the Internet (see Ref. 11). 27. T. Chubb, S. Chubb, and P. Hagelstein, Each of these authors has an abstract of a paper to be present at the March 2004 meeting of American Physical Society. These abstracts can be seen at the APS web site: http://www.eps.org/aps/meet/MAR03/baps/abs/S9530.html. 28. J. Bockris, Early contributions from workers at texas A&M university to (so-called) low energy nuclear reactions, J. N. Energy 4 (2), 40 (1999). 29. J. Bockris, G. Lin, and N. Packham, A review of the investigations of the FleischmannPons phenomena, Fusion Technol. 18, 11-31 (1990). 30. M. Miles and B.F. Bush, Heat and helium measurements in deuterated palladium, Trans. Fusion Technol. 26 (4T), 156 (1994). 31. . Y. Arata and Y. Zhang, Helium (He , He ) within deuterated Pd-black, Proc. Jpn. Acad. B 73, 1 (1997). 32. T. Ohmori et al, Iron formation in gold and palladium cathodes, J. N. Energy 1 (1), 15-22 (1996). 33. G. Miley et al., Advances in thin-film electrode experiments, in Proceedings of the 8th International Conference on Cold Fusion (Lerici, Italy, 2000). This paper is downloadable from the library at http://www.lenr-canr.org. 34. Y. Iwamura et al., Energy nuclear transmutation in condensed matter induced by D2 gas permeation through Pd complexes: correlation between deuterium flux and nuclear products. This paper is available over the Internet (see Ref. 1). 35. Y. Iwamura et al., Elemental analysis of Pd complexes: effects of D2 gas permeation, Jpn. J. Appl. Phys. 4 1 , 4642-4648 (2002). 36. T. Higashiyama et al, Low energy nuclear transmutation in condensed matter induced by D2 gas permeation through Pd complexes: correlation between deuterium flux and nuclear products. This paper is available over the Internet (see Ref. 1). 37. The executive summary of the Energy Research Advisory Board (ERAB) report can be found in (5). The Cold Fusion Research. A Report of the Energy Research Advisory Board to the United States Department of Energy, can be downloaded from the Internet site: http://www.ncas.org/erab.
HISTORY OF A T T E M P T S TO P U B L I S H A P A P E R
LUDWIK KOWALSKI Department of Mathematical Sciences, Montclair State University Upper Montclair, NJ 07043, USA
My 2004 paper, reviewing recent cold fusion claim, has been rejected (without sending it to referees and without offering any criticism) by editors of seven journals: (1) (2) (3) (4) (5) (6) (7)
Physics Today, USA. American Scientist, USA. Scientific American, USA. Nature, UK. New Scientist, UK. The Physics Teacher, USA. Science, USA.
Please read the rejected article; it is available as http://blake.montclair.edu/~kowalskil/cf/152summary.html
a
webpage
at:
1. Here is How M y Paper was Introduced to the Editor of One of the Above Journals. Other Accompanied Letters were Similar "I am sure that you are aware of the DOE move to review the cold fusion field, as reported in The New York Times (25 March 2004). Attached is a review article that, I hope, can be published in Scientific American. The title is "Recent cold fusion claims: are they valid?" It is not a paper defending cold fusion claims; it is a paper describing them, no matter what one is inclined to think. Scientifically literate readers are likely to appreciate my short summary of recent claims made by cold fusion researchers. Some of these claims, such as turning Sr into Mo, or Cs into Pr, without stellar temperatures, are even more extraordinary than the claims made by Pons and Fleischmann. The strange thing is that authors of such reports seem to be reputable scientists associated with prestigious universities and laboratories. Is it a matter of fraud? Is it a matter of self-deception, or incompetence? Is it a matter of progressive degeneration due to the isolation of the field from mainstream science? My article does not try to answer these questions; its purpose is to present a summary of what has been recently reported without taking sides. The subject is interesting no matter what the final verdict of the second DOE evaluation will be.
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Like many other science teachers, I am in no position to verify validity of hard-to-accept claims in a specialized laboratory. That is why, as suggested in the concluding section, a new evaluation of cold fusion claims, by an appointed panel of experts, is highly desirable. In writing this I was not aware of the pending DOE investigation. I deliberately avoided references to social aspects, which are interesting but highly controversial. I am a physics teacher at Montclair State University. Studying cold fusion was my 2003/2004 sabbatical project, which resulted in the attached manuscript." 2. In Rejecting My Paper the Editor of Physics Today Wrote "Dear Dr. Kowalski, We received your article submission titled 'Recent Cold Fusion Claims: Are They Valid?,' and appreciate your sending it to Physics Today. However, after reviewing it we have concluded that it does not meet our editorial needs. Thank you for your interest in Physics Today. Sincerely, Stephen G. Benka Editor-in-Chief." That is it. Not a single word about the content of the article. How can the phrase "does not meet our editorial needs" be interpreted? Why was the article not sent to referees? They do publish many field summaries each year. Why was my summary not given the same chance to be reviewed by experts? Was I writing about sociology, poetry, business or something else unconnected to physics? Are recent cold fusion claims described in the article already widely known to most physicists? Was my description of these claims erroneous? Was the article rejected because of its style, its limited scope, or its disregard for ethical standards? 3. And Here How the Editor of American Scientist Responded to my submission "Dear Dr. Kowalski: Yes, we've received your original manuscript and the follow-up. I'm afraid we're not always able to acknowledge receipt immediately. I try to give a prospective author an idea of whether we'll be able to consider a manuscript, and sometimes it takes a little time to determine that. We have certain basic criteria for submissions. When a submission does not meet those criteria, I prefer to say that it cannot be considered rather than simply acknowledge receipt. In the case of this submission, I'm unsure. We publish feature-length articles and commentaries based on original published research. The authors of American Scientist articles are the people who have done the work and therefore are in a position to survey their own field. I don't actually have evidence (in the form of cited publications or a c.v.) that you have done original research on the topic you propose to write about. If you would like to publish a short commentary, we do have a department with different criteria, called 'Macroscope.' This is where we publish short essays conveying a scientist's point of view on a matter of personal or professional interest to scientists and engineers. The maximum word count is 1500. If you would like
890
us to consider publishing your piece in a short form, please let me know, and I'll share it with my colleagues and let you know the response. Sincerely, Rosalind Reid Editor, American Scientist." 4. Responding to the Above I Wrote "Dear Dr. Reid: Thank you for your prompt reply. I understand your hesitation. Protecting readers of American Scientist from people who are not qualified to write about science should be one of your tasks. To help you decide here is a little summary about myself. I am an experimental nuclear physicist (PhD, 1963) with a large number of publications (mostly as coauthor) in that field. The attached abbreviated list of publications, spanning four decades, makes it clear that my teaching commitment has not prevented me from active participation in nuclear physics research. Like most scientists, I accepted the 1989 verdict about cold fusion. And you are correct, I have no publications about cold fusion. My new interest in this field was triggered in October 2002. I attended a nuclear conference in New Mexico and heard several scientists talking about cold fusion research. It was the beginning of my sabbatical year. The paper I submitted is the product of that work. I hope your hesitation will not prevent you from sending my article to competent and unbiased reviewers. Please let me know what your decision will be. Meanwhile I would like to follow your suggestion about writing a short commentary on the anticipated review of cold fusion by the DOE; see the attached file. Thank you for your consideration. Sincerely yours, Ludwik Kowalski." A list of my selected publications and a file containing my "short piece" (see below) were attached. 5. Seek not the Golden Egg, Seek the Goose According to a recent article in The New York Times (25 March 2004) the US Department of Energy (DOE) is going to review the field of cold fusion this year. This is a significant event; the controversial field of cold fusion (CF) has often been called pseudoscience. If it were up to me I would suggest that the panel of DOE scientists focus on essential scientific questions and not on practical applications which are far away, at best. Promising too much, and too early, was one of the mistakes made 15 years ago. In my opinion the six most important scientific questions are as follows. (1) Are unexpected neutrons, protons, tritons and a. particles emitted (at low rates) in some CF experiments? (2) Is generation of heat, in some CF experiments, linearly correlated with the accumulation of 4 He at the rate of 24 MeV per atom of 4 He? (3) Have highly unusual isotopic ratios been observed among the elements found in some CF systems? (4) Have radioactive isotopes been produced in some CF systems?
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(5) Has transmutation of elements occurred in some CF setups? (6) Are the ways of validating scientific findings in the areas of CF research consistent with accepted methodologies in other areas of science? I think that a positive answer to even one of these six questions should be sufficient to justify an official declaration that "cold fusion, in light of recent data, should be treated as a legitimate area of research." The normal peer review mechanisms will then be used to separate valid claims from wishful thinking.
6. In a Subsequent Reply I Wrote . . . I already mentioned two reasons making such review urgent: the 15th anniversary of the Utah announcement and the pending DOE investigation. In my opinion, by publishing my paper, or a review written by somebody else, you will contribute to something desirable. Nobody is happy with the unhealthy feud between a group of well motivated researchers and official representatives of "mainstream science." Most people are passive but those who do take extreme positions often use highly pejorative adjectives, such as "pathological," "stubborn," "misguided," and "fraudulent." Please do not miss an opportunity to contribute to ending this unnecessary feud. I would be happy to give you names and addresses of top people in five main areas of cold fusion... So now you have several excuses for bending a rule of your editorial policy. They are: (a) the anniversary, (b) the pending DOE investigation, (c) my paper is a review describing (very objectively, and without accusations of any kind, as you probably noticed) several very different areas of a broad field, (d) my background as an active nuclear physicist, and (e) my unpublished research in two areas of cold fusion. You are certainly aware how difficult it is to publish cold fusion research papers in important scientific journals. Will the situation change after the pending DOE investigation of cold fusion? I hope so. Please help to contribute to this cause. If you decide to approach Fleischmann, be aware that he is an electrochemist; I do not consider him to be an expert in nuclear physics. This became clear in 1989 and contributed heavily to the cold fusion controversy. One can only imagine what would happen if Fleischmann and Pons, who are chemists, refused to participate in the infamous press release, organized by the administrators of the University of Utah, and decided to work with Steven Jones, who is a physicist. A year or two later they would publish a peer reviewed paper and... But I refuse to speculate; my goal is heal the wound by focusing on purely scientific topics and by ignoring stupid things people said or wrote before. Please help me. I think that cold fusion, no matter what the final verdict will be, is a highly significant episode in the history of science. Let your journal be a part of that history... I also gave Dr. Reid names and e-mail addresses of five people (who are certainly much more knowledgeable than myself) I suggested that she contacts one of them to write a longer review paper of the journal. Steven Jones, Martin Fleicshmann
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and George Miley were among the scientists I selected. I did not hear from Dr. Reid again. Will she accept my "short piece?" Probably not. 7. The Manuscript was Submitted to Scientific American Here is the reply that came after a long delay: "Dr. Kowalski: Thank you for your offer to contribute to Scientific American. After much consideration, I regret to say that the piece you propose is not suited to our somewhat limited editorial needs. We appreciate your interest in Scientific American. Regards, Jacob Lasky Editorial Administrator." 8. I then Tried to Publish the Paper in Nature Instead of sending the article to them I decided to follow the presubmission path. The most impressive part of the path was that the negative reply came about ten hours later. The process of presubmission consists of filling two text boxes on their web site. The first box was for the letter about my article; I wrote essentially the same as what I wrote to other editors. The second box was for the first paragraph of my paper, and for the references used in it. The reply was short and clear: "Thank you for your inquiry about submitting your paper entitled 'Cold fusion 15 years later' to Nature. I regret that the paper that you describe seems unlikely to prove suitable for publication in Nature, and we accordingly suggest that you pursue publication elsewhere. I am sorry that we cannot respond more positively on this occasion. Yours sincerely Dr Karen Southwell, Senior Editor." 9. I then Tried Another UK Journal, N e w Scientist But they never responded. After waiting about a month the article was submitted to The Physics Teacher, a journal in which several of my teacher-oriented review papers were published in the past. In submitting the article I wrote: "Dear Dr. Mamola: As you probably remember, the manuscript on Cold Fusion that I submitted about 2 years ago was rejected by your reviewers. My letter to the editor, however, was published last summer. I was pleased by this. The topic, as you know (see the "DOE WARMS to Cold Fusion" article in last April issue of Physics Today), is likely to be of great interest in the near future. With this in mind I wrote a new article on Cold Fusion and I hope that you will be able to publish it next fall. As you will see, I am simply describing controversial claims, I am not defending them. An extensive list of references is provided for those teachers who might wish to familiarize themselves with recent papers. The length is 3302 words, including 37 references. If necessary I can shorten the article, and reduce the list of references. But I prefer not to do this because I believe that everything is important. . . . I am still undecided about validity of cold fusion claims but I think that they should be known to physics teachers. Unfortunately, most teachers are not familiar with experimental data gathered in the last 10 years. The pending evaluation of the
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field by the DOE is likely to be publicized in the media; this will lead to student interest and questions. Hopefully, my paper will help teachers deal with the renewed interest in the "forbidden field." More that a month later I received the following rejection: "Dear Professor Kowalski: We have reviewed your manuscript "Cold Fusion 15 Years Later" in the light of the recent Physics Today article "DOE Warms to Cold Fusion." While a paper in T P T on this subject may be warranted, we do not believe there is any great urgency to publish one immediately. After all, according to the Physics Today piece, DOE Deputy Director Decker says that their "review of cold fusion will begin in the next month or so [that was back in April]" and it "won't take a long time - it's a matter of weeks or months." We believe that it would be premature to publish a cold fusion paper in T P T before the results of the DOE review are announced. Were we to do so, a follow-up piece would almost certainly be required later, regardless of how that review turns out, and we don't feel that two papers on the subject are warranted. We will consider your paper again (along with any revisions induced by the DOE report) after the report is made public." 10. M y Immediate Reply "Dear Dr. Mamola: Was my manuscript examined by referees? I would very much like to see what they had to say about its content. Thanks in advance." This message has not yet been answered. Will I see the referee's comments? Probably not. Will the pending DOE review end the unhealthy feud about cold fusion? Will it result in elimination of administrative barriers (such as rejection of articles without the peer review process)? What motivates defenders of the status quo? Who benefits from it? Yes these questions belong to the realm of social sciences. But that does not mean they should remain unanswered. The reply from Dr. Mamola came much later than I expected. He wrote "Dear Professor Kowalski, My apologies for the delay in responding to your email. I have been out of the office for several weeks. To answer your question, the manuscript was reviewed by our editorial staff. We consulted with one of our referees but did not ask for a formal review, believing it would be premature at this point. Sincerely, Karl C. Mamola Editor." 11. The Manuscript was then Submitted to the Editor in Chief of Science Donald Kennedy. Here is the reply received next day, Saturday afternoon: "I've consulted with our editorial staff in the physical sciences. Unfortunately, we don't think this topic is an appropriate one for review in Science at this time. Thanks for thinking of Science. Sincerely yours. Donald Kennedy." Hmm, very efficient; they had only couple of hours on Friday to read the manuscript. It was rejected because the topic is not appropriate. Why is it not appropriate? Aren't the described claims scientific?
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Author Index
A
Dash, J., 477 Di Stefano, V., 108, 392 Dorsch, T., 210 Du, B. Q., 102 Dyad'kin, A. P., 374
Abyaneh, M., 587 Adamenko, S. V., 505 Akimoto, T., 312 Akleyev, A. V., 537 Ambadkar, A., 477 Andreassi, V., 108 Aoki, Y., 161
E El-Boher, A.,
84
F
B
Falcioni, F., 108 Fasano, G., 405 Filimonov, V., 776 Filippov, D. V., 806, 838 Fisher, J. C , 281, 295 Fleischman, M., 587 Focardi, S., 70, 405, 414 Fontana, F., 108 Fukuhara, M., 546 Fulvio, F., 612 Furuyama, Y., 218
Bazhutov, Yu. N., 374, 818 Bazhutova, S. Yu., 374 Benson, T. B., 147 Branover, H., 84
c Cai, N. N., 635 Campari, E., 405, 414 Cao, D. X., 351, 635 Castano, C , 128 Catena, C , 108 Celani, F., 108, 312, 392 Celia, E., 108 Chen, G., 102 Chen, S., 635 Chubb, S. R., 646 Chubb, T. A., 23, 665, 678, 685 Chung, D. Y., 161 Cirillo, D., 492 Cravens, D., 269 Czerski, K., 194, 210, 228
G Gabbani, V., 70, 405, 414 Gamberale, L., 108 Garbelli, D., 108 Gareev, F. A., 459 Gavritenkov, D. V., 438 Giudice, E. D., 587 Gordon, F. E., 359 Greenspan, E., 84
D
H
D'agostaro, G., 108 Dardik, I., 81, 84
Hagelstein, P. L., 23, 743 Heide, P., 194, 210, 228
895
896
Hekman, R. J., 23 Hora, H., 822 Huke, A., 194, 210, 228
I Iorio, V., Ishikawa, Itoh, T., Iwamura,
492 T., 339 339 Y., 339
J Jin, L. H., 102 Jones, S. E., 269
K Karabut, A. B., 178, 253 Kasagi, J., 339 Kelly, J. C , 822 Khachaturov, B., 84 Kim, Y. E., 703, 711, 718 Kitamura, A., 218 Koltick, D. S., 703 Kornilova, A. A., 521, 530 Kowalski, L., 269, 879, 888 Kozima, H., 769 Krakov, V., 84 Kuribayashi, S., 339
L Lesin, S., 84 Letts, D., 269 Lewis, E., 854 Lewis, E. H., 304 Li, X. Z., 351, 635, 822 Lipson, A., 128 Lipson, A. G., 324, 379 Liu, B., 351, 635 Lochak, G., 421, 787, 838 Lorusso, G., 405 Lyakhov, B., 128 Lyakhov, B. F., 324
M Mancini, A., 108 Marchesini, M., 108 Marini, P., 108, 392 Mastromatteo, U., 108 McKubre, M. C. H., 23 Miley, G., 128 Miley, G. H., 324, 379, 822 Minari, T., 218 Mitin, A., 128 Mizuno, T., 161, 312 Mo, Yu. X., 351 Montalbano, V., 70, 405, 414 Moon, D. D., 868 Mosier-Boss, P. A., 359
N Nagel, D. J., 23, 60 Nakamura, M., 108 Nekrasov, V. V., 374 Nishio, R., 218 Novaxo, E., 108
o Odintsov, A., 530 Okumura, H., 694 Oriani, R. A., 281, 295 Osman, F., 822
P Passell, T. O., 147, 718 Pavlovich, V. N., 530 Prez-Pariente, J., 554 Piantelli, F., 70, 405, 414 Pletnikov, E. V., 818 Pryakhin, E. A., 537
Q Quercia, P.,
108
897
R Rambaut, M., 798 Ratis, Yu. L., 459 Reifenberger, R. G., 703 Righi, E., 108 Rothwell, J., 871 Roussetski, A. S., 274, 324 Rukhadze, A. A., 806, 838
s Sakano, M., 339 Savvatimova, I. B., 438 Sesftel, F., 161 Sharkov, V. F., 374 Sona, R G., 108 Song, B., 102 Spallone, A., 108, 392 Stanghini, C , 405 Stefano, V. D., 108, 392 Storms, E., 11 Stringham, R., 1, 238 Szpak, S., 359
T Takahashi, A., 312, 730 Taniike, A., 218 Tashirev, A. B., 530 Terada, Y., 339 Tian, J., 102, 351 Toimela, T., 622 Trenta, G., 108 Triassi, A., 485
Tryapitsina, G. A., 537 Tsirlin, M., 84 Tsuchiya, K.-L, 694
u Urutskoev, L., 421 Urutskoev, L. I., 806, 838
V Veronesi, S., 70, 405, 414 Vitiello, G., 587 Vysotskii, V. I., 505, 521, 530
w Wallace, K., 1 Wang, X. M., 351 Wei, Q. M., 351, 635 Weng, Z. K., 102
X Xiao, Z. J.,
102
Y Yamazaki, N.,
339
z Zhao, X. L., 102 Zheng, S. X., 351, 635 Zhidkova, I. E., 459 Zilov, T., 84 Zubarev, A. L., 703, 711
clondensed mlatter nluclear slcience The
International
Conference
on
C o n d e n s e d M a t t e r N u c l e a r Science is held annually o n a d i f f e r e n t c o n t i n e n t every t i m e . This volume documents the proceedings of the I I t h conference held in Marseilles, France. It includes articles that indicate the c u r r e n t position of the condensed matter nuclear science field.
W i t h an extensive collection o f articles, this volume is indispensable since very few papers related t o this field are published in scientific journals.
6012 he ISBN 981 -256-840-6
orld Scientific YEARS OF P U B L I S H I N G I
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