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LIQUID SCINTILLATION COUNTING RECENT DEVELOPMENTS EDITED BY Philip E. Stanley Waite Agricultural Research Institute Department of Agricultural Biochemistry University of Adelaide Glen Osmond, South Australia Bruce A. Scoggins Howard Florey Institute of Experimental Physiology and Medicine University of Melbourne Parkville, Victoria, Australia Academic Press, Inc. New York and London 1974 A Subsidiary of Harcourt Brace Jovanovich, Publishers COPYRIGHT © 1974, BY ACADEMIC PRESS, INC. ALL RIGHTS RESERVED. NO PART OF THIS PUBLICATION MAY BE REPRODUCED OR TRANSMITTED IN ANY FORM OR BY ANY MEANS, ELECTRONIC OR MECHANICAL, INCLUDING PHOTOCOPY, RECORDING, OR ANY INFORMATION STORAGE AND RETRIEVAL SYSTEM, WITHOUT PERMISSION IN WRITING FROM THE PUBLISHER. ACADEMIC PRESS, INC. Ill Fifth Avenue, New York, New York 10003 United Kingdom Edition published by ACADEMIC PRESS, INC. (LONDON) LTD. 24/28 Oval Road, London NW1 LIBRARY OF CONGRESS CATALOG CARD NUMBER: 73-7444 PRINTED IN THE UNITED STATES OF AMERICA Preface The International Symposium on Liquid Scintillation Counting was held from 20th - 22nd August, 1973 at the Wentworth Hotel, Sydney, Australia. One hundred delegates attended the Symposium and discussed the current status of many recent developments in liquid scintillation spectrometry. The decision to hold a Symposium of this type in Australia was based on what was considered a need for a forum to discuss both the theoretical and applied aspects of liquid scintillation counting. In Australia, the technique of liquid scintillation spectrometry has had an important role in the majority of universities, laboratories and institutes involved in nuclear physics, biomédi- cal science, geophysics, and agriculture. However, geographical isolation and the fact that scientists utilizing the same basic principles and equipment work in many different disciplines means that there is seldom an opportunity to exchange ideas. It was hoped that by inviting scientists who are research leaders in the varied and important aspects of liquid scintillation spectrome- try overseas and within Australia, a suitable interchange of information could be achieved. In this regard our hopes were truly fulfilled. We were pleased that Dr. J. L. Symonds, Acting Director of the Australian Atomic Energy Commission Research Establishment, could be present to open the Symposium. It was a special pleasure and privilege to have Dr. John Birks present at the Symposium on the occasion of his 25th Jubilee in the Realm of the Scintillation Process, and to present a plenary lecture covering his endeavors in the field. A different aspect of John Birk's ingenuity is seen in his closing remarks which so skillfully analyzed the "state of the art." The other plenary lecturers, Dr. Yutaka Kobayashi, Dr. Harley Ross, and Professor Eric Schräm, were to provide expertise and a solid basis for discus- sion in three important areas of scintillation counting. Our colleague, Dr. John Coghlan, took the unenviable responsibility of organizing and chairing the Workshop Session. A panel consisting of Drs. Bransome, Kobayashi, Laney, Ross, and Schräm ably discussed a number of contentious issues which arose during the Symposium. An edited synopsis of the Workshop Session is included in this volume. Also included in this book is the paper ix PREFACE of Dr. Laumas (India) who regrettably was unable to attend the meeting because of illness. To our plenary lecturers, workshop participants, session chairman and to those contributing to the published proceedings, we extend our grateful thanks for making the Symposium a success. We gratefully acknowledge the active participation of Mr. Peter Annand, Marketing Director of Searle Nucleonics, a Division of Searle Australia Pty. Ltd., who with us conceived the idea of holding the Symposium in Australia. As a member of the organizing committee his encouragement and moral support during the Symposium were of great value. Also, we wish to thank Searle Nucleonics for their generous financial support which enabled us to carry through a long gestation period and then to give birth to the actual meeting. Convention Organizers Pty. Ltd. handled most professionally the logistical aspects of the Symposium for us. Of their staff, we are greatly indebted to Mrs. Karen Forbes who carried out seemingly impossible tasks with efficiency and willingness. We wish to thank Miss Jan Peavy of the Waite Agricultural Research Institute for valuable secretarial assistance and especially for her preparation of the abstracts. The assistance of the secretar- ial staff at the Howard Florey Institute is also acknowledged and also that of the many other people who in various ways contributed to the Symposium. Finally, we wish to record our sincere appreciation to Academic Press for their assistance and advice in preparing this volume for publication. Philip E. Stanley Bruce A. Scoggins x List of Contributors Adu, J. K., Department of Agricultural Biochemistry and Soil Science, Waite Agricultural Research Institute, The University of Adelaide, Glen Osmond, South Australia 5064 Apelgot, S., Fondation Curie-Institut du Radium 11, Rue P. et M. Curie et 26, Rue d'Ulm. 75231, Paris Baucom, Terry L., Department of Biochemistry, University of Georgia, Athens, Georgia 30602 Birks, J. B., The Schuster Laboratory, University of Manchester, U.K. Bransome, E. D. Jr., Division of Metabolic and Endocrine Disease, Medical College of Georgia, Augusta, Georgia Butkus, Aldona, Howard Florey Institute of Experimental Physiology and Medicine, University of Melbourne, Parkville, 3052, Australia Calf, G. E., Australian Atomic Energy Commission, Lucas Heights, N.S.W. 2232 Carter, T. P., Department of Experimental Pathology, University of Birmingham Medical School, Birmingham B15 2TJ. England Chemama, R., Fondation Curie-Institut du Radium 11, Rue P. et M. Curie et 26, Rue d'Ulm. 75231, Paris Church, V. E., Australian Atomic Energy Commission Research Establish- ment, Lucas Heights, N.S.W. Coghlan, John P., Howard Florey Institute of Experimental Physiology and Medicine, University of Melbourne, Parkville, 3052, Australia Dodeja, Nancy, Endocrine-Metabolic Unit, Department of Medicine, Peter Bent Brigham Hospital and Harvard Medical School, Boston, Massachusetts xi LIST OF CONTRIBUTORS Downes, A. M., C.S.I.R.O., Division of Animal Physiology, Ian Clunies Ross Research Laboratory, Prospect, N.S.W., Australia Ediss, C, Division of Bionucleonics and Radiopharmacy, University of Alberta, Edmonton, Alberta, Canada Everett, L. J., Research Manager, Packard Instrument Company, Inc., 2200 Warrenville Road, Downers Grove, Illinois 60515 Faini, George, J., Department of Biochemistry, University of Georgia, Athens, Georgia 30602 Fardy, John J., Chemical Technological Division, Australian Atomic Energy Commission, Private Mail Bag, Sutherland, N.S.W. 2232, Australia Fraser, I., The University of Sydney, Department of Physical Chemistry, Sydney, Australia Frilley, M., Fondation Curie-Institut du Radium 11, Rue P. et M. Curie et 26, Rue d'Ulm. 75231, Paris Gezing, Michael, Amersham/Searle Corp., Arlington Heights, Illinois Gillespie, R., The University of Sydney, Department of Physical Chemistry, Sydney, Australia Gresham, P. A., Department of Experimental Pathology, University of Birmingham Medical School, Birmingham B15 2TJ, England Hartley, P. E., Australian Atomic Energy Commission, Research Establish- ment, Lucas Heights, N.S.W. 2232 Jackson, N., C.S.I.R.O. Division of Animal Genetics, Epping, N.S.W. Australia Kaartinen, N., Consultant, Packard Instrument Pty, Ltd., 2-4 Vale Street, St. Kilda, Victoria, 3182 Australia Kisieleski, Walter, Argonne National Laboratory, Argonne, Illinois 60439 Kobayashi, Yutaka, The Worcester Foundation for Experimental Biology, Shrewsbury, Massachusetts 01545 Kreveld, P., District Manager, Packard Instrument Pty, Ltd., 2-4 Vale Street, St. Kilda, Victoria, 3182 Australia Laney, Barton H., Searle Analytic Inc., Des Plaines, Illinois xii LIST OF CONTRIBUTORS Laumas, K. R., Department of Reproductive Biology, All-India Institute of Medical Sciences, New Delhi 110016, India Lee, John, Department of Biochemistry, University of Georgia, Athens, Georgia 30602 Lowenthal, G. C, Australian Atomic Energy Commission Research Estab- lishment, Lucas Heights, N.S.W. 2232 Malcolm, Philip J., Biometry Section, Waite Agricultural Research Institute, The University of Adelaide, Glen Osmond, South Australia Maudsley, David V., The Worcester Foundation for Experimental Biology, Shrewsbury, Massachusetts 01545 Maxwell, C. A., C.S.I.R.O., Division of Animal Physiology, Ian Clunies Ross Research Laboratory, Prospect, N.S.W., Australia Murphy, Charles L., Department of Biochemistry, University of Georgia, Athens, Georgia 30602 Neary, Michael P., Geochronology Laboratory, The University of Georgia, Athens, Georgia 30602 Noakes, John E., Geochronology Laboratory, The University of Georgia, Athens, Georgia 30602 Noujaim, A. A., Division of Bionucleonics and Radiopharmacy, University of Alberta, Edmonton, Alberta, Canada Oades, J. M., Department of Agricultural Biochemistry and Soil Science, Waite Agricultural Research Institute, The University of Adelaide, Glen Osmond, South Australia 5064 Painter, Kent, Amersham/Searle Corporation, Arlington Heights, Illinois* Polach, Harry A., The Australian National University, Radiocarbon Dating Laboratory, Canberra, Australia Rahman, S. A., Department of Reproductive Biology, All-India Institute of Medical Sciences, New Delhi, 110016, India * Present address: Micromedic Diagnostics, Inc. P.O. Box 464 Fort Collins, Colorado xiii LIST OF CONTRIBUTORS Rasmussen, G. T., Analytic Chemistry Division, Oak Ridge National Laboratory Oak Ridge, Tennessee 37830 Ross, H. H., Analytic Chemistry Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee Schräm, Eric, University of Brussels, Belgium Scoggins, Bruce A., Howard Florey Institute of Experimental Physiology and Medicine, University of Melbourne, Parkville, 3052, Australia Sharpe, S. E. Ill, Division of Metabolic and Endocrine Disease, Medical College of Georgia, Augusta, Georgia Sharry, L. F., C.S.I.R.O., Division of Animal Physiology, Ian Clunies Ross Research Laboratory, Prospect, N.S.W., Australia Spaulding, James D., Geochronology Laboratory, The University of Georgia, Athens, Georgia 30602 Stanley, Philip E., Department of Agricultural Biochemistry, Waite Agricultural Research Institute, The University of Adelaide, Glen Osmond, South Australia* Temple, R. B., The University of Sydney, Department of Physical Chemistry, Sydney, Australia ten Haaf, F. E. L., Nuclear Applications Laboratory, N. V. Philips' Gloeilampenfabrieken Eindhoven, The Netherlands Underwood, Richard H., Endocrine-Metabolic Unit, Department of Medicine, Peter Bent Brigham Hospital and Harvard Medical School, Boston, Massachusetts Wiebe, L. I., Division of Bionucleonics and Radiopharmacy, University of Alberta, Edmonton, Alberta, Canada * Present address: Department of Clinical Pharmacology The Queen Elizabeth Hospital Woodville, South Australia 5011 xiv TOWARDS AN UNDERSTANDING OF THE SCINTILLATION PROCESS IN ORGANIC MOLECULAR SYSTEMS J. B. Birks The Schuster Laboratory, University of Manchester, U.K. Introduction» ^y interest in organic scintillators began just 25 years ago, and I have been interested in them ever since. Silver jubilees are rare occasions« I propose to celebrate this particular anniversary by departing from the usual pattern of review papers and restricting this talk to an account of my own personal voyage of discovery« There have been many other contributors to the field, and accounts of their work are to be found in my books (l-5l and other review articles C6-23] • The story opens in 194-8 in the Department of Natural Philosophy at the University of Glasgow where I was com- pleting my Ph.D. studies on the microwave properties of ferromagnetic materials. All my colleagues were engaged in research related to nuclear physics, and Professor P. I. Dee suggested that I should seek a suitable project in this area and join the "team". In one of the labor- atories I found an unusual instrument consisting of a large naphthalene crystal attached to a photoraultiplier. Its designer, G. M. Lewis, explained that this was an organic scintillation counter of the type discovered the previous year by H. Kallmann. "Ionizing radiations impinge on the scintillator and produce light flashes or scintillations", he explained. "Why?", I asked. "We don't know", he replied. The next day I informed Professor Dee of my new project, the study of the scint- illation process in organic molecular systems. 25 years later I am still working on it. It was a much tougher assignment than I realised, but en route there has been a lot of interesting physics. We've found answers to many of the original questions, and in turn we've uncovered many new questions that we didn't know existed. Organic crystals. Kallmann's first organic scintillator Ï194-7) was a naphthalene crystal, grown from moth-balls 1 J. B. BIRKS bought in a chemist's shop in war-ravaged Berlin. In 194.8 P. R. Bell reported that crystalline anthracene had a scintillation yield about 5 times that of crystalline naphthalene. 25 years later crystalline anthracene remains the most efficient organic scintillator in general use. unfortunately it cannot be grown in such large crystals as naphthalene. It was to overcome this limitation that 1 decided to study the scintillations from naphthalene crystals ^con- taining different small concentrations of anthracene \ZU\ . There is an efficient solvent-solute energy transfer process in organic crystal solutions due to exciton migration and transfer, and above a certain anthracene concentration the scintillation yield equals and even exceeds that of a pure anthracene crystal. Because of the elimination of the self-absorption which occurs in anthracene crystals [65] , mixed organic crystals have the highest scintillation yields of any known organic mole- cular systems \103 ♦ Moreover they can readily be grown in volumes as large as pure naphthalene crystals. Despite these virtues mixed organic crystals have found little practical application, because of the parall- el discovery of two more convenient types of organic solution scintillator. M. Ageno, M. Chiozzotto and R. Querzoli discovered organic liquid solution scintillators in 1949, and in 1950 M. G. Schorr and F. L. Torney found the first organic plastic solution scintillators. Although organic liquid and plastic solutions have lower scintillation yields than organic crystal solutions, they suffer from no limitations of size and shape. Huge sheets and massive blocks of plastic scintillator are used in high energy physics and whole-body counting, and kilo- litre tanks of liquid scintillator are used in cosmic ray and neutrino research. There is no need to remind this Symposium of the advantages of liquid scintillators for the direct incorporation and assay of radio-active specimens using the internal counting technique. Scintillation response. The next topic which I decided to study was the relative scintillation response to different types of ionizing radiation. The scintillation response of an organic scintillator to 5 MeV oC -particles is only about 10 per cent of that to ß> -particles of the same 2

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