Charged Particle and Photon Interactions with Matter C he mi c a I, Physic oc h emi c a I, a nd B iolog i ca I Consequences with Applications edited by A. Mozurnder University of Notre Dame Notre Dame, Indiana, USA. Y. Hatano Tokyo Institute of Technology Tokyo, Japan MARCEL MARCEL DEKKER, INC. ~ DEKKER NEW YORK BASEL Copyright © 2004 by Taylor & Francis Group, LLC Although great care has been taken to provide accurate and current information, neither the author(s) nor the publisher, nor anyone else associated with this publication, shall be liable for any loss, damage, or liability directly or indirectly caused or alleged to be caused by this book. The material contained herein is not intended to provide specific advice or recommendations for any specific situation. Trademark notice: Product or corporate names may be trademarks or registered trademarks and are used only for identification and explanation without intent to infringe. 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Neither this book nor any part may be reproduced or transmitted in any form or by any means, electronic or mechanical, including photocopying, microfilming, and recording, or by any information storage and retrieval system, without permission in writing from the publisher. Current printing (last digit): 10987654321 PRINTED IN THE UNITED STATES OF AMERICA Copyright © 2004 by Taylor & Francis Group, LLC Preface The purpose of this work is to present a coherent account of high-energy charged particle and photon interactions with matter, in vivo and in vitro, that will be of use to both students and practicing scientists and engineers. The book encompasses not only radiation chemis- try and photochemistry, but also other aspects of charged particle and photon interactions, such as radiation physics, radiation biochemistry, radiation biology , and applications to medical and engineering scien ces and to radiation syn thesis and processing and food irradiation. Any phenomenon of ionization and excitation induced by charged particle and photon interactions with matter is considered of interest, since information on the interactions of photons with matter help us understand the interactions of charged particles with matter. Further, the study of the interactions of high-energy photons, particularly in the vacuum ultraviolet–soft X-ray (VUV-SX) region, is of great importance in bridging the areabetweenphotochemistryandradiationchemistry(seeChapter5).Throughoutthe book a major aim has been to elucidate the physical and chemical principles involved in applications of significance to practicing scientists and engineers. We have secured the foremost workers in their respective areas to contribute chapter articles in a manner that ensures contact with adjacent disciplines, keeping in mind the needs of the general reader- ship. Since its inception, radiation effects have had ramification s in various fields, which sometimes use different technical langua ge, units, etc. Reviews condense the subject matter while amplifying important points and bring these up-to-date for students and researchers. In a field that is developing as rapidly as radiation effects in vivo and in vitro, there is a need for periodic summaries in the form of a book. In the present millenium, a great need has developed for in-depth studies with a balance of experiment, theory, and application. Yet, chapters written by severa l authors in the same book may use different styles, outlooks, or even notations. We have paid particular attention to these factors and have striven to make the presentations uniform. By its very nature this book is interdisciplinary. The first eleven chapters delineate the fundamentals of radiat ion physics and radiation chemistry that are common to all irra- diation effects. Chapters 12 and 13 deal with specific liquid systems, while Chapter 14 is concerned with LET effects. Chapters 1 5 to 18 describe biological and medical consequences of photon and charged-particle irradiation. The rest of the book is much more applied in character, starting with irradiated polymers in Chapter 19 and ending with applications of heavy ion impact in Chapter 27. Our aim has been to provide a self-contained volume with sufficient information and discussion to take the reader to the frontier of investigation. The level of presentation is at the advanced undergraduate level, so that undergraduates, graduate students, researchers, Copyright © 2004 by Taylor & Francis Group, LLC and practicing professionals may all benefit from it. It is assumed that the reader has some knowledge of chemistry or biology or physics but is not necessarily versed in the properties of high-energy radiation. It is our pleasure and privilege to thank our friends and colleagues all over the world who have contributed to our understanding of the high-energy charged particle and photon interactions with matter. A. Mozumder Y. Hatano Copyright © 2004 by Taylor & Francis Group, LLC Contents Preface Chapter1Introduction A. Mozumder and Y. Hatano Chapter2InteractionofFastChargedParticleswithMatter A. Mozumder Chapter 3 Ionization and Secondary Electron Production by Fast ChargedParticles Larry H. Toburen Chapter 4 Modeling of Physicoch emical and Chemical Processes intheInteractionsofFastChargedParticleswithMatter Simon M. Pimblott and A. Mozumder Chapter 5 Interaction of Photons with Molecules: Photoabsorption, Photoionization,andPhotodissociationCrossSections Noriyuki Kouchi and Y. Hatano Chapter 6 Reactions of Low-Energy Electrons, Ions, Excited Atoms and Molecules, and Free Radicals in the Gas Phase as Studied by PulseRadiolysisMethods Masatoshi Ukai and Y. Hatano Chapter 7 Studies of Solvation Using Electrons and Anions in AlcoholSolutions Charles D. Jonah Chapter8ElectronsinNonpolarLiquids Richard A. Holroyd Chapter 9 Interactions of Low-Energy Electrons with Atomic and MolecularSolids Andrew D. Bass and Le ´ on Sanche Copyright © 2004 by Taylor & Francis Group, LLC Chapter 10 Electron–Ion Recombination in Condensed Matter: GeminateandBulkRecombinationProcesses Mariusz Wojcik, M. Tachiya, S. Tagawa, and Y. Hatano Chapter11RadicalIonsinLiquids Ilya A. Shkrob and Myran C. Sauer, Jr. Chapter 12 The Radiation Chemistry of Liquid Water: Principles and Applications G. V. Buxton Chapter 13 Photochemistry and Radiation Chemistry of Liquid Alkanes: FormationandDecayofLow-EnergyExcitedStates L. Wojnarovits Chapter14RadiationChemicalEffectsofHeavyIons Jay A. LaVerne Chapter 15 DNA Damage Dictates the Biological Consequences of IonizingIrradiation:TheChemicalPathways William A. Bernhard and David M. Close Chapter16Photon-InducedBiologicalConsequences Katsumi Kobayashi Chapter17TrackStructureStudiesofBiologicalSystems Hooshang Nikjoo and Shuzo Uehara Chapter18MicrodosimetryandItsMedicalApplications Marco Zaider and John F. Dicello Chapter19ChargedParticleandPhoton-InducedReactionsinPolymers S. Tagawa, S. Seki, and T. Kozawa Chapter 20 Charged Particle and Photon Interactions in Metal Clusters andPhotographicSystemStudies Jacqueline Belloni and Mehran Mostafavi Chapter 21 Application of Radiati on Chemical Reactions to the Molecular DesignofFunctionalOrganicMaterials Tsuneki Ichikawa Chapter 22 Applications to Reaction Mechanism Studies of Organic Systems Tetsuro Majima Chapter23ApplicationofRadiationChemistrytoNuclearTechnology Yosuke Katsumura Copyright © 2004 by Taylor & Francis Group, LLC Chapter24ElectronBeamApplicationstoFlueGasTreatment Hideki Namba Chapter 25 Ion-Beam Therapy: Rationale, Achievements, and Expectations Andre ´ Wambersie, John Gueulette, Dan T. L. Jones, and Reinhard Gahbauer Chapter26FoodIrradiation Jo ´ zsef Farkas Chapter 27 New Applications of Ion Beams to Material, Space, and BiologicalScienceandEngineering Mitsuhiro Fukuda, Hisayoshi Itoh, Takeshi Ohshima, Masahiro Saidoh, and Atsushi Tanaka Copyright © 2004 by Taylor & Francis Group, LLC Contributors Andrew D. Bass University of Sherbrooke, Sherbrooke, Que ´ bec, Canada Jacqueline Belloni UMR CNRS–UPS, Universite ´ Paris-Sud, Orsay, France William A. Bernhard University of Roches ter, Rochester, New York, U.S.A. G. V. Buxton University of Leeds, Leeds, England David M. Close East Tennessee State University, Johnson City, Tennessee, U.S.A. John F. Dicello Johns Hopkins University School of Medicine, Baltimore, Maryland, U.S.A. Jo ´ zsef Farkas Szent Istva ´ n University, Budapest, Hungary Mitsuhiro Fukuda Japan Atomic Energy Research Institute, Takasaki, Gunma, Japan Reinhard Gahbauer Ohio State University, Columbus, Ohio, U.S.A. John Gueulette Universite ´ Catholique de Louvain, Brussels, Belgium Y. Hatano Tokyo Institute of Technology, Tokyo, Japan Richard A. Holroyd Brookhaven National Laboratory, Upton, New York, U.S.A. Tsuneki Ichikawa Hokkaido University, Sapporo, Japan Hisayoshi Itoh Japan Atomic Energy Research Institute, Takasaki, Gunma, Japan Charles D. Jonah Argonne National Laboratory, Argonne, Illinois, U.S.A. Dan T. L. Jones iThemba Laboratory for Accelerator Based Sciences, Somerset West, South Africa Yosuke Katsumura The University of Tokyo, Tokyo, Japan Katsumi Kobayashi High Energy Accelerator Research Organization, Tsukuba, Japan Noriyuki Kouchi Tokyo Institute of Technology, Tokyo, Japan Copyright © 2004 by Taylor & Francis Group, LLC T. Kozawa Osaka University, Osaka, Japan Jay A. LaVerne University of Notre Dame, Notre Dame, Indiana, U.S.A. Tetsuro Majima Osaka University, Osaka, Japan Mehran Mostafavi UMR CNRS–UPS, Universite ´ Paris-Sud, Orsay, France A. Mozumder University of Notre Dame, Notre Dame, Indiana, U.S.A. Hideki Namba Japan Atomic Energy Research Institute, Takasaki, Gunma, Japan Hooshang Nikjoo Medical Research Council, Harwell, Oxf ordshire, England Takeshi Ohshima Japan Atomic Energy Research Institute, Takasaki, Gunma, Japan Simon M. Pimblott University of Notre Dame, Notre Dame, Indiana, U.S.A. Masahiro Saidoh Japan Atomic Energy Rese arch Institute, Takasaki, Gunma, Japan Le ´ on Sanche* University of Sherbrooke, Sherbrooke, Que ´ bec, Canada Myran C. Sauer, Jr. Argonne National Laboratory, Argonne, Illinois, U.S.A. S. Seki Osaka University, Osaka, Japan IIya A. Shkrob Argonne National Laboratory, Argonne, Illinois, U.S.A. M. Tachiya National Institute of Advanced Industrial Science and Technology (AIST), Tsukuba, Japan S. Tagawa Osaka University, Osaka, Japan Atsushi Tanaka Japan Atomic Energy Research Institute, Takasaki, Gunma, Japan Larry H. Toburen East Carolina University, Greenville, North Carolina, U.S.A. Shuzo Uehara Kyushu University, Fukuoka, Japan Masatoshi Ukai Tokyo University of Agriculture and Technology, Tokyo, Japan Andre ´ Wambersie Universite ´ Catholique de Louvain, Brussels, Belgium Mariusz Wojcik Technical University of Lodz, Lodz, Poland L. Wojnarovits Hungarian Academy of Sciences, Budapest, Hungary Marco Zaider Memorial Sloan-Kettering Cancer Center, New York, N ew York, U.S.A. * Canada Chair in the Radiation Sciences. Copyright © 2004 by Taylor & Francis Group, LLC 1 Introduction A. Mozumder University of Notre Dame, Notre Dame, Indiana, U.S.A. Y. Hatano Tokyo Institute of Technology Tokyo, Japan 1. EARLY INVESTIGATIONS The effect of visible and UV-light on matter, in vitro and in vivo, has a long history. In this sense photochemistry and photobiology are forerunners, respectively, of rad iation chem- istry and radiation biology. The involv ement of visible light on the discoloration of dyes and on the growth and transformation of plants has been known since time immemorial. In the 18th century the action of light on silver salts was definitely established, culminating inrudimentaryphotographyinthemid-19thcentury(seeChapter20).Somequalitative understanding of photochemical action was obtained by Grottus (1817) and by Draper (1841) in which it was stated that only the absorbed light can be effective in bringing out chemical transformation and that the rate of chemical change should be proportional to the light intensity. With the advent of the quantum theory, Einstein (1912) formalized what has since been called the first law of photochemistry, i.e., only one quantum of light is absorbed per reacting molecule. This actually applies to the primary process and at relatively low light intensity to which all early studies were confined. Later work at high intensity provided by lasers has necessitated some modification of this important law. As not all primary activations are observable, the idea of the quantum yield or the number of molecules transformed per quantum of light absorbed was introduced by Bodenstein (1913) who also noticed chain reactions in the combination of hydrogen and chlorine giving quantum yields many orders of magnitude greater than 1. It is clear that, along with the discovery of x-rays in 1895, Roentgen also found the chemical action of ionizing radiation. He drew attention to the similarity of the photo- graphic effect induced by light and x-rays. Application to medicine appeared very quickly, followed by industrial applications. However, this field of investigation remained nameless until Milton Burton, in 1942, christened it ‘‘radiation chemistry’’ to separate it from radio- chemistry which is the study of radioac tive nuclei. Historical and classical work in radia- tion chemistry has been reviewed by Mozumder elsewhere [1]. Here we will only make a few brief remarks. Copyright © 2004 by Taylor & Francis Group, LLC [...]... a CRC handbook edited by Ferradini and Jay-Gerin [7] Further, specific applications to atomic and molecular processes in reactive plasmas have been summarized by Hatano [8] Chapters 15 through 27 of this book are involved with radiation applications including radiobiological, medical, and industrial applications In addition, Chapters 16, 19, and 20 discuss, in considerable details, the effects and applications... INTERACTIONS OF HIGH-ENERGY CHARGED PARTICLES AND PHOTONS WITH MATTER In the interactions of high-energy incident particles, i.e., photons, electrons, heavy charged particles (or positive and negative ions), and other particles, with matter, the succession of events that follow the absorption of their energies has been classified into three characteristic temporal stages: physical, physico-chemical, and chemical... be correct, absolute, and comprehensive, is of great importance and is helpful for understanding the essential features of the fundamental processes in these two stages [21] Such information is available both experimentally and theoretically in the gas-phase (see Chapter 3), but in some cases also in the condensed-phase as well (see Chapter 9) Cross sections for the ionization and excitation of molecules... electrons and positrons of appropriate energy Electrons of various energy are the most important sources as primary radiations in the laboratory and in the industry [1], and also as secondary radiations in any form of ionizing event Other often-used irradiations include x-rays, radioactive radiations (a, h, or g), protons, deuterons, various accelerated stripped nuclei, and fission fragments X-rays differ... recent progress in the experimental and theoretical investigations of electron–molecule collision processes [21] The experimental and theoretical investigations of the physical, physico-chemical, and chemical stages of the interactions of high-energy incident particles with matter have made a remarkable contribution to recent progress in fundamental studies of the static and dynamic behavior of reactive... Hatano, Y In: Handbook of Radiation Chemistry; Tabata, Y Ito, Y., Tagawa, S., Eds.; CRC Press: Boca Raton, 1991 19 Hatano, Y In: Electronic and Atomic Collisions; Lorents, D.C Meyerhof, W.E., Peterson, J.R., Eds.; Elsevier: Amsterdam, 1986; 153 pp 20 Hatano, Y Aust J Phys 1997, 50, 615 21 Inokuti, M., Ed In: Atomic and Molecular Data for Radiotherapy and Radiation Research; IAEA-TECDOC-799 IAEA: Vienna,... 1960s Spinks and Woods [5] have summarized radiation-induced synthesis and processing; Mozumder [1] has also given a brief account of various applications to science and industry including dosimetry, food irradiation, waste treatment, sterilization of medical equipment, etc Salient features of radiation chemistry, both in the gaseous and condensed phases, have been discussed in the CRC Handbook of Radiation... exponential and a power-law extrapolation beyond the upper limit of experiments were used Later, LaVerne and Mozumder [31], requiring transparency in the visible region and the correct number of valence electrons (8.2 for water), opted for the power-law with index 3.8, close to the theoretical limit of 4.0 for valence electrons The contribution of the K electrons remains the same as in the gas phase and are,... scattering in liquid water, forcing many investigators to use gas phase data for that purpose Typical values of computed ranges in water are f550 nm for 5-keV electrons, f0.5 mm for 5-MeV protons, and f0.04 mm for 5-MeV a-particles Ranges of slow heavy ions and fission fragments are nearly proportional to energy, because the increase of stopping power in relation to slowing down is largely compensated by... particle range [37] A collision-by-collision approach was introduced by Mozumder and LaVerne [38] for range straggling of low-energy electrons without the consideration of large-angle elastic scattering The probability density of pathlength x for the first collision is given by P1(x) = KÀ1 exp(Àx/K), where the mean free path K is computed from the same differential cross-section of energy loss as used . 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