Charged Particle and Photon Interactions with Matter Recent Advances, Applications, and Interfaces

Edited by Yoshihiko Hatano Yosuke Katsumura A. Mozumder

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Contents

Preface...... xi Editors ...... xiii Contributors ...... xv

Chapter 1 Introduction ...... 1 Yoshihiko Hatano, Yosuke Katsumura, and Asokendu Mozumder

Chapter 2 Oscillator Strength Distribution of Molecules in the Gas Phase in the Vacuum Ultraviolet Range and Dynamics of Singly Inner-Valence Excited and Multiply Excited States as Superexcited States ...... 9 Takeshi Odagiri and Noriyuki Kouchi

Chapter 3 Electron Collisions with Molecules in the Gas Phase ...... 27 Hiroshi Tanaka and Yukikazu Itikawa

Chapter 4 Time-Dependent Density-Functional Theory for Oscillator Strength Distribution ...... 65 Kazuhiro Yabana, Yosuke Kawashita, Takashi Nakatsukasa, and Jun-Ichi Iwata

Chapter 5 Generalized Oscillator Strength Distribution of Liquid Water ...... 87 Hisashi Hayashi and Yasuo Udagawa

Chapter 6 New Directions in W-Value Studies ...... 105 Isao H. Suzuki

Chapter 7 Positron Annihilation in Radiation Chemistry ...... 137 Tetsuya Hirade

Chapter 8 Muon Interactions with Matter ...... 169 Khashayar Ghandi and Yasuhiro Miyake

Chapter 9 Electron Localization and Trapping in Hydrocarbon Liquids ...... 209 Gordon L. Hug and Asokendu Mozumder

vii viii Contents

Chapter 10 Reactivity of Radical Cations in Nonpolar Condensed Matter ...... 237 Ortwin Brede and Sergej Naumov

Chapter 11 Radiation Chemistry and Photochemistry of Ionic Liquids...... 265 Kenji Takahashi and James F. Wishart

Chapter 12 Time-Resolved Study on Nonhomogeneous Chemistry Induced by Ionizing Radiation with Low Linear Energy Transfer in Water and Polar Solvents at Room Temperature ...... 289 Vincent De Waele, Isabelle Lampre, and Mehran Mostafavi

Chapter 13 Radiation Chemistry of Liquid Water with Heavy Ions: Steady-State and Pulse Radiolysis Studies ...... 325 Shinichi Yamashita, Mitsumasa Taguchi, Gérard Baldacchino, and Yosuke Katsumura

Chapter 14 Radiation Chemistry of Liquid Water with Heavy Ions: Monte Carlo Simulation Studies ...... 355 Jintana Meesungnoen and Jean-Paul Jay-Gerin

Chapter 15 Radiation Chemistry of High Temperature and Supercritical Water and Alcohols ...... 401 Mingzhang Lin and Yosuke Katsumura

Chapter 16 Radiation Chemistry of Water with Ceramic Oxides ...... 425 Jay A. LaVerne

Chapter 17 Ionization of Solute Molecules at the Liquid Water Surface, Interfaces, and Self-Assembled Systems ...... 445 Akira Harata, Miki Sato, and Toshio Ishioka

Chapter 18 Low-Energy Electron-Stimulated Reactions in Nanoscale Water Films and Water–DNA Interfaces ...... 473 Gregory A. Grieves, Jason L. McLain, and Thomas M. Orlando

Chapter 19 Physicochemical Mechanisms of Radiation-Induced DNA Damage ...... 503 David Becker, Amitava Adhikary, and Michael D. Sevilla

Chapter 20 Spectroscopic Study of Radiation-Induced DNA Lesions and Their Susceptibility to Enzymatic Repair ...... 543 Akinari Yokoya, Kentaro Fujii, Naoya Shikazono, and Masatoshi Ukai Contents ix

Chapter 21 Application of Microbeams to the Study of the Biological Effects of Low Dose Irradiation ...... 575 Kevin M. Prise and Giuseppe Schettino

Chapter 22 Redox Reactions of Antioxidants: Contributions from Radiation Chemistry of Aqueous Solutions ...... 595 K. Indira Priyadarsini

Chapter 23 Computational Human Phantoms and Their Applications to Radiation Dosimetry...... 623 Kimiaki Saito

Chapter 24 Cancer Therapy with Heavy-Ion Beams ...... 647 Koji Noda and Tadashi Kamada

Chapter 25 Nanoscale Charge Dynamics and Nanostructure Formation in Polymers ...... 671 Akinori Saeki, Shu Seki, Kazuo Kobayashi, and Seiichi Tagawa

Chapter 26 Radiation Chemistry of Resist Materials and Processes in Lithography ...... 711 Takahiro Kozawa and Seiichi Tagawa

Chapter 27 Radiation Processing of Polymers and Its Applications ...... 737 Masao Tamada and Yasunari Maekawa

Chapter 28 UV Molecular Spectroscopy from Electron Impact for Applications to Planetary Atmospheres and Astrophysics ...... 761 Joseph M. Ajello, Rao S. Mangina, and Robert R. Meier

Chapter 29 Chemical Evolution on Interstellar Grains at Low Temperatures ...... 805 Kenzo Hiraoka

Chapter 30 Radiation Effects on Semiconductors and Polymers for Space Applications ...... 841 Takeshi Ohshima, Shinobu Onoda, and Yugo Kimoto

Chapter 31 Applications of Rare Gas Liquids to Radiation Detectors ...... 879 Satoshi Suzuki and Akira Hitachi

Chapter 32 Applications of Ionizing Radiation to Environmental Conservation ...... 923 Koichi Hirota

Chapter 33 Applications to Biotechnology: Ion-Beam Breeding of Plants ...... 943 Atsushi Tanaka and Yoshihiro Hase x Contents

Chapter 34 Radiation Chemistry in Nuclear Engineering ...... 959 Junichi Takagi, Bruce J. Mincher, Makoto Yamaguchi, and Yosuke Katsumura Index �� 1025 Preface

The editors of Charged Particle and Photon Interactions with Matter: Chemical, Physicochemical, and Biological Consequences with Applications, eds., A. Mozumder and Y. Hatano, Marcel Dekker, New York (2004), received, soon after its publication, highly supportive comments from international communities of radiation research distributed widely into physics, chemistry, biology, medicine, and technology, and also from other broad areas of science and technology, concerned, in part, with the common phenomena of ionization and excitation of matter. These comments strongly motivated the editors to bring forth a new book that includes more detailed scientic contents, such as recent advances, future perspectives, and information on applications, than those only brie¡y summarized in the rst book. There have been recently two kinds of applications: one is the relatively direct application used mainly by those in radiation research elds, and the other is the interface between radiation research and other elds. Thus, the subtitle of this book is Recent Advances, Applications, and Interfaces. The rst book was published in 2004, and each chapter had referred to papers published before 2000. For this book, a further analysis of recent advances in these respective research elds has been strongly requested. A detailed survey of the applications in these elds, which were introduced only brie¡y in the rst book (in supplementary Chapters 20 through 26, as discussed in Chapter 1, Introduction, in this book) has also been strongly suggested, since the applications have progressed much in recent years. Active interfaces with different research elds have been in evidence. Here, there are two important points of caution in further activating the applications and interfaces in radiation research elds. One is that the applications and interfaces are produced not only in technology but also in basic science. The other is that these applications and interfaces certainly activate the traditionally important core part of radiation research elds, so that the real activation of the core part is essential for the newer applications and interface production in future. With this scope and focus, we began our editorial work for this book. To select the chapters and their authorship, we planned an international symposium on the topics we had in mind. Thus, the symposium on Charged Particle and Photon Interactions with Matter was held as the 7th International Symposium on Advanced Science Research (ASR2007) at the Advanced Science Research Center of the Japan Atomic Energy Agency, Tokai, Japan, November 6–9, 2007, hosted by Y. Katsumura. We wish to record our appreciation to the Japan Atomic Energy Agency and to the Japanese Society for the Promotion of Science for their generous nancial and organiza- tional support (see the special issue for this symposium published in Radiat. Phys. Chem., 77, 1119–1339, 2008). Our plans, together with a list of the candidates for the chapter titles and their authors, were reviewed by scientists and by the editors at Taylor & Francis. These were then modied in accor- dance with their comments and suggestions. In the preparatory stage of our editorial work, we decided that the chapters should be written with the following necessary conditions. We asked the contributors not to overlap with any scientic contents addressed in the previous book. We also requested them to be careful for referring to chapters in the earlier book and to other chapters in that book by other authors. We also asked them to avoid using jargon or special technical terms in their own research elds, since, as clearly shown in the table of contents in this book, the topics and research elds are distributed across a wide variety of scientic and technological elds. If any specialized terminology is used at all, it should be brie¡y explained in plain terms.

xi xii Preface

In Chapter 1, we have incorporated the introduction from the 2004 book and the scientic background that brought it to publication. We also discuss the relation between the scientic contents of the rst book and the present one, as well as the internal relation among the chapters in this book. We, the editors, acknowledge the cooperative work of senior chemistry editor, Barbara Glunn, editorial assistant, Jennifer Derima, and project coordinator, David Fausel, during the initial stages of production. We would also like to thank project editor, Richard Tressider, and project manager, Dr. Sedumadhavan Vinithan, for reviewing the proofs comprehensively just before printing. We are greatly indebted to all the contributors for their scientically excellent contributions to this book and for their cooperation during the editorial work. Finally, we hope that this book, as well as the rst one, will contribute much to the advancement of the research elds that address charged particle and photon interactions with matter, and also, more generally, to great progress in science and technology.

Yoshihiko Hatano Japan Atomic Energy Agency Tokai, Japan

Yosuke Katsumura The University of Tokyo Tokyo, Japan

Asokendu Mozumder University of Notre Dame Notre Dame, Indiana Editors

Yoshihiko Hatano, director general, Advanced Science Research Center, Japan Atomic Energy Agency (JAEA), Tokai, and professor emeritus, Tokyo Institute of Technology, Japan, received his PhD in chemistry from Tokyo Institute of Technology in 1968. Since then he has worked in different capacities in the Department of Chemistry at Tokyo Institute of Technology, as follows: associate professor, 1970–1984; professor, 1984–2000; and dean of the Faculty of Science, 1997–1999. After retiring from Tokyo Institute of Technology in 2000, he worked as a professor in the Department of Molecular and Material Sciences at Kyushu University, Kasuga, Japan, from 2000 to 2003 and as distinguished professor at the Synchrotron Radiation Research Center at Saga University, Saga, Japan, from 2004 to 2009. Since 2005, he has served as the director general of the Advanced Science Research Center, JAEA until his retirement from it at the end of March 2010. Dr. Hatano has been a visiting scientist/professor at many institutions, including the University of Notre Dame, Indiana; the University of Kaiserslautern, Germany; the University of California, Berkeley; the University of Science and Technology of China, Hefei; International Atomic Energy Agency (IAEA); and High Energy Accelerator Research Organization (KEK) at Photon Factory. He has also served in other scientic capacities: chairperson of the Japanese Society of Radiation Chemistry and the Society for Atomic Collision Research; advisory editor of Chemical Physics Letters; coeditor of Charged Particle and Photon Interactions with Matter: Chemical, Physicochemical, and Biological Consequences with Applications, Marcel Dekker, New York (2004); councilor of the International Association for Radiation Research, the Chemical Society of Japan, and the Japanese Society of Synchrotron Radiation Research; and chair/cochair of the International Symposium on Chemical Applications of Synchrotron Radiation, the International Symposium on Electron-Molecule Collisions and Swarms, the International Conference on Photonic, Electronic, and Atomic Collisions; and the International Symposium on Advanced Science Research. His research interests include (1) primary and fundamental processes in charged particle and photon interactions with matter, (2) spectroscopy and dynamics of molecular superexcited states in the dissociative excitation of molecules in photonic or electronic collisions with molecules, (3) electron attachment and recombination, and (4) collisional de-excitation of excited rare gas atoms. He is the author or coauthor of more than 280 refereed journal articles, scientic papers, and books.

Yosuke Katsumura, professor, received his PhD from the Department of Nuclear Engineering and Management, School of Engineering, the University of Tokyo, Tokyo, in 1981. He is also a group leader of Basic Radiation Research, Advanced Science Research Center, Japan Atomic Energy Agency. He has previously worked as a research associate, Nuclear Engineering Research Laboratory, 1972–1984; as an associate professor, Department of Nuclear Engineering, 1984– 1994; as a professor, Department of Quantum Engineering and Systems Sciences, 1994–1996; Nuclear Engineering Research Laboratory, 1996–2004; Department of Nuclear Engineering and Management, the University of Tokyo, 2005–present. Dr. Katsumura has been a visiting professor/fellow at many universities and institutions worldwide, including the Swiss Federal Institute of Technology (ETH, Zürich), Switzerland; the University of Science and Technology of China; the University of Sherbrooke, Canada; and the University of Paris- Sud, Orsay, France. He was the president of the Japan Society of Radiation Chemistry in 2007 and 2008, and is the division head of the Water Chemistry Division, Atomic Energy Society of Japan, since 2009. He received an award from the Japan Society of Radiation Chemistry in 2005. He has published more than 220 articles in peer-reviewed journals and books. He has also organized several international symposia of radiation chemistry and edited special issues of Radiation Physics and Chemistry.

xiii xiv Editors

Dr. Katsumura has been working on subjects related to nuclear engineering such as radiolysis of high-temperature water, radiation effects in spent fuel reprocessing, and radiation effects in high-level waste repository. His recent interests include radiolysis of supercritical water, ultrafast pulse radiolysis, and heavy ion beam radiolysis of water.

Asokendu Mozumder, research professor emeritus, Radiation Laboratory and Department of Chemistry, University of Notre Dame, received his PhD in theoretical physics from the Indian Institute of Technology (IIT), Kharagpur, India, in 1961. Since then he has worked as a lecturer in physics at IIT, 1961–1962; as a postdoctoral research associate at the Radiation Laboratory, University of Notre Dame, 1962–1965; as a scientist, 1965–1969; as an associate faculty fellow and research associate professor, Radiation Laboratory and Department of Chemistry, University of Notre Dame, 1969–1986; and as a research professor, 1986–1996, when he retired from active employment. He has been a visiting professor/fellow at many universities and institutions worldwide, including the Bhabha Atomic Research Centre, Trombay, India; Kyoto University, Japan; Waseda University, Tokyo, Japan; Japan Atomic Energy Agency; University of Paris-Sud; and Oxford University, the United Kingdom (Harwell Fellow at Wolfson College and the Department of Physical Chemistry). He has been chairperson/principal speaker at several international conferences, including Gordon conferences in radiation chemistry; Tihany symposium on radiation chemistry; and the recently held ASR 2007 conference on charged particle and photon interactions with matter, Tokai, Japan. He is a coeditor of Charged Particle and Photon Interactions with Matter: Chemical, Physicochemical, and Biological Consequences with Applications, Marcel Dekker, New York (2004). His research interests include (1) theoretical aspects of radiation chemistry, (2) early stages of radiolysis, (3) theories of electron localization and trapping, and (4) free-ion yield and mobility in liquid hydrocarbons. He is the author or coauthor of nearly 125 articles in refereed journals; a comprehensive book, Fundamentals of Radiation Chemistry (Academic Press, 1999); an article in Encyclopedia Britannica; and several chapters in other books. Contributors

Amitava Adhikary Khashayar Ghandi Department of Chemistry Department of Chemistry Oakland University Mount Allison University Rochester, Michigan Sackville, New Brunswick, Canada

Joseph M. Ajello Gregory A. Grieves Jet Propulsion Laboratory School of Chemistry and Biochemistry California Institute of Technology Georgia Institute of Technology Pasadena, California Atlanta, Georgia

Gérard Baldacchino Akira Harata Institut Rayonnement Matière Saclay o E S Commissariat à I’ Énergie Atomique et aux Faculty f ngineering ciences U Énergies Alternatives Kyushu niversity J Saclay, France Kasuga, apan and Yoshihiro Hase Laboratoire Claude Fréjacques Quantum Beam Science Directorate Centre National de la Recherche Scientique Japan Atomic Energy Agency Gif-sur-Yvette, France Takasaki, Japan

David Becker Yoshihiko Hatano Department of Chemistry Advanced Science Research Center Oakland University Japan Atomic Energy Agency Rochester, Michigan Tokai, Japan

Ortwin Brede Hisashi Hayashi Faculty of Chemistry and Mineralogy of Ch an Bi Sc University of Leipzig Department emical d ological iences Ja W U Leipzig, Germany pan oman’s niversity Tokyo, Japan Vincent De Waele Laboratoire de Chimie Physique Tetsuya Hirade Centre National de la Recherche Scientique Nuclear Science and Engineering Directorate Université Paris-Sud Japan Atomic Energy Agency Orsay, France Tokai, Japan and Kentaro Fujii Advanced Science Research Center Institute of Applied Beam Science Japan Atomic Energy Agency Ibaraki University Tokai, Japan Mito, Japan

xv xvi Contributors

Kenzo Hiraoka Yosuke Katsumura Clean Energy Research Center Department of Nuclear Engineering University of Yamanashi and Management Kofu, Japan The University of Tokyo Tokyo, Japan Koichi Hirota and Quantum Beam Science Directorate Japan Atomic Energy Agency Advanced Science Research Center Takasaki, Japan Nuclear Science Research Institute Japan Atomic Energy Agency Akira Hitachi Tokai, Japan Molecular Biophysics Kochi Medical School Nankoku, Japan Yosuke Kawashita Graduate School of Pure and Gordon L. Hug Applied Sciences Radiation Laboratory University of Tsukuba University of Notre Dame Tsukuba, Japan Notre Dame, Indiana and Yugo Kimoto R a D Faculty of Chemistry Aerospace esearch nd evelopment Di Adam Mickiewicz University rectorate A E A Poznan, Poland Japan erospace xploration gency Tsukuba, Japan Toshio Ishioka Faculty of Engineering Sciences Kazuo Kobayashi Kyushu University The Institute of Scientic and Industrial Kasuga, Japan Research Osaka University Yukikazu Itikawa Osaka, Japan Department of Basic Space Science Institute of Space and Astronautical Science Sagamihara, Japan Noriyuki Kouchi Department of Chemistry Jun-Ichi Iwata Tokyo Institute of Technology Center for Computational Sciences Tokyo, Japan and Institute of Physics University of Tsukuba Tsukuba, Japan Takahiro Kozawa The Institute of Scientic and Industrial Jean-Paul Jay-Gerin Research Département de Médecine Nucléaire Osaka University et de Radiobiologie Osaka, Japan Université de Sherbrooke Sherbrooke, Québec, Canada Isabelle Lampre Tadashi Kamada Laboratoire de Chimie Physique Research Center for Charged Particle Therapy Centre National de la Recherche Scientique National Institute of Radiological Sciences Université Paris-Sud Chiba, Japan Orsay, France Contributors xvii

Jay A. LaVerne Mehran Mostafavi Radiation Laboratory Laboratoire de Chimie Physique and Centre National de la Recherche Scientique Department of Physics Université Paris-Sud University of Notre Dame Orsay, France Notre Dame, Indiana Asokendu Mozumder Mingzhang Lin Radiation Laboratory Advanced Science Research Center University of Notre Dame Japan Atomic Energy Agency Notre Dame, Indiana Tokai, Japan Takashi Nakatsukasa Yasunari Maekawa RIKEN Nishina Center Quantum Beam Science Directorate Wako, Japan Japan Atomic Energy Agency Takasaki, Japan Sergej Naumov Department of Chemistry Rao S. Mangina Leibniz Institute of Surface Modication Jet Propulsion Laboratory Leipzig, Germany California Institute of Technology Pasadena, California Koji Noda Ce fo Ch Jason L. McLain Research nter r arged Particle Therapy School of Chemistry and Biochemistry I o R S Georgia Institute of Technology National nstitute f adiological ciences J Atlanta, Georgia Chiba, apan

Jintana Meesungnoen Takeshi Odagiri Département de Médecine Nucléaire Department of Chemistry et de Radiobiologie Tokyo Institute of Technology Université de Sherbrooke Tokyo, Japan Sherbrooke, Québec, Canada Takeshi Ohshima Robert R. Meier Quantum Beam Science Directorate Department of Physics and Astronomy Japan Atomic Energy Agency George Mason University Takasaki, Japan Fairfax, Virginia Shinobu Onoda Bruce J. Mincher Quantum Beam Science Directorate Aqueous Separations and Radiochemistry Japan Atomic Energy Agency Department Takasaki, Japan Idaho National Laboratory Idaho Falls, Idaho Thomas M. Orlando School of Chemistry and Biochemistry Yasuhiro Miyake and Japan Proton Accelerator Complex School of Physics High Energy Accelerator Research Organization Georgia Institute of Technology Tokai, Japan Atlanta, Georgia xviii Contributors

Kevin M. Prise Isao H. Suzuki Centre for Cancer Research and Photon Factory Cell Biology High Energy Accelerator Research Organization Queen’s University Belfast Tsukuba, Japan Belfast, United Kingdom and

K. Indira Priyadarsini National Metrology Institute of Japan Radiation and Photochemistry Division National Institute of Advanced Industrial Bhabha Atomic Research Centre Science and Technology Mumbai, India Tsukuba, Japan

Satoshi Suzuki Akinori Saeki Advanced Research Institute for Science The Institute of Scientic and Industrial and Engineering Research Waseda University Osaka University Tokyo, Japan Osaka, Japan Seiichi Tagawa Kimiaki Saito The Institute of Scientic and Industrial Quantum Beam Science Directorate Research Japan Atomic Energy Agency Osaka University Tokai, Japan Osaka, Japan

Miki Sato Mitsumasa Taguchi Faculty of Engineering Sciences Quantum Beam Science Directorate Kyushu University Japan Atomic Energy Agency Kasuga, Japan Takasaki, Japan

Giuseppe Schettino Junichi Takagi Centre for Cancer Research and Chemical System Design and Engineering Cell Biology Department Queen’s University Belfast Toshiba Corporation Belfast, United Kingdom Yokohama, Japan Kenji Takahashi Shu Seki Department of Chemistry and Chemical o A C Division f pplied hemistry Engineering U Osaka niversity Kanazawa University J Osaka, apan Kanazawa, Japan

Michael D. Sevilla Masao Tamada Department of Chemistry Quantum Beam Science Directorate Oakland University Japan Atomic Energy Agency Rochester, Michigan Takasaki, Japan

Naoya Shikazono Atsushi Tanaka Advanced Science Research Center Quantum Beam Science Directorate Japan Atomic Energy Agency Japan Atomic Energy Agency Tokai, Japan Takasaki, Japan Contributors xix

Hiroshi Tanaka Kazuhiro Yabana Department of Physics Center for Computational Sciences Sophia University and Institute of Physics Tokyo, Japan University of Tsukuba Tsukuba, Japan Yasuo Udagawa Institute of Multidisciplinary Research Makoto Yamaguchi for Advanced Materials Geological Isolation Research Tohoku University and Development Directorate Sendai, Japan Japan Atomic Energy Agency Tokai, Japan Masatoshi Ukai Department of Applied Physics Shinichi Yamashita Tokyo University of Agriculture Advanced Science Research Center and Technology Japan Atomic Energy Agency Tokyo, Japan Tokai, Japan

James F. Wishart Akinari Yokoya Chemistry Department Advanced Science Research Center Brookhaven National Laboratory Japan Atomic Energy Agency Upton, New York Tokai, Japan

1 Introduction Yoshihiko Hatano Japan Atomic Energy Agency Tokai, Japan Yosuke Katsumura The University of Tokyo Tokyo, Japan and Japan Atomic Energy Agency Tokai, Japan Asokendu Mozumder University of Notre Dame Notre Dame, Indiana

CONTENTS 1.1 Theoretical Studies as New Approaches to Primary Processes That Motivate New Experiments ...... 3 1.2 Advances in the Theoretical and Experimental Studies of the Physicochemical, Chemical, and Biological Stages ...... 6 References ...... 7

In Chapter 1 of Charged Particle and Photon Interactions with Matter: Chemical, Physicochemical, and Biological Consequences with Applications (Mozumder and Hatano, 2004), early investigations were brie¡y described with respect to photochemistry and radiation chemistry. The Bethe theory was also discussed brie¡y in terms of the quantitative similarity of the excitation and ionization processes of a molecule by photon and charged particle impacts, with emphasis on the importance of optical oscillator strength. It was further pointed out that the applications in the eld of charged particle and photon interactions with matter have a relatively short history, except for some medical applications. However, their importance has gradually increased in science and technology since the 1960s. The chapter brie¡y discussed the timescale of charged particle and photon interactions with matter, for example, in liquid water. Fundamental processes in the physical, physicochemical, and chemical stages of these interactions were delineated. The 2004 book was organized into 26 chapters, and a list of chapters along with their contributors follows:

1. Introduction (A. Mozumder and Y. Hatano) 2. Interaction of Fast Charged Particles with Matter (A. Mozumder) 3. Ionization and Secondary Electron Production by Fast Charged Particles (L. H. Toburen)

1 2 Charged Particle and Photon Interactions with Matter

4. Modeling of Physicochemical and Chemical Processes in the Interactions of Fast Charged Particles with Matter (S. M. Pimblott and A. Mozumder) 5. Interaction of Photons with Molecules: Photoabsorption, Photoionization, and Photodissocia tion Cross Sections (N. Kouchi and Y. Hatano) 6. Reactions of Low-Energy Electrons, Ions, Excited Atoms and Molecules, and Free Radicals in the Gas Phase as Studied by Pulse Radiolysis Methods (M. Ukai and Y. Hatano) 7. Studies of Solvation Using Electrons and Anions in Alcohol Solutions (C. D. Jonah) 8. Electrons in Nonpolar Liquids (R. A. Holroyd) 9. Interactions of Low-Energy Electrons with Atomic and Molecular Solids (A. D. Bass and L. Sanche) 10. Electron−Ion Recombination in Condensed Matter: Geminate and Bulk Recombination Processes (M. Wojcik, M. Tachiya, S. Tagawa, and Y. Hatano) 11. Radical Ions in Liquids (I. A. Shkrob and M. C. Sauer, Jr.) 12. The Radiation Chemistry of Liquid Water: Principles and Applications (G. V. Buxton) 13. Photochemistry and Radiation Chemistry of Liquid Alkanes: Formation and Decay of Low-Energy Excited States (L. Wojnarovits) 14. Radiation Chemical Effects of Heavy Ions (J. A. LaVerne) 15. DNA Damage Dictates the Biological Consequences of Ionizing Irradiation: The Chemical Pathways (W. A. Bernhard and D. M. Close) 16. Photon-Induced Biological Consequences (K. Kobayashi) 17. Track Structure Studies of Biological Systems (H. Nikjoo and S. Uehara) 18. Microdosimetry and Its Medical Applications (M. Zaider and J. F. Dicello) 19. Charged Particle and Photon-Induced Reactions in Polymers (S. Tagawa, S. Seki, and T. Kozawa) 20. Charged Particle and Photon Interactions in Metal Clusters and Photographic System Studies (J. Belloni and M. Mostafavi) 21. Applications of Radiation Chemical Reactions to the Molecular Design of Functional Organic Materials (T. Ichikawa) 22. Applications to Reaction Mechanism Studies of Organic Systems (T. Majima) 23. Applications of Radiation Chemistry to Nuclear Technology (Y. Katsumura) 24. Electron Beam Applications to Flue Gas Treatment (H. Namba) 25. Ion-Beam Therapy: Rationale, Achievements, and Expectations (A. Wambersie, J. Gueulette, D. T. L. Jones, and R. Gahbauer) 26. Food Irradiation (J. Farkas) 27. New Applications of Ion Beams to Material, Space, and Biological Science and Engineering (M. Fukuda, H. Itoh, T. Ohshima, M. Saidoh, and A. Tanaka)

The 2004 book was motivated by two projects. One was a long-term IAEA international project, from 1985 to 1995, that surveyed the accomplishments in basic radiation research over the past 100 years following the discovery of ionizing radiation by Curie and Roentgen in the late nineteenth century (Inokuti, 1995). The other was a textbook of radiation chemistry published in 1999 (Mozumder, 1999). Since the activities of the former project, summarized in an IAEA report, were unfortunately not well known among the international science and technology communities, the participants of the IAEA project agreed that the scientic results of the activities should be published elsewhere, in a book with wider circulation. Furthermore, the IAEA project focused mainly on primary interactions, that is, the physical stage of the fundamental processes of radiation chemistry. Therefore, Mozumder and Hatano collaborated to edit a new book that would include the physicochemical and chemical stages, in addition to the physical stage, of the fundamental processes of radiation chemistry, and, consequently, those of radiation biology. Introduction 3

TABLE 1.1 Fundamental Processes of Radiation Chemistry AB AB+ + e− Direct ionization AB** Superexcitation (direct excitation) AB* Excitation (direct excitation)

AB** → AB+ + e− Autoionization → A + B Dissociation AB+ → A+ + B Ion dissociation AB+ + AB or S → Products Ion–molecule reaction AB+ + e− → AB* Electron–ion recombination AB+ + S−→ Products Ion–ion recombination e− + S → S− Electron attachment − − e + nAB → e s Solvation AB* → A + B Dissociation → AB Internal conversion and intersystem crossing → BA Isomerization → AB + hν Fluorescence AB* + S → AB + S* Energy transfer

AB* + AB → (AB)2* Excimer formation

2A → A2 Radical recombination → C + D Disproportionation

A + AB → A2B Addition

→ A2 + B Abstraction

Source: Mozumder, A. and Hatano, Y. (eds.), Charged Particle and Photon Interactions with Matter: Chemical, Physicochemical, and Biological Consequences with Applications, Marcel Dekker, New York, 2004.

The fundamental processes of radiation chemistry are shown in Table 1.1 (Mozumder and Hatano, 2004), in which the rst three constitute the physical stage or the primary process of the charged particle and photon interactions with matter (Hatano, 2003). Here “primary” means the earliest stage that is conceivable either theoretically or experimentally. Sometimes “initial” is used for measured yields at the shortest time that is possible in a given experimental setup. The primary stage is followed by the physicochemical and chemical stages. These are followed by the biological stages. See also Chapter 1 of the 2004 book. The 2004 book succeeded in surveying critically and in detail the comprehensive features of the physical, physicochemical, chemical, and biological stages. Further, the applications of charged particle and photon interactions with matter were treated brie¡y. Most of the papers referred in the 2004 book were published before 2000.

1.1 THEORETIcAL STUDIES AS NEW APPROAcHES TO PRIMARY PROcESSES THAT MOTIVATE NEW EXPERIMENTS From the late nineteenth century to the rst half of the twentieth century, studies of the interaction of ionizing radiation with matter were mainly phenomenological in character. A new theoretical approach, particularly for the primary process, that is, the physical stage, was initiated during 1955–1965 by Platzman, Fano, and Inokuti. They considered the interaction to be the collision of 4 Charged Particle and Photon Interactions with Matter high-energy particles with matter, that is, basically molecules. The important ndings of their studies are summarized as follows (Platzman, 1962a,b; Hatano, 1999, 2003; Mozumder and Hatano, 2004, Chapters 1 and 5; and Chapter 2):

1. Ionizing radiation is generally classied according to high-energy (a) photons; (b) electrons; (c) heavy charged particles; and (d) other particles such as neutrons, positrons, muons, etc. Although the initial interaction of each of these particles with a molecule depends largely on the kind and energy of the particle, common features among the initial interactions and further the following electron−molecule collisions should be the formation of electrons in a wide energy range. These are called “secondary electrons.” The secondary electrons are classied according to their energy in the middle- and high-energy ranges, and those in the subexcitation energy region. It was concluded that the essential features of the interaction of ionizing radiation with molecules in the primary process is electron−molecule collisions in a wide range of collision energies, which are followed by cascades of multiple electron−molecule collisions in matter (Spencer and Fano, 1954; Mozumder and Hatano, 2004, Chapters 3, 6, and 9; and Chapter 3). 2. Secondary electron collisions with molecules in the middle- and high-energy ranges may be treated approximately by the Bethe theory (Inokuti, 1971), resulting in the important conclusion that the generalized oscillator strength and, further, the optical oscillator strength are of great importance in interpreting the primary result of the interaction of ionizing radiation with matter. Thus, G-values have been estimated theoretically from the optical oscillator strength by “the optical approximation” (Platzman, 1962a,b). That is, the energy deposition spectra in the interaction of ionizing radiation with molecules can be estimated from the optical oscillator strength (Hatano, 2003, 2009; Mozumder and Hatano, 2004, Chapter 5; and Chapter 2). 3. Since the optical oscillator strength, which is of the great importance in basic sciences, had not yet been calculated either theoretically or experimentally, Platzman and Fano realized and pointed out for the rst time in the late 1950s that synchrotron radiation should be a powerful photon source in a wide span of photon energies from UV-visible to hard x-rays (Hatano, 1995). 4. After a scientically careful and intuitive analysis of the primary interaction of ionizing radiation with molecules, as obtained from the Bethe theory and optical approximation, Platzman realized that for most molecules there is a big difference between the ionization threshold energy and the energy region where the major part of the oscillator strength distribution is located, as deduced from optical data and sum rules. He presented his idea of “superexcited states,” which are neutral excited states located in the energy region above the ionization threshold (Platzman, 1962a,b; Hatano, 2003; Mozumder and Hatano, 2004, Chapter 5; and Chapter 2).

The theoretical studies, summarized above in (1) through (4), have motivated much new experimental research since the late 1960s as described below (Hatano, 1999; Mozumder and Hatano, 2004, Chapter 5; and Chapter 2):

1. Experimental evidence was rst obtained, independent of these theoretical studies, for the reaction of hot hydrogen atoms formed from the dissociation of highly excited states, produced by direct excitation during the radiolysis of liquid olens (Hatano and Shida, 1967). The experimental results were analyzed in terms of the theoretical studies to compare the experimental G-values with the theoretical ones for the superexcited states estimated by the optical approximation, giving the rst experimental evidence for the important role of superexcited states in radiolysis (Hatano et al., 1968). Introduction 5

2. To obtain experimentally the electronic states of superexcited molecules and their dissociation dynamics to form hot hydrogen atoms, which could be electronically and/or translationally excited, Doppler spectroscopy combined with an electron−molecule collision apparatus was developed (Ito et al., 1976, 1977; Hatano, 1983; Kouchi et al., 1997). In this experiment using molecular hydrogen, the doubly excited and singly excited (with vibrational/rotational excitation) high Rydberg states converging individually to each of the ionized states were observed as superexcited states for the rst time. For other mol-

ecules such as HF, H2O, NH3, and CH4, the doubly and inner-core excited states were also observed. 3. To obtain more detailed information with state selectivity and higher-energy resolution, synchrotron radiation (SR) has been used as an excitation source for this kind of investigation (Hatano, 1999). The measurements in these SR experiments are classied into two types: One is the absolute measurements of photoabsorption cross sections (optical oscillator strengths), photoionization cross sections, photodissociation cross sections, and photoionization quantum yields. The other is the measurement, with high-energy resolution, of state-specied dissociation fragments formed from state-specied superexcited states. It was concluded that the electronic states and the dissociation dynamics of molecular superexcited states were experimentally evidenced for the rst time in these investigations (Hatano, 1999). Accordingly, an important role of the superexcited states in the primary process of the interaction of ionizing radiation with matter has been well substantiated (Hatano, 2003). The results obtained are summarized as follows. Further, these investigations have made great progress recently, which are described in Chapter 2. a. Superexcited states are (i) vibrationally/rotationally excited high Rydberg states, (ii) doubly excited states, or (iii) inner-core excited states, giving conclusive experimental evidence for Platzman’s idea. b. They dissociate into neutral fragments, with excess electronic or translational energies, in competition with autoionization. c. Their dissociation dynamics, as well as the dissociation products, are quite different from those for the lower excited states below ionization thresholds. d. Molecules are not easily ionized, which is an unexpected phenomenon. e. New information obtained has motivated fresh investigations of quantum theories applied to the spectroscopy and dynamics of such highly excited molecules (see Chapter 2), as well as explaining the oscillator strengths (see Chapter 4). f. The new information obtained has also substantiated, to a great extent, the superexcited states considered as a collision complex in some important processes such as Penning ionization, electron−ion recombination, and electron attachment to molecules. g. The new information has greatly motivated the reanalysis of various other kinds of phenomena, besides radiolysis, for the ionization and excitation of molecules, such as reactive plasmas, plasmas in the upper atmosphere and space, and so on. h. The new information was previously almost limited to molecules in the gas phase. The oscillator strengths in the condensed phase were discussed brie¡y (Hatano and Inokuti, 1995) and have recently been measured using a newly developed method (see Chapter 5). 4. Measurements of optical oscillator strengths (photoabsorption cross sections and photoionization cross sections) as deduced from electron−molecule collision experiments have been made in which the optimum conditions were selected using the Bethe theory. This method has been called the “poor man’s synchrotron experiments” or “imaginary-photon experiments” as opposed to “real-photon experiments” using synchrotron radiation, which requires the construction of big-scale facilities. These two types of experiments were compared in detail in Chapter 5 of the 2004 book. The data obtained by these methods have been critically evaluated and compiled elsewhere as recommended ones (Kameta et al., 2003). 6 Charged Particle and Photon Interactions with Matter

An important part of the new theories of the primary processes was obtained from W-value studies (Platzman, 1961). New directions in these studies have been made possible by using synchrotron radiation and are reviewed in Chapter 6. Remarkable progress has recently been made of the interaction of positrons and muons with matter, which are surveyed in Chapters 7 and 8, respectively. With regard to the information summarized above, future perspectives and future research programs that need more work on the theoretical and experimental aspects of the primary processes have recently been discussed elsewhere (Hatano, 2009).

1.2 ADVANcES IN THE THEORETIcAL AND EXPERIMENTAL STUDIES Of THE PHYSIcOcHEMIcAL, CHEMIcAL, AND BIOLOGIcAL STAGES Virtually all important studies published in or before 2000 of the physical, physicochemical, chemical, and biological stages of the charged particle and photon interactions with matter were surveyed critically and in detail, both theoretically and experimentally, in the 2004 book. Some of these are detailed in the next paragraph. The theoretical studies were surveyed in Chapters 2, 4, 10, and 17. Reactions of electrons, ions, excited atoms and molecules, and also of free radicals in the gas phase, as studied by pulse radiolysis methods, were surveyed in Chapter 6, while those in the condensed phase in Chapters 7, 8, 10, and 11. The radiation chemistry of liquid water, liquid alkanes, polymers, and metal clusters/photographic systems was surveyed in Chapters 12, 13, 19, and 20, respectively. Radiation chemistry at high-LET was reviewed in Chapter 14. Biological consequences were followed up in Chapters 15 and 16. Applications in medical microdosimetry, molecular designing, organic chemistry, nuclear technology, ¡ue gas treatment, ion-beam therapy, food irradiation, and other new material, space, and biological science and engineering were surveyed in Chapters 18, 21 through 27, respectively. New advances in the studies of these stages, which were not covered in the 2004 book, have been remarkable since 2000. This has been pointed out in the preface. Furthermore, great progress has recently been made in the applications and interface formation. The outline of recent advances in the studies of primary processes (the physical stage) is described brie¡y in Section 1.2 (also refer Chapters 2 through 8). Those of the physicochemical, chemical, and biological stages, as well as of the applications and the interface formation, are brie¡y described below. New theoretical studies of the physicochemical and chemical stages are introduced in Chapters 9 and 14, respectively; these studies describe the behavior of electrons in liquid hydrocarbons and for the high-LET radiolysis of liquid water. In Chapter 9, the authors make the rst application of the Anderson localization concept for electron mobility in liquid hydrocarbons. New experimental research in the physicochemical and chemical stages are described in Chapters 10 through 13, 15 through 18 for each of the specic characteristics of matter to be studied or under their specic experimental conditions. New experimental studies of the biological stage are introduced in Chapters 19 through 22. The applications in health physics and cancer therapy are found in Chapters 23 and 24, respectively. Applications to polymers are discussed in Chapters 25 through 27. The applications and the interface formation in space science and technology are introduced in Chapters 28 through 30. Applications for the research and development of radiation detectors, environmental conservation, plant breeding, and nuclear engineering are further available in Chapters 31 through 34, respectively. With regard to the information summarized above, future perspectives and research programs that need more theoretical and experimental work on the physicochemical and chemical stages of the fundamental processes have recently been discussed elsewhere (Hatano, 2009). Introduction 7

REfERENcES Hatano, Y. 1983. Electron impact dissociation of simple molecules. Comments Atom. Mol. Phys. 13: 259–273. Hatano, Y. 1995. Applications of synchrotron radiation to radiation research. In Radiation Research (Congress Lecture, the 10th International Congress of Radiation Research, Wurzburg, Germany), U. Hagen, D. Harder, H. Jung, and C. Streffer (eds.), Vol. II, pp. 86–92. Wurzburg, Germany: Universitatsdrukerei, H. Strutz AG. Hatano, Y. 1999. Interaction of vacuum ultraviolet photons with molecules. Formation and dissociation dynamics of molecular superexcited states. Phys. Rep. 313: 109–169. Hatano, Y. 2003. Spectroscopy and dynamics of molecular superexcited states. Aspects of primary processes of radiation chemistry. Radiat. Phys. Chem. 67: 187–198. Hatano, Y. 2009. Future perspectives of radiation chemistry. Radiat. Phys. Chem. 78: 1021–1025. Hatano, Y. and Inokuti, M. 1995. Photoabsorption, photoionization, and photodissociation cross sections. In Atomic and Molecular Data for Radiotherapy and Radiation Research, IAEA-TECDOC-799, M. Inokuti (ed.), Chapter 5. Vienna, Austria: IAEA. Hatano, Y. and Shida, S. 1967. Hydrogen formation in the radiolyses of liquid butene-1 and trans-butene-2. J. Chem. Phys. 46: 4784–4788. Hatano, Y., Shida, S., and Inokuti, M. 1968. Hydrogen formation and superexcited states in the radiolysis of liquid olens. J. Chem. Phys. 48: 940–941. Inokuti, M. 1971. Inelastic collisions of fast charged particles with atoms and molecules. The Bethe theory revisited. Rev. Mod. Phys. 43: 297–347. Inokuti, M. (ed.). 1995. Atomic and Molecular Data for Radiotherapy and Radiation Research, IAEA- TECDOC-799. Vienna, Austria: IAEA. Ito, K., Oda, N., Hatano, Y., and Tsuboi, T. 1976. Doppler prole measurements of Balmer-α radiation by electron impact on H2. Chem. Phys. 17: 35–43. Ito, K., Oda, N., Hatano, Y., and Tsuboi, T. 1977. The electron energy dependence of the Doppler proles of

Balmer-α emission from H2, D2, CH4 and other simple hydrocarbons by electron impact. Chem. Phys. 21: 203–210. Kameta, K., Kouchi, N., and Hatano, Y. 2003. Cross sections for photoabsorption, photoionization, and photodissociation of molecules. In Landolt-Boernstein, Y. Itikawa (ed.), New Series, Vol. I/17C. Berlin, Germany: Springer. Kouchi, N., Ukai, M., and Hatano, Y. 1997. Dissociation dynamics of superexcited molecular hydrogen. J. Phys. B: Atom. Mol. Opt. Phys. 30: 2319–2344. Mozumder, A. 1999. Fundamentals of Radiation Chemistry. San Diego, CA: Academic Press. Mozumder, A. and Hatano, Y. (eds.). 2004. Charged Particle and Photon Interactions with Matter: Chemical, Physicochemical, and Biological Consequences with Applications. New York: Marcel Dekker. Platzman, R. L. 1961. Total ionization in gases by high energy particles: An appraisal of our understanding. Int. J. Appl. Radiat. Isot. 10: 116–127. Platzman, R. L. 1962a. Superexcited states of molecules, and the primary action of ionizing radiation. Vortex 23: 372–385. Platzman, R. L. 1962b. Superexcited states of molecules. Radiat. Res. 17: 419–425. Spencer, L. V. and Fano, U. 1954. Energy spectrum resulting from electron slowing down. Phys. Rev. 93: 1172–1181.

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