Nuclear and Radiochemistry

Jens-Volker Kratz is a retired Professor of Nuclear Chemistry at Johannes Gutenberg University in Mainz, Germany. He obtained his degrees in Chemistry at this university, followed by postdoctoral research with Glenn T. Seaborg at Berkeley. Before moving back to Mainz, he worked as a group leader between 1974 and 1982 at GSI in Darmstadt. He has published 350 scientific articles and two editions of this textbook. For 24 years, he served as editor of Radiochimica Acta. He was nominated Fellow of the International Union of Pure and Applied Chemistry and has received numerous prizes, including the Otto Hahn Award.

• Volume 1Preface vii1 Fundamental Concepts 11.1 The Atom 11.2 Atomic Processes 21.3 Discovery of the Atomic Nucleus 41.4 Nuclear Decay Types 61.5 Some Physical Concepts Needed in Nuclear Chemistry 101.5.1 Fundamental Forces 101.5.2 Elements from Classical Mechanics 111.5.3 Relativistic Mechanics 111.5.4 The de Broglie Wavelength 131.5.5 Heisenberg Uncertainty Principle 141.5.6 The Standard Model of Particle Physics 151.5.7 Force Carriers 19Reference 20Further Reading 212 Radioactivity in Nature 232.1 Discovery of Radioactivity 232.2 Radioactive Substances in Nature 262.3 Nuclear Forensics 30References 33Further Reading 333 Radioelements and Radioisotopes and Their Atomic Masses 353.1 Periodic Table of the Elements 353.2 Isotopes and the Chart of Nuclides 363.3 Nuclide Masses and Binding Energies 403.4 Evidence for Shell Structure in Nuclei 483.5 Precision Mass Spectrometry 51References 56Further Reading 564 Other Physical Properties of Nuclei 594.1 Nuclear Radii 594.2 Nuclear Angular Momenta 644.3 Magnetic Dipole Moments 664.4 Electric Quadrupole Moments 694.5 Statistics and Parity 704.6 Excited States 71References 72Further Reading 725 The Nuclear Force and Nuclear Structure 755.1 Nuclear Forces 755.2 Charge Independence and Isospin 785.3 Nuclear Matter 825.4 Fermi Gas Model 845.5 Shell Model 865.6 Collective Motion in Nuclei 955.7 Nilsson Model 1005.8 The Pairing Force and Quasi-Particles 1045.9 Macroscopic–Microscopic Model 1065.10 Interacting Boson Approximation 1085.11 Further Collective Excitations: Coulomb Excitation, High-Spin States, Giant Resonances 110References 116Further Reading 1166 Decay Modes 1196.1 Nuclear Instability and Nuclear Spectroscopy 1196.2 Alpha Decay 1196.2.1 Hindrance Factors 1246.2.2 Alpha-Decay Energies 1256.3 Cluster Radioactivity 1276.4 Proton Radioactivity 1296.5 Spontaneous Fission 1326.6 Beta Decay 1466.6.1 Fundamental Processes 1466.6.2 Electron Capture-to-Positron Ratios 1566.6.3 Nuclear Matrix Elements 1576.6.4 Parity Non-Conservation 1606.6.5 Massive Vector Bosons 1626.6.6 Cabibbo–Kobayashi–Maskawa Matrix 1636.7 Electromagnetic Transitions 1686.7.1 Multipole Order and Selection Rules 1696.7.2 Transition Probabilities 1716.7.3 Internal Conversion Coefficients 1766.7.4 Angular Correlations 180References 183Further Reading 1847 Radioactive Decay Kinetics 1877.1 Law and Energy of Radioactive Decay 1877.2 Radioactive Equilibria 1897.3 Secular Radioactive Equilibrium 1917.4 Transient Radioactive Equilibrium 1937.5 Half-Life of Mother Nuclide Shorter than Half-Life of Daughter Nuclide 1947.6 Similar Half-Lives 1947.7 Branching Decay 1967.8 Successive Transformations 197Reference 199Further Reading 1998 Nuclear Radiation 2018.1 General Properties 2018.2 Heavy Charged Particles (A ≥1) 2038.3 Beta Radiation 2108.4 Gamma Radiation 2158.5 Neutrons 2218.6 Short-Lived Elementary Particles in Atoms and Molecules 226References 228Further Reading 2289 Measurement of Nuclear Radiation 2319.1 Activity and Counting Rate 2319.2 Gas-Filled Detectors 2359.2.1 Ionization Chambers 2389.2.2 Proportional Counters 2399.2.3 Geiger–Müller Counters 2419.3 Scintillation Detectors 2429.4 Semiconductor Detectors 2459.5 Choice of Detectors 2519.6 Spectrometry 2539.7 Determination of Absolute Disintegration Rates 2559.8 Use of Coincidence and Anticoincidence Circuits 2589.9 Low-Level Counting 2589.10 Neutron Detection and Measurement 2599.11 Track Detectors 2609.11.1 Photographic Emulsions and Autoradiography 2609.11.2 Dielectric Track Detectors 2629.11.3 Cloud Chambers 2639.11.4 Bubble Chambers 2639.11.5 Spark Chambers 2639.12 Detectors Used in Health Physics 2639.12.1 Portable Counters and Survey Meters 2649.12.2 Film Badges 2649.12.3 Pocket Ion Chambers 2649.12.4 Thermoluminescence Dosimeters 2649.12.5 Contamination Monitors 2659.12.6 Whole-Body Counters 265Reference 265Further Reading 26510 Statistical Considerations in Radioactivity Measurements 26910.1 Distribution of Random Variables 26910.2 Probability and Probability Distributions 27110.3 Maximum Likelihood 27710.4 Experimental Applications 27810.5 Statistics of Pulse-Height Distributions 28010.6 Statistical Assessments of Lifetimes in α-Decay Chains of Odd-Z Heavy Elements 28210.7 Setting Upper Limits when no Counts Are Observed 285References 285Further Reading 28511 Techniques in Nuclear Chemistry 28711.1 Special Aspects of the Chemistry of Radionuclides 28711.1.1 Short-Lived Radionuclides and the Role of Carriers 28711.1.2 Radionuclides of High Specific Activity 28911.1.3 Microamounts of Radioactive Substances 29011.1.4 Radiocolloids 29411.1.5 Tracer Techniques 29711.2 Target Preparation 29811.3 Measuring Beam Intensity and Fluxes 30411.4 Neutron Spectrum in Nuclear Reactors 30611.4.1 Thermal Neutrons 30611.4.2 Epithermal Neutrons and Resonances 30811.4.3 Reaction Rates in Thermal Reactors 30911.5 Production of Radionuclides 30911.5.1 Production in Nuclear Reactors 30911.5.2 Production by Accelerators 31411.5.3 Separation Techniques 32211.5.4 Radionuclide Generators 32611.6 Use of Recoil Momenta 32911.7 Preparation of Samples for Activity Measurements 33711.8 Determination of Half-Lives 33811.9 Decay-Scheme Studies 34011.10 In-Beam Nuclear Reaction Studies 342References 356Further Reading 357Volume 2Preface ix12 Nuclear Reactions 36112.1 Collision Kinematics 36212.2 Coulomb Trajectories 36412.3 Cross Sections 36712.4 Elastic Scattering 37112.5 Elastic Scattering and Reaction Cross Section 37812.6 Optical Model 38112.7 Nuclear Reactions and Models 38312.7.1 Investigation of Nuclear Reactions 38412.7.2 Compound Nucleus Model 38412.7.3 Precompound Decay 40012.7.4 Direct Reactions 40112.7.5 Photonuclear Reactions 40312.7.6 Fission 40412.7.7 High-Energy Reactions 41412.8 Nuclear Reactions Revisited with Heavy Ions 41912.8.1 Heavy-Ion Fusion Reactions 42012.8.2 Quasi-Fission 42912.8.3 Deep Inelastic Collisions 43512.8.3.1 The 238U+238U Reaction 44712.8.3.2 Isotope Distributions at Fixed Z Below Z =92 44912.8.3.3 Bombarding-Energy Dependence of the Deep-Inelastic Collisions 45112.8.3.4 Isotope Distributions at Fixed Z Above Z =92 45412.8.3.5 The 238U + 248Cm Reaction 45912.8.3.6 Comparison of the Element Yields with Diffusion-Model Predictions 46112.8.4 “Simple” (Quasi-elastic) Reactions at the Barrier 46412.8.5 “Complex” Transfer Reactions 46912.8.6 Relativistic Heavy-Ion Collisions, the Phases of Nuclear Matter 475References 480Further Reading 48413 Chemical Effects of Nuclear Transmutations 48913.1 General Aspects 48913.2 Recoil Effects 49013.3 Excitation Effects 49513.4 Gases and Liquids 49913.5 Solids 50213.6 Szilard–Chalmers Reactions 50613.7 Recoil Labeling and Self-labeling 506References 508Further Reading 50914 Influence of Chemical Bonding on Nuclear Properties 51114.1 Survey 51114.2 Dependence of Half-Lives on Chemical Bonding 51214.3 Dependence of Radiation Emission on the Chemical Environment 51414.4 Mössbauer Spectrometry 522References 527Further Reading 52815 Nuclear Energy, Nuclear Reactors, Nuclear Fuel, and Fuel Cycles 53115.1 Energy Production by Nuclear Fission 53115.2 Nuclear Fuel and Fuel Cycles 53615.3 Production of Uranium and Uranium Compounds 54115.4 Fuel Elements 54415.5 Nuclear Reactors, Moderators, and Coolants 54715.6 The Chernobyl and Fukushima Accidents 55415.7 Reprocessing 56115.8 RadioactiveWaste 56715.9 The Natural Reactors at Oklo 57615.10 Controlled Thermonuclear Reactors 57715.11 Nuclear Explosives 579References 580Further Reading 58116 Sources of Nuclear Bombarding Particles 58516.1 Neutron Sources 58516.2 Neutron Generators 58616.3 Research Reactors 58716.4 Charged-Particle Accelerators 58916.4.1 Direct Voltage Accelerators 59116.4.2 Linear Accelerators 59416.4.3 Cyclotrons 59616.4.4 Synchrocyclotrons, Synchrotrons 59816.4.5 Radioactive Ion Beams 60116.4.5.1 FAIR – The Universe in the Lab 60116.4.5.2 Research at FAIR 60216.4.5.3 Construction of FAIR 60416.4.5.4 International Partners 60416.4.5.5 High Tech for FAIR 60416.4.6 Photon Sources 605References 606Further Reading 60617 Radioelements 60917.1 Natural and Artificial Radioelements 60917.2 Technetium and Promethium 61317.3 Production of Transuranic Elements 61617.3.1 Hot-Fusion Reactions 62217.3.2 Cold-Fusion Reactions 62517.3.3 48Ca-Induced Fusion Reactions 63217.3.4 Other Disciplines 63817.4 Cross Sections 64017.5 Nuclear Structure of Superheavy Elements 64517.6 Spectroscopy of Actinides and Transactinides 64917.7 Properties of the Actinides 65217.8 Chemical Properties of the Transactinides 66717.8.1 Prediction of Electron Configurations and the Architecture of the Periodic Table of the Elements 66817.8.2 Methods to Investigate the Chemistry of the Transactinides 67017.8.3 Selected Experimental Results 690References 721Further Reading 72718 Radionuclides in Geo- and Cosmochemistry 73518.1 Natural Abundances of the Elements and Isotope Variations 73518.2 General Aspects of Cosmochemistry 73818.3 Early Stages of the Universe 73818.4 Synthesis of the Elements in the Stars 74118.4.1 Evolution of Stars 74118.4.2 Evolution of the Earth 74318.4.3 Thermonuclear Reaction Rates 74418.4.4 Hydrogen Burning 74618.4.5 Helium Burning 74718.4.6 Synthesis of Nuclei with A <60 74818.4.7 Synthesis of Nuclei with A >60 74818.4.7.1 The s- (Slow) Process 74918.4.7.2 The r (Rapid) Process 74918.4.7.3 The p (Proton) Process 75318.5 The Solar Neutrino Problem 75418.6 Absolute Neutrino Masses 76218.6.1 m(νμ) from Pion Decay 76318.6.2 m(ντ) from Tau Decay 76318.6.3 m(νe) from Nuclear β-Decay 76418.6.4 The Karlsruhe Tritium Experiment on the Neutrino Mass KATRIN 76418.7 Interstellar Matter and Cosmic Radiation 76518.7.1 Interstellar Matter 76518.7.2 Cosmic Radiation 76718.7.3 Radionuclides from Cosmic Rays 76718.7.4 Cosmic-Ray Effects in Meteorites 76818.7.5 Abundance of Li, Be, and B 769References 769Further Reading 77019 Dating by Nuclear Methods 77519.1 General Aspect 77519.2 Cosmogenic Radionuclides 77619.3 Terrestrial Mother/Daughter Nuclide Pairs 78119.4 Natural Decay Series 78319.5 Ratios of Stable Isotopes 78619.6 Radioactive Disequilibria 78819.7 Fission Tracks 788References 789Further Reading 79020 Radioanalysis 79320.1 General Aspects 79320.2 Analysis on the Basis of Inherent Radioactivity 79420.3 Neutron Activation Analysis (NAA) 79620.4 Activation by Charged Particles 80020.5 Activation by Photons 80020.6 Special Features of Activation Analysis 80220.7 Isotope Dilution Analysis 80520.8 Radiometric Methods 80720.9 Other Analytical Applications of Radiotracers 80820.10 Absorption and Scattering of Radiation 80920.11 Radionuclides as Radiation Sources in X-ray Fluorescence Analysis (XFA) 81020.12 Analysis with Ion Beams 81120.13 Radioisotope Mass Spectrometry 81520.13.1 Resonance Ionization Mass Spectrometry (RIMS) 81520.13.2 Accelerator Mass Spectrometry (AMS) 82020.13.3 Measurements of Ionization Potentials 824References 830Further Reading 83221 Radionuclides in the Life Sciences 83721.1 Survey 83721.2 Application in Ecological Studies 83821.3 Radioanalysis in the Life Sciences 83821.4 Application in Physiological and Metabolic Studies 84021.5 Radionuclides Used in Nuclear Medicine 84121.6 Single-Photon Emission Computed Tomography (SPECT) 84321.7 Positron Emission Tomography (PET) 84421.8 Labeled Compounds 844References 850Further Reading 85122 Radionuclides in the Geosphere and the Biosphere 85522.1 Sources of Radioactivity 85522.2 Mobility of Radionuclides in the Geosphere 85822.3 Reactions of Radionuclides with the Components of NaturalWaters 86122.4 Interactions of Radionuclides with Solid Components of the Geosphere 86522.5 Radionuclides in the Biosphere 87322.6 Speciation Techniques with Relevance for Nuclear Safeguards, Verification, and Applications 87822.6.1 Redox Reactions, Hydrolysis, and Colloid Formation of Pu(IV) 88322.6.2 Investigation of the Homologs Th(IV) and Zr(IV) 88822.6.3 Time-Resolved Laser-Induced Fluorescence 89522.7 Conclusions 899References 900Further Reading 90223 Dosimetry and Radiation Protection 90923.1 Dosimetry 90923.2 External Radiation Sources 91123.3 Internal Radiation Sources 91223.4 Radiation Effects in Cell 91523.4.1 BNCT 91623.5 Radiation Effects in Humans, Animals, and Plants 92123.6 Non-occupational Radiation Exposure 92523.7 Safety Recommendations 92523.8 Safety Regulations 92823.9 Monitoring of the Environment 93223.10 Geological Disposal of RadioactiveWaste 933References 936Further Reading 937Index 941