Analysis of Environmental Radionuclides: Sample collection. 2. Treatment of environmental samples. 3. Radiochemical separation methods. 4. Sources of background and its reduction. 5. Radiometrics methods. 6. Underground counting laboratories. 7. In site m

The purpose of this book is to present a state of art summary of current knowledge of methods of assessment of radionuclides in the terrestrial and marine environments. It cover the traditional methods of radioactivity measurements such as radiometrics techniques, but also recent developments in the mass spectrometry sector. The book starts with a short preface introducing the subject of the book, summarising content and philosophy of the book, as well as the most important historical achievements. The scientific topics are introduced by description of sampling methods, optimisation of sampling sites and sampling frequency. The recent developments in radiochemical separation methods using chromatography resins for the treatment of actinides, transuranics and other groups of radioelements are also described. No other book is available covering all aspects of environmental radioactivity measurements, although remarkable progress has been made in detection techniques over the last ten years. At present the new methods enable to carry out investigations which were not possible before, either because of lack of sensitivity or because of the fact that they required too large samples. cover.jpg......Page 1 sdarticle.pdf......Page 2 General sampling concepts and principles......Page 4 Simple random sampling......Page 5 Analysis of the results from a simple random sample......Page 6 Example: 60Co activity in an estuary......Page 7 Systematic sampling......Page 9 Introduction......Page 10 Spatial scale......Page 11 Classical spatial sampling methods......Page 12 Other sampling methods......Page 13 Practical sampling issues......Page 14 References......Page 15 Introduction......Page 17 Sampling homogenization versus speciation......Page 19 Ontology of environmental analysis......Page 21 Data quality objectives......Page 23 Sampling plan......Page 24 Simple random sampling......Page 27 Stratified-random sampling......Page 28 Geostatistical (random field) sampling......Page 29 Hot spot identification......Page 30 Visual Sample Plan VSP 3.0......Page 31 Replicates, composite and collocated samples......Page 32 Field sample preparation and preservation......Page 35 Sample spiking and isotope labeling......Page 36 Air and aerosols......Page 37 Water and precipitation......Page 39 Archaeological and geological samples......Page 40 Biota and food......Page 42 References......Page 43 Introduction......Page 48 Early history......Page 50 Recent history; toward international consensus......Page 51 ISO-IUPAC harmonization efforts: 1993-1998......Page 52 Detection decisions and detection, quantification capabilities: introduction to the basic concepts and relationships......Page 53 Defining relations; algebraic formulation......Page 54 Graphical representation: detection of earthquake precursors......Page 55 Simplified relations3......Page 57 Heteroscedasticity and counting experiments......Page 58 Accuracy of the (Poisson-normal) expressions for SC, SD......Page 59 Confidence intervals (normal, Poisson) for B, given Bobs......Page 60 Minimum B for acceptable uncertainties in SD and alpha......Page 62 Uncertainty in alpha and use of a threshold......Page 63 A conservative approach to SC; a lesson from accelerator mass spectrometry......Page 64 The concentration (x-) domain......Page 65 Calibration function known or assumed (eA negligible or fixed)......Page 66 Case I: The x distribution; application of the Taylor expansion IUP1995,Kur1985......Page 67 Case II: Quasi-concentration domain: calibration-based limits......Page 69 Notes......Page 70 Case III: Exact treatment for xC, xD......Page 71 Multicomponent detection......Page 73 Setting the stage......Page 74 Multiple, independent detection decisions......Page 76 Multiple false negatives (quasi-Bayesian approach)......Page 77 Multivariate detection decisions and limits......Page 78 The multivariate blank and estimated covariance......Page 80 The blank as an ultimate limiting factor; blank manifestations, dimensionality......Page 82 Assessment of the blank......Page 84 Calibration based detection limits: the blank as the intercept of the calibration function, and sigma2B as the intercept of the variance function......Page 86 Sensitivity as an ultimate limiting factor; the transition from decay counting to atom counting......Page 87 Detection vs Discrimination Limits: impact of the environmental background......Page 90 Distribution of the sulfur laboratory blank......Page 94 Distribution of the 85Kr environmental background......Page 95 Conclusion.......Page 97 Notation.......Page 99 Overcoming the inequality......Page 101 Extreme low-level (Poisson) detection decisions and limits for paired counting (eta=2)......Page 102 Critical region.......Page 103 alpha-Control.......Page 104 Some closing observations, and reference to other work......Page 105 Background as a Poisson process; expected characteristics......Page 107 Empirical distributions and tests of the Poisson (background) hypothesis......Page 108 Conclusion.......Page 110 Detection limits: intralaboratory vs interlaboratory perspectives......Page 111 Statement of the problem; values and non-values......Page 115 Substitution bias functions.......Page 116 Impact of hardware/software thresholds.......Page 117 Examples of applications......Page 118 Peak detection (gamma-ray spectrometry)......Page 119 Example 1: low-level beta counting (39Ar)......Page 120 Equations for Poisson-normal variables (counts)......Page 121 Set-2 data......Page 122 Example 2: gamma-ray peak detection......Page 123 Background limiting......Page 124 Algorithm dependence.......Page 125 Detection, quantification limits (replication variance)......Page 126 t-Statistics......Page 127 Summary......Page 128 Notes......Page 129 References......Page 130 Introduction......Page 135 Background......Page 137 Recommended procedure......Page 139 Surface 137Cs in the ocean......Page 140 Cross-section of 137Cs along 165°E in the Pacific......Page 143 Background......Page 144 Radiochemical separation......Page 145 90Sr concentrations in the water column in the Pacific Ocean......Page 146 Background......Page 147 Pre-concentration of Pu......Page 149 Radiochemical separation......Page 150 Electrodeposition......Page 151 Surface 239,240Pu concentrations in the open ocean......Page 152 Vertical profiles of 239,240Pu in the ocean......Page 153 Conclusion......Page 155 References......Page 156 Introduction......Page 161 Cosmic radiation......Page 162 Radioactivity of construction materials of the shielding......Page 166 Radioactivity of construction materials of the detector......Page 168 Fluxes of cosmic muons......Page 169 Muon momentum......Page 170 Polar direction......Page 171 Temporal variations......Page 172 Ionization and delta electron production......Page 173 Direct electron-positron pair production......Page 174 Multiple scattering......Page 175 Muon decay......Page 176 Negative muon capture......Page 177 Ionization and delta electron production......Page 178 Compton scattering......Page 179 Surface simulations......Page 180 Anti-Compton shielding......Page 183 Single gamma-ray spectrometer......Page 185 Anti-Compton spectrometer......Page 189 Comparison of modeling and experimental results......Page 191 Gamma-ray spectrometers with anticosmic shielding......Page 192 Coincidence-anticoincidence (anti-Compton) gamma-ray spectrometer......Page 194 Background characteristics of HPGe detectors with anticosmic shielding......Page 197 Background characteristics of the anti-Compton gamma-ray spectrometer......Page 201 Conclusions......Page 202 References......Page 204 Introduction......Page 207 Cosmic rays in the atmosphere......Page 209 Nuclear reactions in the atmosphere......Page 210 Production of neutrons......Page 211 Muons......Page 212 Electrons (positrons) and photons......Page 213 Radioactivity of rocks and building materials......Page 214 Measures for the reduction of the intrinsic detector radioactivity......Page 215 Selection of paint for the protection of the inner surfaces of the shielded chamber and of installation materials......Page 216 Shielding of detectors......Page 217 Muons......Page 218 Rocks as natural neutron sources......Page 219 Reaction of cosmic rays with the shielding material......Page 220 Electrons and photons......Page 223 Selected underground laboratories......Page 224 IAEA-MEL laboratory......Page 226 ``Felsenkeller'' underground laboratory in Dresden......Page 227 Solotvina underground laboratory......Page 228 Gran Sasso National Laboratory......Page 229 Gas counters in underground laboratories......Page 230 Liquid scintillation counting......Page 231 Investigation of meteorites......Page 232 Intrinsic radioactivity of detectors......Page 233 References......Page 234 Introduction......Page 238 Radiocarbon dating by accelerator mass spectrometry......Page 239 The NSF Arizona Accelerator Mass Spectrometry Laboratory......Page 240 Sample pretreatment and processing......Page 241 Plasma oxidation sample preparation system......Page 242 Automated sample processing......Page 243 Extension of the tree ring record......Page 244 INTCAL98 and INTCAL04......Page 245 Other calibration records......Page 246 Paleoclimate studies......Page 248 Forest fire studies......Page 249 Studies of extinct megafauna......Page 250 In situ-produced cosmogenic radionuclides......Page 251 10Be studies......Page 252 Acknowledgements......Page 254 References......Page 255 Introduction......Page 260 Uranium-236......Page 261 Neptunium-237......Page 262 Iodine-129......Page 263 Technetium-99......Page 264 Advantages of AMS relative to conventional mass spectrometry......Page 265 Negative ion source......Page 266 Acceleration and stripping......Page 267 Final analysis and detection......Page 268 Ionization chambers......Page 269 Time-of-flight systems......Page 272 ANU......Page 273 Lawrence Livermore National Laboratory......Page 274 VERA......Page 275 ETH, Zurich......Page 276 Efficiency......Page 277 Plutonium......Page 278 Uranium-236......Page 280 Sample preparation......Page 281 Tracing discharges from plutonium-processing and fuel reprocessing plants......Page 282 Safeguards......Page 284 Plutonium as a tracer of soil erosion and sediment transport......Page 285 Ores......Page 286 Summary......Page 287 References......Page 288 Introduction......Page 291 Analysis of Pu-isotopes......Page 297 Abundance sensitivity and UH+......Page 298 Polyatomic interferences......Page 301 Sample introduction system......Page 303 Analysis of 237Np......Page 306 Analysis of 99Tc......Page 309 Interferences......Page 312 Analysis of 129I......Page 314 Analysis of 90Sr, 135Cs and 137Cs......Page 316 Analysis of 210Pb......Page 318 Analysis of 226Ra......Page 319 Analysis of U and Th isotopes......Page 320 References......Page 321 Introduction......Page 327 Principles of resonance ionization mass spectrometry......Page 328 Atom sources......Page 329 Resonant optical excitation......Page 330 Mass analyzers and ion detection......Page 333 High sensitivity, moderate resolution pulsed laser RIMS......Page 334 Pulsed laser RIMS in a laser ion source......Page 336 High resolution RIMS for ultra high isotopic selectivity......Page 338 Noble gas determination using pre-enrichment and pulsed laser RIMS......Page 339 Multi-step RIMS on thermal atomic beams-a universal approach......Page 340 Future prospects of RIMS......Page 343 Conclusion and outlook......Page 345 References......Page 346 Introduction......Page 351 Characterization of depleted uranium particles......Page 353 Characterization of uranium-containing particles originating from a nuclear fuel reprocessing plant......Page 355 Characterization of U/Pu particles from an inadvertent destruction of nuclear weapons......Page 358 Conclusions......Page 363 References......Page 364 Introduction......Page 367 Principle of activation analysis......Page 368 Methodology and equipment......Page 370 Sampling......Page 371 Sample preparation......Page 372 Irradiation......Page 373 Measurement......Page 374 Chemical recovery......Page 375 Analysis of gamma spectrum and NAA calculation......Page 376 Evaluation and quality assurance......Page 377 Advantage of activation analysis for the determination of long-lived radionuclides......Page 379 Iodine-129......Page 380 Neptunium-237......Page 386 Technetium-99......Page 390 Cesium-135......Page 392 Uranium-235, 238 and thorium-232......Page 394 References......Page 397 The philosophy and scope......Page 402 Historical perspective......Page 404 Soil compositions......Page 406 Photon fluence equations and fields of view......Page 407 Depth distributions......Page 411 Spectral processing......Page 413 Instrumentation......Page 416 HPGe detectors......Page 417 Calibration......Page 419 Conversion to gamma dose quantities......Page 420 Total or partial energy method......Page 421 Calibration corrections......Page 422 The full energy peak to forward scattered ratio (peak to valley method)......Page 423 Mapping the accumulation of 137Cs in salt marsh environments......Page 425 Mapping soil erosion and field moist bulk density across cultivated fields through in situ gamma-ray spectrometry......Page 428 The UK's national soil and herbage pollution survey......Page 430 Instrumentation......Page 432 Airborne gamma ray surveys of nuclear sites: Mol Dessel, Belgium......Page 434 ECCOMAGS European Intercomparison Exercise......Page 436 Summary and conclusions......Page 437 References......Page 438 Introduction......Page 444 Dual HPGe-NaI(Tl) detector system......Page 446 Small NaI(Tl) detector......Page 447 Stationary detection system......Page 448 Investigation of radioactive waste dumping sites in the Kara Sea......Page 451 Mapping of radionuclides in Mururoa and Fangataufa lagoons sediments......Page 452 Mapping of 137Cs in Irish Sea sediments......Page 454 In situ stationary monitoring of radionuclides in seawater in the NW Irish Sea......Page 459 Submarine groundwater discharge studies......Page 461 Monitoring of SGD using an underwater gamma-ray spectrometer......Page 462 Study area offshore of SE Sicily......Page 463 Study area offshore of SE Brazil......Page 465 Submarine groundwater discharge estimates offshore of Brazil......Page 468 Comparison of Sicilian and Brazilian results......Page 469 Acknowledgements......Page 470 References......Page 471 sdarticle_015.pdf......Page 475 sdarticle_016.pdf......Page 518