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Handbook of radioactivity analysis vol 2

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Handbook of Radioactivity
Analysis
Volume 2: Radioanalytical Applications

Fourth Edition

Edited by

Michael F. L’Annunziata
Academic Press is an imprint of Elsevier
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elsevier.com/permissions.
This book and the individual contributions contained in it are protected under copyright by the Publisher (other than as may
be noted herein).
Notices
Knowledge and best practice in this field are constantly changing. As new research and experience broaden our understanding,
changes in research methods, professional practices, or medical treatment may become necessary.
Practitioners and researchers must always rely on their own experience and knowledge in evaluating and using any
information, methods, compounds, or experiments described herein. In using such information or methods they should be
mindful of their own safety and the safety of others, including parties for whom they have a professional responsibility.
To the fullest extent of the law, neither the Publisher nor the authors, contributors, or editors, assume any liability for any
injury and/or damage to persons or property as a matter of products liability, negligence or otherwise, or from any use or
operation of any methods, products, instructions, or ideas contained in the material herein.

Library of Congress Cataloging-in-Publication Data


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A catalogue record for this book is available from the British Library
ISBN: 978-0-12-814395-7

For information on all Academic Press publications visit our website at


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Publisher: Susan Dennis


Acquisition Editor: Kathryn Eryilmaz
Editorial Project Manager: Hilary Carr
Production Project Manager: Prem Kumar Kaliamoorthi
Cover Designer: Matthew Limbert
Typeset by TNQ Technologies
Contributors

Nicole Barthe, Univ. Bordeaux, bioingénierie tissulaire, Agustín Grau Carles, Academia BIC, Madrid, Spain
Bordeaux, France; INSERM, bioingénierie tissulaire, Agustín Grau Malonda, CIEMAT, Madrid, Spain
Bordeaux, France
Xiaolin Hou, Technical University of Denmark, Depart-
Maria Betti, Directorate G - Nuclear Safety and Security, ment of Environmental Engineering, Roskilde,
European Commission, DG Joint Research Centre, Denmark; Lanzhou University, School of Nuclear
Karlsruhe, Germany; Formerly at the International Science and Technology, Lanzhou, China
Atomic Energy Agency, Environmental Laboratories,
Monaco Philip Hypes, Los Alamos National Laboratory, Hazard-
ous Materials Management Group, Los Alamos, NM,
Ana Cardona (In Memoriam), Institut Pasteur, Paris, United States
France
Alexandra Ioannidou, Aristotle University of Thessalo-
Nicolas Carvou, Biospace Lab UK, Warwick, United niki, Physics Department, Nuclear Physics Laboratory,
Kingdom Thessaloniki, Greece
Xiongxin Dai, China Institute for Radiation Protection, Miroslav Jeskovský, Comenius University, Faculty of
Taiyuan, Shanxi Province, China Mathematics, Physics and Informatics, Department of
Oleg B. Egorov, Medvio, LLC, West Richland, WA, Nuclear Physics and Biophysics, Bratislava, Slovakia
United States Jakub Kaizer, Comenius University, Faculty of Mathe-
Konstantinos Eleftheriadis, Environmental Radioactivity matics, Physics and Informatics, Department of Nuclear
Laboratory, Institute of Nuclear and Radiological Sci- Physics and Biophysics, Bratislava, Slovakia
ence & Technology, Energy & Safety, N.C.S.R. Ivan Kontul’, Comenius University, Faculty of Mathe-
“Demokritos”, Ag. Paraskevi, Attiki, Greece matics, Physics and Informatics, Department of Nuclear
Rudolf Engelbrecht, Radiochemistry, Seibersdorf Labor Physics and Biophysics, Bratislava, Slovakia
GmbH, Seibersdorf, Austria; Currently - Austrian Michael J. Kristo, Lawrence Livermore National Labo-
Agency for Health and Food Security, GmbH, Vienna ratory, Livermore, CA, United States
Mats Eriksson, Swedish Radiation Safety Authority, Michael F. L’Annunziata, The Montague Group, Ocean-
Department of Radiation Protection, Stockholm, Swe- side, CA, United States
den; Formerly at the International Atomic Energy
Agency, Environmental Laboratories, Monaco Galina Lujaniené, SRI Center for Physical Sciences and
Technology, Vilnius, Lithuania
William Geist, Los Alamos National Laboratory, Safe-
guards Science Technology Group, Los Alamos, NM, Serge Maîtrejean, SMTJ Consulting, Paris, France
United States Monika Müllerová, Comenius University, Faculty of

Zeljko Grahek, Laboratory for Radioecology, RuCer Mathematics, Physics and Informatics, Department of
Boskovic Institute, Zagreb, Croatia Nuclear Physics and Biophysics, Bratislava, Slovakia
Jay W. Grate, Pacific Northwest National Laboratory, Matthew J. O’Hara, Pacific Northwest National Labo-
Richland, WA, United States ratory, Richland, WA, United States

xxvii
xxviii Contributors

Pavel P. Povinec, Comenius University, Faculty of Jan Scholten, Institute of Geosciences, Kiel University,
Mathematics, Physics and Informatics, Department of Kiel, Germany; Formerly at the International Atomic
Nuclear Physics and Biophysics, Bratislava, Slovakia; Energy Agency, Environmental Laboratories, Monaco
Formerly at the International Atomic Energy Agency, Natasa Todorovic, University of Novi Sad, Faculty of
Environmental Laboratories, Monaco Sciences, Department of Physics, Nuclear Physics
Peter Santi, Los Alamos National Laboratory, Safeguards Laboratory, Novi Sad, Serbia
Science Technology Group, Los Alamos, NM, United
States
About the Founding Editor

(IAEA) in Vienna, Austria, where he served as IAEA Head


of Fellowships and Training during 1987e91. From 1977
to 2007, he served as IAEA Expert in fact-finding, plan-
ning, and implementation assignments in peaceful appli-
cations of nuclear energy for development in more than 50
countries of the world in Asia, Africa, Europe, Latin
America, and the Middle East. L’Annunziata was a mem-
ber of the Board of Governors, International Science
Programs at Uppsala University, between 1988 and 1991.
His main research interests have been focused on the
development of chemical and instrumental methods for the
detection and measurement of radioactive nuclides as
tracers in research. He was the first to postulate the soil
Michael F. L’Annunziata microbial epimerization of myo-inositol to other inositol
stereoisomers as a source of the stereoisomers of inositol
phosphates in soils (PhD dissertation, 1970, https://
Michael F. L’Annunziata, PhD, is the founding editor dissexpress.proquest.com/dxweb/results.html?QryTxt¼&By¼
and coauthor of the Handbook of Radioactivity Analysis. L%27Annunziata&Title¼&pubnum ¼ ) and in 1975 (SSSA
He majored in chemistry with a BSc degree from Journal 39(2), 377e379) and first to demonstrate in 1977,
St. Edward’s University in 1965, and he was awarded MSc with the use of the radioisotope carbon-14, the soil mi-
and PhD degrees from the University of Arizona, Tucson, crobial epimerization of myo-inositol to chiro-inositol as a
in 1967 and 1970, respectively. His graduate thesis research mechanism involved in the origin of the unique soil inositol
in the 1960s, financed by the then US Atomic Energy phosphate stereoisomers (SSSA Journal 41(4), 733e736,
Commission, dealt with the analysis of the radionuclides https://dl.sciencesocieties.org/publications/sssaj/abstracts/
89
Sr and 90Sr and the remediation of soils contaminated 41/4/SS0410040733). The first edition of the Handbook of
with radiostrontium in the event of nuclear fallout, pub- Radioactivity Analysis was planned by L’Annunziata in
lished as a thesis in 1967 (https://repository.arizona.edu/ 1995, and he edited and coauthored the subsequent edi-
handle/10150/318640). After a short stint in the chemical tions, including the current fourth edition published by
industry (Amchem Products, Inc, Ambler, Pennsylvania) Elsevier in 2019. He has authored and coauthored 11 books
during 1970e71 as 14C-tracer chemist, he joined the since 1979 on radionuclide analysis and radiation physics
faculty at the Postgraduate College in Chapingo, Mexico, among which his book entitled Radioactivity: Introduction
as a professor and thesis advisor during 1972e75, and and History, First Edition, published by Elsevier in 2007,
during 1975e77, L’Annunziata was a senior research sci- was included on the Best Sellers List in Physics (Librar-
entist at the Nuclear Center of the National Institute of yJournal Academic Newswire) in 2008. His much
Nuclear Research (ININ), Mexico, where he served also as expanded Second Edition entitled Radioactivity: Introduc-
a thesis research advisor to graduate students of chemistry tion and History, From the Quantum to Quarks (https://
of the Autonomous University of the State of Mexico in www.sciencedirect.com/book/9780444634894/radioactivity),
Toluca, Mexico, in the field of radionuclide analysis and published by Elsevier in 2016, was awarded an Honorary
applications. During 1977e91, he was a scientific officer in Mention in the 2017 PROSE AWARDS in the category of
the Departments of Research and Isotopes and Technical Chemistry and Physics.
Cooperation of the International Atomic Energy Agency

xxix
Foreword

Radioactive sources play a significant role in promoting human development and health worldwide. Whether through its
application to treat cancer, diagnose various diseases, develop new crop varieties, sterilize medical supplies, or provide
clean energy, peaceful uses of radioactive sources are ubiquitous in our daily lives. These wide-ranging applications can
only be implemented appropriately when radioactivity is measured precisely. Thus, the accurate measurement of nuclear
radiation is indispensable for the peaceful applications of radioactive materials. For example, in fields such as nuclear
medicine, whether for the treatment or diagnosis of disease, accurate measurements of radionuclides are essential.
Dosimetric measurements are the cornerstone of safe and effective radiation therapy for the treatment of cancer whether for
brachytherapy, proton beam therapy, or other sources of radiation therapy.
With more than 170 Member States in all continents of the world, the International Atomic Energy Agency (IAEA)
serves as the global focal point for nuclear cooperation. The Handbook of Radioactivity Analysis will serve Member States
as one of many tools available in the application of nuclear science and technology for peaceful purposes. The importance
of this guidance is demonstrated by the wide range of areas in which the IAEA supports Member States to contribute to
their well-being and development. Such examples include biological sciences research, insect pest control, health, fertilizer
and water use efficiency, water resources and the environment including marine science and climate change, radiation
technology, neutron diffraction, radiography and activation analysis, radiation processing in industry, radiation protection,
nuclear power, nuclear safeguards, radiation preparedness and response, and research in the field of nuclear fusion, among
others.
The Handbook of Radioactivity Analysis is now in its fourth edition since the successful first edition in 1998. Over the
past two decades, this book has expanded in its scope from an initial 12 chapters to the current 22 chapters, encompassing
the numerous modern applications and methods of radiation detection and measurement. The chapters in this book are
written by experts from 16 countries around the world. This new edition will continue to serve as an important resource in
our search to optimize radioactivity measurements both in research and in its applications, leading to the peaceful utili-
zation of radioactive sources for health and development.

May Abdel-Wahab, MD, PhD, FACR


Director, Division of Human Health
Department of Nuclear Sciences and Applications
International Atomic Energy Agency, Vienna

xxxi
Preface to the fourth edition

In 1996, I proposed to Academic Press the idea of a book that would provide readers with a reference source to state-of-the-
art radiation detectors and methods of analysis of radionuclides and other sources of nuclear radiation. Thus, the first
edition of this book was published in 1998 as a single volume with only 12 chapters, and the book has expanded in scope
and depth over the past two decades with the current fourth edition and its 22 chapters in two volumes.
The numerous advances that have been made since the publication of the previous third edition warranted the partition
of the Handbook of Radioactivity Analysis into two volumes. It was decided to separate the chapters into two categories,
namely, Volume 1, Radiation Physics and Detectors and Volume 2, Radioanalytical Applications. The two volumes of this
book were expanded greatly to provide material, which would serve as a valuable resource in teaching and a reference
source to the researcher in his or her unique analytical requirements in the measurement of radioactive materials.
The first chapter in Volume 1, which was previously entitled Radiation Physics and Radionuclide Decay, was
expanded to almost double in volume with a corresponding change in the chapter title to The Atomic Nucleus, Nuclear
Radiation, and the Interaction of Radiation with Matter, which includes additional material helpful to supplement the
academic curricula and aid in the decisions and calculations made by researchers in their measurement of nuclear radiation
and radionuclide analysis. Current principles of operation of all classes of radiation detectors and their applications have
been expanded and updated, including semiconductor detectors, gas ionization detectors, liquid and solid scintillation
detectors, solid-state nuclear track detectors, Cherenkov detectors, calorimeters and bolometers, as well as advances in
atom counting (i.e., mass spectrometry) for the measurement of radioactive and stable nuclides and radiation from other
sources such as cosmic radiation, synchrotron radiation, and particle emissions from nuclear reactions.
In light of increased concern for radioactivity in the environment, a chapter was added on the Analysis of Environ-
mental Radionuclides in Volume 2. Also, all chapters in Volume 2 have been expanded and updated with material required
in the analysis of radionuclides and radiation in our land, air, and water resources, including the marine environment, as
well as particle identification and measurement by Cherenkov counting, radiation counting statistics, radionuclide stan-
dardization, imaging techniques required in the applications of radionuclides in biological research and nuclear medicine,
flow-cell analytical techniques, automation in radiochemical analysis together with analytical techniques required in the
fields of nuclear safeguards and nuclear forensics.
Again, we have completed this book as an international effort by drawing upon the expertise of researchers and teachers
from 16 countries of the world. Although coming from many branches of science, chapter authors all share one common
objective, that being the most accurate measurement of radiation sources and radionuclides both natural and man-made,
vital to all branches of science and human development. Readers interested in radiation physics, the applications of ra-
dionuclides and radiation sources, and how these have been vital to our well-being and development may refer to another
text by the writer entitled “Radioactivity: Introduction and History, From the Quantum to Quarks” (ISBN: 978-0-444-
63489-4), published in 2016 by Elsevier (https://www.elsevier.com/books/radioactivity/lannunziata/978-0-444-63489-4).
Women are the senior authors of three chapters in this new edition, which is evidence of the increasing role of women
as leaders in this field of science. We may expect to see yet in the future an ever-increasing number of women, who will
make great advances in this field of science following the pioneering examples of Marie Curie, Lise Meitner, Maria
Goeppert-Mayer, Rosalind Franklin, Marietta Blau, and Chien-Shiung Wu, among others.
Mention of commercial products in this book does not imply recommendation or endorsement by the chapter authors or
editor. Other or more suitable products may be available. Names of products are included for convenience or information
purposes only.
I would like to thank the authors of each chapter, who have covered their fields of expertise with an unwavering
commitment to meet the objectives of this book. Acknowledgment is extended to Kathryn Eryilmaz (nee Morrissey),

xxxiii
xxxiv Preface to the fourth edition

Aquisition Editor, at Elsevier in Cambridge for approaching me with the suggestion that we consider a fourth edition and
for working with me during the planning stage of this book. Many thanks go to Hilary Carr, Elsevier Editorial Project
Manager, for her constant support and advice throughout the writing and production of this book. I thank also Ashwathi P.
Aravindakshan of Elsevier for her assistance in completing the legal requirements for the publication of this book.
Appreciation is also extended to Prem Kumar Kaliamoorthi, Elsevier Production Project Manager, for his meticulous
attention to every detail throughout the production process of this book. Thanks are also extended to Susan Dennis,
Publisher of Elsevier Chemistry and Chemical Engineering Books, and Mona Zahir, Elsevier Editorial Project Manager,
for their guidance and support during this project. Above all, I thank my wife Maria del Carmen (aka Reyna) for her
understanding, encouragement, and unflagging patience.

Michael F. L’Annunziata, PhD


Acronyms, Abbreviations, and Symbols

A Mass number ANL Argonne National Laboratory


A Ampere (1 A ¼ 1 C/s), amplifier ANN Artificial neural network
a Year(s) ANSI American National Standards Institute
Å Angstrom (1010 m ¼ 0.1 nm) ANSTO Australian Nuclear Science and Technology Organisation
AABW Antarctic Bottom Water ANTARES ANTArctic RESearch, Astronomy with a Neutrino
AAIW Antarctic Intermediate Water Telescope and Abyss Environmental RESearch, Mediterranean
AAS Atomic absorption spectrometry Sea
AASI Advanced alpha-spectrometric simulation ANZECC Australian and New Zealand Environment Conservation
ATTA Atom trap trace analysis Council
ABACC BrazilianeArgentine Agency for Accounting and Control APCI Atmospheric pressure chemical ionization
of Nuclear Materials APD Avalanche photodiode
ABEC aqueous biphasic extraction chromatography APDC Ammonium pyrrolidine dithiocarbamate
AC Alternating current APE Alkyl phenol ethoxylate
ACC Antarctic Circumpolar Current APMP AsiaePacific Metrology Program
ACFM Actual cubic feet per minute (28.3 L/min.) APS Advanced Photon Source, Argonne National Laboratory
ADC Analog-to-digital converter AQC Automatic quench compensation
ADF Advanced digital filter AQCS Analytical Quality Control Services (of IAEA)
ADME Absorption, distribution, metabolism, and excretion AQP(I) Asymmetric quench parameter of the isotope
ADS Accelerator-driven subcritical reactor ARC Agulhas Return Current
AEC Automatic efficiency compensation, Atomic Energy ARMCANZ Agriculture and Resource Management Council of
Commission Australia and New Zealand
AES Atomic emission spectrometry, Auger electron spectroscopy AS Alpha spectrometry
AF Agulhas Front ASTAR Alpha stopping power and range
AFM Atomic force microscope ASTM American Society for Testing and Materials
AFS Atomic fluorescence spectrometry atm Atmosphere (standard) ¼ 1.01325  105 Pa
a Alpha particle, internal conversion coefficient at % Atom percent
f Proportional to ATP Adenosine triphosphate
ag Attogram ¼ 1018 g ATSDR Agency for Toxic Substances and Disease Registry
AGeV GeV per nucleon AUV Autonomous underwater vehicle
AkeV keV per nucleon AWCC Active Well Coincidence Counter
A2LA American Association for Laboratory Accreditation AWE United Kingdom Atomic Weapons Establishment
AM b-artemether, arithmetic mean b Particle relative phase velocity, beta particle
AMAD Activity median aerodynamic diameter bb Double-beta decay
AMANDA Antarctic Muon and Neutrino Detector Array, South b Negatron, negative beta particle
Pole bþ Positron, positive beta particle
AMANDE Accelerator for Metrology and Neutron Applications in b Barn ¼ 1028 m2 ¼ 1024 cm2
External Dosimetry, IRSN, France BAC N,N0 -bisacrylylcystamine
AMAP Arctic Monitoring and Assessment Programme bar 105 N/m2 ¼ 100  103 Pa
AMeV MeV per nucleon BBD 2,5-Di-(4-biphenylyl)-1,3,4-oxadiazole
AMP Adenosine monophosphate, ammonium molybdophosphate, BBO 2,5-Di(4-biphenylyl)oxazole
amplifier BBOT 2,5-Bis-2-(5-t-butyl-benzoxazolyl) thiophene
amp. Amplifier BCC Burst counting circuitry, Bragg curve counter
AMS Accelerator mass spectrometry BDs Bubble detectors
amu Atomic mass units BDE Bond dissociation energy
ANDA 7-Amino-1,3-naphthalenedisulfonic acid BE Binding energy
ANFESH Ferric potassium hexacyanoferrate on a cellulose carrier BEAGLE Blue Ocean Global Expedition
ANITA ANtarctic Impulsive Transient Antenna BEGe Broad-energy germanium detector

xxxv
xxxvi Acronyms, Abbreviations, and Symbols

BGO Bismuth germanate (Bi4Ge3O12) CFN Cross-flow nebulizer


BIPM Bureau international des poids et mesures, Sèvres, France CGE Chamber Gram Estimator
bis-MSB p-Bis-(o-methylstyryl)benzene Ch Channel
BK K-shell electron binding energy CHEREN2 Anisotropy detection model for Cherenkov counting
bkg, BKG Background efficiency
BNCT boron neutron capture therapy CHU Centre hospitalier universitaire
BNL Brookhaven National Laboratory, Upton, New York Ci Curie ¼ 2.22  1012 dpm ¼ 3.7  1010 dps ¼ 37 GBq
BOD Biological oxygen demand CIAE China Institute of Atomic Energy
BOMARC Boeing Michigan Aeronautical Research Center CICM Conventional integral counting method
BOREXINO BOron EXperiment, solar neutrino detector, Italy CID Collision-induced dissociation
Bq Becquerel ¼ 1 dps CIEMAT Centro de Investigaciones Energéticas, Medioambientales
BQM Bqmeter (Consortium BQM, Czech Republic) y Technológicas, Madrid
BR Branching ratio CIRIA Construction Industry Research and Information
BS Backscatter Association
BSA Bovine serum albumin cm Centimeter
BSI The British Standards Institute cm/d Unit of flux from cm3/cm2 per day
BSO Bismuth silicate (Bi4Si3O12) CMB Cosmic microwave background
BSS Bonner sphere spectrometer, Board of Safety Standards CMOS Complementary metal-oxide-semiconductor
BT Bound tritium CMPO Octyl(phenyl)-N,N-di-isobutylcarbamoylmethylphosphine
BTP Bistriazinylpyridine oxide
butyl-PBD 2-(4-t-Butylphenyl)-5-(4-biphenylyl)1,3,4-oxadiazole CMX-4 Collaborative Materials Exercise (fourth by the ITWG)
BWR Boiling water reactor C/N CIEMAT/NIST (efficiency tracing method)
c Speed of light in vacuum (2.9979  108 m/s) CN Cellulose nitrate
C Coulomb (1 C ¼ 1 A s) CN* Unstable compound nucleus
o
C Degrees Celsius CNC Condensation nuclei counter
CAI Calciumealuminum-rich inclusions CNET CIEMAT/NIST efficiency tracing
CaF2(Eu) Europium-activated calcium fluoride CNRS Centre National de la Recherche Scientifique, France
CALEX Calorimetry Exchange Program CNS Central nervous system
CAM Continuous air monitoring COG Center of gravity
CAMAC Computer-automated measurement and control COMPASS Community Pentascale Project for Accelerator Science
CANDLES CAlcium fluoride for the study of Neutrinos and Dark and Simulation
matter by Low Energy Spectrometer COTS Commercial off-the-shelf (system)
CANDU Canadian deuterium uranium reactor cph, CPH Counts per hour
CART Classification and regression tree algorithm cpm, CPM Counts per minute, channel photomultiplier
CAVE Counting lAboratory for enVironmental radionuclidEs, cps, CPS Counts per second
Monaco CR-39 Polyallyldiglycol carbonate plastic SSNTD
CC Charged current (interaction), charge comparison, carbonate CRESST Cryogenic Rare Event Search with Superconducting
carbon Thermometers
CCD Charge-coupled device CRL Compound refractive lens
CCRI Consultative Committee for Ionizing Radiation CRM Certified reference material
CD ROM Compact disc read-only memory CS Calibration source
CDW Circumpolar Deep Water CSDA Continuous Slowing Down Approximation range
CE Chemical etching, capillary electrophoresis CSIC Instituto de Física Fundamental, Madrid
CEA Commissariat à l’Energie Atomique CsI(Na) Sodium-activated cesium iodide
CEFAS Centre for Environment, Fisheries and Aquaculture Sci- CsI(Tl) Thallium-activated cesium iodide
ence (UK) CT Computerized tomography
CE-ICP-MS Capillary electrophoresiseinductively coupled plasma CTBT Comprehensive Nuclear-Test-Ban Treaty
mass spectrometry CTBTO Comprehensive Nuclear-Test-Ban Treaty Organization
CELLAR Collaboration of European Low-level Underground CTD Conductivity/temperature/density detector
Laboratories CTF Contrast transfer function
CENTA Centre for Nuclear and Accelerator Technologies, CTFE Chlorotrifluoroethylene
Bratislava CTR Controlled thermonuclear reactor
CERN European Organization for Nuclear Research, Geneva cts Counts
CET Compton efficiency tracing method CV Core valence
CF Feedback capacitor cv Column volume
CF Calibration factor, correction factor CWOSL Continuous wave optically stimulated luminescence
CFD Constant fraction discriminator CZT Cadmium zinc telluride (semiconductor detectors)
cfm Cubic feet per minute D Deuterium
Acronyms, Abbreviations, and Symbols xxxvii

d Days, deuteron, down quark DSP Digital signal processing


d Antidown quark DT Dead time
2D Two-dimensional DTPA Diethylenetriamine pentaacetic acid
DA Destructive analysis DTSA Desktop spectrum analyzer (software)
Da Dalton (unified atomic mass unit, also abbreviated as u) DU Depleted uranium
DAC Derived air concentration DWL Drinking water limit
DAP Diallyl phthalate DWPF Defense waste processing facility
DASE Le Département analyse, surveillance, environnement, E Counting efficiency, energy
France Eb Binding energy
DATDA Diallyltartardiamide eD Positron
DBD Double-beta decay eL Electron, negatron
DC Direct current eLhD or eLh Electronhole pair
DCC Digital coincidence counting EBq Exabecquerel (1018 Bq)
dc-GDMS Direct currenteglow discharge mass spectrometry EC Electron capture, extraction chromatography, European Com-
DDCP Dibutyl-N,N-diethylcarbamylphosphonate munity, elemental carbon
DDTC Diethyldithiocarbamate ECD Effective cutoff diameter
DE Double escape ECDL Extended cavity diode laser
DEF Delayed ettringite formation ECE Electrochemical etching
d Delta rays ECR Electron cyclotron resonance
DEMO Demonstration Power Plant (fusion) ED Exponential decrease
DESR Double external standard relation EDS Energy dispersive spectrometer
DESY Deutsches Elektronen Synchrotron EDTA Ethylenediamine tetraacetic acid
Det. Detector EDX Energy dispersive X-ray (spectrometer)
DF Decontamination factor EDXRF Energy dispersive X-ray fluorescence
DF-ICP-MS Double focusing ICP-MS EESI-MS Extractive electrospray ionization tandem mass
DGA Diglycolamide spectrometry
DIC Dissolved inorganic carbon EeV Exaelectron volts (1018 eV)
DIHEN Direct injection high-efficiency nebulizer EF Fermi level
DIM Data interpretation module EF Enrichment factor
dimethyl POPOP 1,4-Bis-2-(4-methyl-5-phenyloxazolyl)benzene Eh Oxidation potential
DiMF Decay in a magnetic field (method) EI Electron impact (e.g., in mass spectrometry)
DIN Diisopropylnaphthalene EIA Enzyme immunoassay
DIPE Diisopropyl ether EM Electromagnetic
DIPEX Bis(2-ethylhexyl)methane-diphosphonic acid EMA Extramural absorber
DIRC Detector of internally reflected Cherenkov light EMCCD Electron multiplier CCD
DJD Diffused junction detector EML Environmental Measurement Laboratory, USA
DLU Digital light units EMPA Electron microprobe analysis
DMCA Digital multichannel analyzer ENEA Italian National Agency for New Technologies, Energy and
DMF Digital microfluidics Sustainable Economic Development
DMG Dimethylglyoxime ENSDF Evaluated Nuclear Structure Data File
DMM Direct matrices multiplication EO Ethylene oxide
DMSO Dimethyl sulfoxide EPA US Environmental Protection Agency
DNA Deoxyribonucleic acid EPCRA Emergency Planning and Community Right-to-Know Act
D2O Heavy water EPR Electron paramagnetic resonance
DOC Dissolved organic carbon ERBSS Extended-range Bonner sphere spectrometer
DOE US Department of Energy erg Energy unit (1 erg ¼ 6.2415  1011 eV ¼ 107 J)
DOELAP Department of Energy Laboratory Accreditation Program ES Elastic scattering, external standard
DOM Digital optical module ESA European Space Agency, Paris; electrostatic analyzer
DOP Dioctyl phthalate ESCR External standard channels ratio
DOT Digital overlay technique ESI Electrospray ionization
dpm, DPM Disintegrations per minute ESIR WG Extended SIR Working Group
dps, DPS Disintegrations per second ESP External standard pulse
DPSD Digital pulse shape discrimination ESTAR Electron stopping power and range
dpy, DPY Disintegrations per year esu Electrostatic unit
DQP Double quench parameter ET Efficiency tracing
DRAM Dynamic random access memory ET-DPM Efficiency tracing disintegrations per minute (method)
DSA Defined solid angle ETH Eidgenössische Technische Hochschule, Zurich
DSES Deep sea echo sounder
xxxviii Acronyms, Abbreviations, and Symbols

ETV-ICP-MS Electrothermal vaporizationeinductively coupled Ge(Li) Lithium-compensated germanium


plasma mass spectrometry GEM Gas electron multiplier
Eav Average energy (beta particle) GEOSECS Geochemical Ocean Sections Programme
Emax Maximum energy (beta particle), Compton electron energy GEOTRACES International Study on Marine Biogeochemical
maximum Cycling of Trace Elements and their Isotopes
Ea Alpha-particle energy GERDA GERmanium Detector Array
Ep Proton energy GeV Gigaelectron volts (109 eV)
Eth Threshold energy GHz Gigahertz (109 Hz)
EU European Union GICNT Global Initiative to Combat Nuclear Terrorism
EUChemS European Chemical Society GIS Geographical Information System
EURACHEM European organization for traceability of chemical GISP Greenland Ice Sheet Projects
measurements GLOMARD Global Marine Radioactivity Database
EURADOS European Radiation Dosimetry Group GLP Good laboratory practice
EURATOM European Atomic Energy Community GM GeigereMüller
EUROMET European Collaboration in Measurement Standards GM-APD Geiger-mode avalanche photodiode
eV Electron volt ¼ 1.602176  1019 J ¼ 1.602176  1012 erg) GPa Gigapascal
EXAFS X-ray absorption fine structure GPC Gas proportional counting (counter)
o
F Degrees Fahrenheit GPD Geometric progression decrease
FADC Fast analog digital converter CPG Coplanar grid
fC Fraction of contemporary cabon GPS Global positioning system
FDA US Food and Drug Administration GRB Gamma ray burst
FDG Fluorodeoxyglucose GS-20 Glass scintillator
FDNPP Fukushima Dai-ichi Nuclear Power Plant, Japan GSD Geometric standard deviation
FDNPS Fukushima Dai-ichi Nuclear Power Station, Japan GSI Gesellschaft für Schwerionenforschung mbH, Darmstadt,
FEP Full energy peak Germany
FET Field effect transistor GSO:Ce Cerium-activated gadolinium orthosilicate (Gd2SiO5:Ce)
FFF Field flow fractionation GUM Guide to the Expression of Uncertainty in Measurement
fg Femtogram (1015 g) GW Groundwater, gate width
FGRM Flow-through gaseous radiochemical method GWe Gigawatt electrical (109 We)
FI Flow injection Gy Gray (1 Gy ¼ 1 J/kg ¼ 6.24  1012 MeV/kg)
fm Fermi or femtometer (1015 m) GZK Greisen-Zatsepin-Kuz’min process of proton-photon
fM Fraction of modern carbon interactions
fmol Femtomole (1015 mol) h Hours
FNTD Fluorescent nuclear track detector h Plank’s constant (6.626  1034 J s), hours

FOM Figure of merit h Plank’s constant reduced (h/2p)
fov Field of view H # Horrock’s number (quench indicating parameter)
fp Fission products HBT 2-(2-Hydroxyphenyl)-benzothiazole
FPGA Field programmable gate array HDE Heat distribution error
FSA Flow scintillation analysis HDEHP Bis(2-ethylhexyl)phosphoric acid
FS-DPM Full-spectrum disintegrations per minute (method) HDPE High-density polyethylene (moderator)
FT Fission track HEDPA 1-Hydroxyethane-1,1-diphosphonic acid
FTD Fission track dating HEN High efficiency nebulizer
FT-ICR Fourier transformeion cyclotron resonance HEP High-energy particle
FTIR Fourier transform infrared spectroscopy HEPES N-2-hydroxyethylpiperazine-N0 -2-ethanesulfonic acid
FWHM Full width at half-maximum HERA-B RICH Particle detector of the Hadron-Elektron-Ring-
FWT Free water tritium anlage, Hamburg, Germany
FWTM Full width at 10th maximum HERM High-energy radio monitor
g Gram, gluon HEU Highly enriched uranium
G # G-number (Grau’s-number, quench-indicating parameter) HEX-ICP-MS Hexapole collision cell ICP-MS
g Gamma radiation HEX-ICP-QMS Hexapole collision cell quadrupole mass
G-8 Group of Eight Countries (IAEA Member States) spectrometry
GBq Gigabecquerels (109 Bq) 3HF 3-Hydroxy flavone
GC Gas chromatography hg Hectograms (102 g)
GC/MS Gas chromatography/mass spectrometry h-index Hirsh index
GCR Galactic cosmic rays HIBA Hydroxy-i-butyric acid
GD Glow discharge HKG Housekeeping gene
GDMS Glow discharge mass spectrometry HLNC High-level neutron coincidence counter
GEANT Geometry ANd Tracking Monte Carlo code HLW High-level waste
Acronyms, Abbreviations, and Symbols xxxix

HPB High-pressure Bridgman INGE International Noble Gas Experiment


HPGe High-purity germanium INP Institute of Nuclear Physics, Tirana, Albania
HPIC High-performance ionic chromatography IN2P3 Institut National de Physique Nucléaire et de Physique des
HPLC High-performance liquid chromatography Particules, France
HPMT Hybrid photomultiplier tube INSERM Institut national de la santé et de la recherché médicale.
HRAS High-resolution alpha spectrometry France
HRGS High-resolution gamma spectrometry I/O Input/output
HR-ICP-MS High-resolution inductively coupled plasma mass IPA Instrument performance assessment, isopropyl alcohol
spectrometry IPRI Laboratoire Primaire des Rayonnements Ionisants, France
HT High tension IPT Intramolecular proton transfer
HV High voltage IR Infrared (spectroscopy)
HWHM Half width at half-maximum IRA Institut Universitaire de Radiophysique, Lausanne, Switzerland
HWZPR Heavy water zero power reactor IRMM Institute for Reference Materials and Measurements, Geel
Hz Hertz (cycles per second) IRMS Isotope ratio mass spectrometry
iin Current pulse IRSN Institute of Radiation Protection and Nuclear Safety, France
IAEA International Atomic Energy Agency, Vienna IS Internal standard
IAEA-EL IAEA Marine Environment Laboratory, Monaco ISH In situ hybridization
IC Internal conversion, ion chromatography ISO International Organization for Standardization
ICC Ice condenser chamber ISOCS In-Situ object calibration software
IC-ICP-MS Ion chromatographyeinductively coupled plasma mass IS-SCR Internal standard and sample channels ratio
spectrometry IT Isomeric or internal transition
IC# Isotope center number ITER International Thermonuclear Experimental Reactor
IceCube Neutrino Observatory, South Pole ITU Institute for Transuranium Elements, Europe
IceTop Surface array of stations for IceCube ITWG Nuclear Forensics International Technical Working Group
ICF Inertial confinement fusion IUPAC International Union of Pure and Applied Chemistry
ICP Inductively coupled plasma IUPAP International Union of Pure and Applied Physics
ICP-CC-QMS Quadrupole inductively coupled plasma mass spec- J Joule ¼ 1 N m ¼ 1 kg m2/s2 ¼ 1 W s
trometry with hexapole collision cell JAERI Japan Atomic Energy Research Institute
ICP-FT-ICR-MS Inductively coupled plasma Fourier transform JET Joint European Torus reactor
ion cyclotron resonance mass spectrometry JFET Junction field effect transistor
ICP-MS Inductively coupled plasma mass spectrometry JCGM Joint Committee for Guidelines in Metrology
ICP-OES Inductively coupled plasma optical emission spectrom- JINR Joint Institute for Nuclear Research, Dubna, Moscow Oblast
eter (spectra) JRC Joint Research Centre (of European Commission)
ICP-QMS Inductively coupled plasma quadrupole mass K particle kinetic energy
spectrometry KD, K, K0 Kaons or K mesons
ICP-SFMS Double-focusing sector field inductively coupled K Degrees Kelvin
plasma mass spectrometry ka Kiloannum (103 years)
ICRP International Commission on Radiological Protection KamLAND Kamioka Liquid Scintillator Anti-Neutrino Detector,
ICRU International Commission on Radiation Units and Japan
Measurements KATRIN Karlsruhe TRItium Neutrino experiment
ID or i.d. Inner diameter, inner detector kBq Kilobecquerels (103 Bq)
IDA Isotope dilution analysis KCFC Potassium cobalt ferrocyanide
IDMS Isotope dilution mass spectrometry kcps Kilocounts per second
ID-TIMS Isotope dilution thermal ionization mass spectrometry KCRV Key comparison reference value
IE Ion exchange KEK The High Energy Accelerator Research Organization, Japan
IEC International Electrotechnical Commission, inertial electrostatic keV Kiloelectron volts (103 eV)
confinement kg Kilograms
IECF Inertial electrostatic confinement fusion kGy Kilogray
IEEE Institute of Electrical and Electronics Engineers kHz Kilohertz
IEF Isoelectric focusing gel electrophoresis km.w.e km-water-equivalent
IFIN-HH Horia Hulubei National Institute of Physics and Nuclear KNN k nearest neighbor algorithm
Engineering, Romania KRISS National Metrology Institute of Korea
IGPC Internal gas proportional counting KSTAR Korea Superconducting Tokamak Advanced Research
IL-5 Interleukin-5 fusion reactor
IMS International Monitoring System of the CTBT kt Kilotons
in. Inch ¼ 2.54 cm ¼ 25.4 mm kV Kilovolts (103 V)
INES International Nuclear and Radiological Event Scale kW Kilowatts (103 W)
INFN Instituto Nazionale di Fisica Nucleare (Italy) ky Kiloyears (103 y)
xl Acronyms, Abbreviations, and Symbols

L, l Liters LS Liquid scintillation, liquid scintillator, “linear-to-square” curve


LA Linear anode LSA Liquid scintillation analysis (analyzer)
LAAPD Large area avalanche photodiode LSC Liquid scintillation counting (counter)
LAB Linear alkyl benzene, dodecylbenzene LSO Cerium-activated lutetium oxyorthosilicate (Ce:Lu2SiO5)
LA-ICP-MS Laser ablation inductively coupled plasma mass LSS Liquid scintillation spectrometer
spectrometry LTC Live-time correction
LA-MC-ICP-MS Laser ablation multiple collector ICP-MS LuAP Cerium-activated lutetium aluminum perovskite (Ce:LuAlO3)
l Wavelength, decay constant, microliter (106 L), free parameter LY Light yield
lnr Nonrelativistic wavelength LXe Liquid xenon
lr Relativistic wavelength M Molar (solution concentration)
LAMMA Laser microprobe mass analysis m Particle mass
LAN Local area network m0 Particle rest mass
LANL Los Alamos National Laboratory mr Speed-dependent particle mass
LAr Liquid argon m Mass, meters, minutes
LARA laser-assisted isotope ratio analysis mA Milliampere (103 ampere)
LAW Low-activity waste Ma Megayear (106 years)
LBD Ligand-binding domain mAbs Monoclonal antibodies
LBNL Lawrence Berkeley National Laboratory MACS Magnetically assisted chemical separations
LC Liquid chromatography MALDI Matrix-assisted laser desorption/ionization
LCDW Lower circumpolar deep water MAPD Micropixel avalanche photodiode
LCMS Liquid chromatography mass spectrometry MAPMT Multianode photomultiplier tube
LD50 Median lethal dose MARG Microautoradiography
LED Light-emitting diode MARIS Marine information system
LEGE Low-energy germanium detector MARSSIM Multi-Agency Radiation Survey and Site Investigation
LENA Low-energy neutrino astrophysics detector Manual
LET Linear energy transfer MATLAB MATrix LABoratory (numerical computing and pro-
LEU Low enriched uranium gramming language)
LHCb RICH Large Hadron Collider beauty experiment detector at mb Millibarn (103 b)
CERN mBq Millibecquerels (103 Bq)
LHD Large Hadron Collider MBq Megabecquerels (106 Bq)
LiI(Eu) Europium-activated lithium iodide mCi Millicurie (103 Ci) ¼ 2.22  109 dpm ¼ 3.7  107 dps ¼ 37
LIMS Laboratory Information Management System MBq
LINAC or linac Linear accelerator MC Multiple ion counting
LIST Laser ion source trap MCA Multichannel analyzer
LL Lower level MCF Moving curve fitting
LL-BSS Large 6LiI(Eu) Bonner sphere spectrometer MC-ICP-MS Multiple ion collector-ICP-MS
LLC Liquid (mobile)eliquid (on solid phase) chromatography MCN Microconcentric nebulizer
LLCM Low-level count mode MCNP Monte Carlo N-Particle code
LLD Lower limit of detection, lower level discriminator MCNP-CP Monte Carlo N-Particle-Correlated Particle code
LLE Liquideliquid extraction MCP Microchannel plate
LLNL Lawrence Livermore National Laboratory MCP-PM Microchannel plate photomultiplier
LLR Long-lived radionuclide MC-TIMS Multiple collector thermal ionization mass spectrometry
LMD Laser microdissection MD Molecular dynamics
LM-OSL Linear modulation optically stimulated luminescence MDA Minimal detectable activity
LN2 Liquid nitrogen MDOA Methyldiooctylamine
LNE Laboratoire National de Métrologie et de E’ssais, France METAS Federal Institute of Metrology, Berne-Wabern,
LNGS Laboratori Nazionali del Gran Sasso, Italy Switzerland
LNHB Laboratoire National Henri Becquerel, Saclay METEPC Multielement tissue-equivalent proportional counter
LNMRI National Metrology Laboratory of Ionizing Radiation, MeV Megaelectron volts
Brazil MeVee Electron equivalent energy
LOD Limit of detection MHSP Microhole and strip plate (imager)
LOV lab-on-valve (system) MHz Megahertz (106 Hz)
lp Line pairs MIBK Methyl isobutyl ketone
LPB Low-pressure Bridgman MICAD Microchannel Array Detector
LPI low-pressure cascade impactor MICM Modified integral counting method
LPRI Laboratoire Primaire des Ionizants, Paris MICROMEGAS Micromesh gas detector
LPS Lipopolysaccharide mg Milligram (103 g)
LRAD Long-range alpha detector mGy Milligray
Acronyms, Abbreviations, and Symbols xli

MIBK Methyl isobutyl ketone n Neutron


min Minutes n Index of refraction
mK MilliKelvin (103 K) NA Avogadro’s constant (6.022  1023/mol)
mL, ml Milliliter (103 L) nA Nanoampere (109 A)
MLR Multiple linear regression NAA Neutron activation analysis
mM Millimolar (103 M) NAC N-acetylcystein
mm Millimeter (103 m) NADW North Atlantic Deep Water
MM Magnetic monopoles NaI(Tl) Thallium-activated sodium iodide
MMAD Mass median aerodynamic diameter NARC Neutrino Array Radio Calibration
MMC Metallic magnetic calorimeter NASA National Aeronautics and Space Administration, Washing-
mmol Millimole (103 mol) ton, D.C.
MNP Magnetic nanoparticle NBL New Brunswick Laboratory of the US DOE
mol Mole (gram-molecular weight) NBR Natural background rejection
MU Megaohm (106 U) NBS National Bureau of Standards (now NIST)
MOX Mixed oxide fuel NC Neutral current (interaction)
MP Multipurpose NCD Neutral current detector
M-P Mandel and Paule mean nCi Nanocurie (109 Ci)
MPa Megapascal (106 Pa) NCM Normal count mode
MPGD Micropattern gas detector NCRP National Council on Radiation Protection and
MPPC Multipixel photon counter Measurements
mrad Millirad (1 mrad ¼ 10 mGy) NDA Nondestructive analysis
MRI Magnetic resonance imaging NEA Nuclear Energy Agency of the OECD
mRNA Messenger RNA Ne/h Number of electronhole pairs
MS Mass spectrometry NEMO Nautic Environment Marine Observatoire
ms, msec Milliseconds (103 s) NE-OBT Nonexchangeable organically bound tritium
MSAP Microscale sample automation platform NF-LA-ICP-MS Near-field laser ablation inductively coupled
MSB Methylstyrylbenzene plasma mass spectrometry
MSC Microplate scintillation counting ng Nanograms (109 g)
MSD Mean standard deviation NHMRC National Health and Medical Research Council, Australia
MSE Multisite events NIDW North Indian Deep Water
MSGC Microstrip gas counter NIM Nuclear instrument module
MSI Mass spectrometry imaging NIMH Nickel metal hydride
MS/MS Tandem mass spectrometry NIST National Institute of Standards and Technology, Gaithersburg
mSv Millisievert nm Nanometer (109 m)
MW Megawatt (106 W) NMI National Metrology Institute
Mt Megaton (106 t) NMM Neutron moisture meter
MTO Magnetooptical trap NMR Nuclear magnetic resonance
mD, mL Muons NNDC National Nuclear Data Center
m Attenuation coefficient NOI Nuclide of interest
mA Microampere (106 A) NORM Naturally occurring radioactive materials
mCi Microcurie (106 Ci) ¼ 2.22  106 dpm ¼ 3.7  104 NP Nanoparticle
dps ¼ 37 kBq NPD 2-(1-Naphthyl)-5-phenyl-1,3,4-oxadiazole
mg Microgram (106 g) NPE Nonyl phenol ethoxylate
mL Microliter (106 L) NPL National Physical Laboratory, UK
mm Micrometer (106 m) NPO 2-(1-Naphthyl)-5-phenyloxazole
mPIC Micropixel gas chamber NPP Nuclear power plant
ms, msec Microseconds (106 s) NRC United States Nuclear Regulatory Commission
m-XANES Microfocused X-ray absorption near edge structure n Neutrino, photon frequency, particle velocity
m-XRF Microfocused X-ray fluorescence n Antineutrino
MEK Methyl ethyl ketone 0nbb Neutrinoless double-beta decay
MW Megawatt (106 W) 2nbb Two-neutrino double-beta decay
MWe Megawatt electrical nM Nanomolar (109 M)
m.w.e. Meter water equivalent nm Nanometer (109 m)
MWPC Multiwire proportional chamber NMM Neutron moisture meter
MV Megavolts (106 V) NMR Nuclear magnetic resonance
MVC Multivariate calibration NNDC National Nuclear Data Center, BNL, Upton, New York
N Newton ¼ 1 kg m/s2 NNFL National nuclear forensics library
N Neutron number NORM Naturally occurring radioactive material
xlii Acronyms, Abbreviations, and Symbols

NPT Nonproliferation Treaty pF Picofarad (1012 F)


NRC Nuclear Regulatory Commission PF Polar front
ns, nsec Nanosecond (109 s) PFA Perfluoroalkoxy
NSTAR Neutron sandwich transmitter/activation-g radiator PFZ Polar frontal zone
NT200 Neutrino telescope, Lake Baikal, Siberia pg Picogram (1012 g)
NTD-Ge Neutron transmutation-doped Ge PGA Pulse gradient analysis
N-TIMS Negative ion thermal ionization mass spectrometry ph Photons
NTP Normal temperature and pressure PHA Pulse height analysis
NTS Nevada test site PHITS Particle and heavy ion transport code system
NU Natural uranium PHOSWICH PHOSphor sandWICH (detector)
NUDAT Nuclear Database of the NNDC p Pi constant ¼ 3.14159
NWT Nuclear weapons test pD, pL, p0 Pions or pi mesons
N/Z Neutron/proton ratio PI Polyimide, pressurized injection
OC Organic carbon PID Particle identification
OD or o.d. Outer detector, outer diameter PIM Parallel ionization multiplier
OECD Organization for Economic Cooperation and Development PIMS Positive-ion mass spectrometry
OES Optical emission spectrometry PIPS, PIPSi Passivated implanted planar silicon
OFHC Oxygen-free high thermal conductivity PIXE Proton-induced X-ray emission
OGE Optogalvanic effect PKC Protein kinase C
OHM National Office of Measurement, Budapest PLC Proportional long counter
OLLSC Online liquid scintillation counting PLI Pulse length index
OM Optical module PLS Partial least squares
OSL Optically stimulated luminescence PLS-DA Partial least squares discriminant analysis
OTPC Optical time projection chamber PLSR Partial least squares regression
P Parity quantum number PM Photomultiplier, particulate matter
p Particle momentum PMM Power-moderated weighted mean
p, pD Proton PMBP 1-Phenyl-3-methyl-4-benzoylpyrazolone-5
Pa Pascal ¼ 1 N/m2 ¼ 1 kg/m,s2 pMC Percent modern carbon
PAC Pulse amplitude comparison (comparator) PMMA Polymethylmethacrylate
PADC Polyallyldiglycol carbonate PMP 1-Phenyl-3-mesityl-2-pyrazoline
PAGE Polyacrylamide gel electrophoresis PMT Photomultiplier tube
PAN Polyacrylonitrile PN Pneumatic nebulizers
PANDA Particles and nondestructive analysis PNNL Pacific Northwest National Laboratory
PAW Physics Analysis Workstation PNX Pacific Northwest eXtraction system
PAZ Partial annealing zone POM Polyoxymethylene
PBBO 2-(40 -Biphenylyl)-6-phenylbenzoxazole POPOP 1,4-Bis-2-(5-phenyloxazolyl)benzene
PBD 2-Phenyl-5-(4-biphenylyl)-1,3,4-oxadiazole PPAC Parallel plate avalanche chamber
PBO 2-(4-Biphenylyl)-5-phenyloxazole ppb Parts per billion
PBq Petabecquerel (1015 Bq) PPC P-type point contact
PBS Phosphate buffered saline PPD 2,5-Diphenyl-1,3,4-oxadiazole
PC Proportional counter(ing), personal computer, paper chromato- PPE Personal protective equipment
gram, polycarbonate ppm Parts per million
PCA Principal component analysis ppmw Parts per million by weight
PCB Polychlorinated biphenyl PPO 2,5-Diphenyloxazole
pCi Picocurie (1012 Ci) PS Plastic scintillator, polystyrene
PCR Principle component regression ps Picosecond (1012 s)
PD Photodiode PSA Pulse shape analysis
PDA Pulse decay analysis PSD Pulse shape discrimination
PDB Pee Dee Belemnite (standard) PSf Plastic scintillator foils
PDD Pulse decay discriminator psi 6.895  103 Pa ¼ 68.95  103 bar ¼ 51.715 torr
PE Phosphate ester, polyethylene PSL Photostimulable light (or luminescence)
PEC Power and event controller PSm Plastic scintillator microspheres
PENELOPE PENetration and Energy Loss of Positrons and Elec- PSPC Position-sensitive proportional counter
trons Monte Carlo code PSr Plastic scintillator resins
PERALS Photon Electron Rejecting Alpha Liquid Scintillation PSUP Photomultiplier SUPport structure
PET Positron emission tomography, polyethylene terephthalate P/T Peak-to-total ratio
PETAC Pentaerythritol tetrakis allyl carbonate PTB Physikalisch-Technische Bundesanstalt, Braunschweig
PeV Petaelectron volts (1015 eV) PTBT Partial Test-Ban Treaty
Acronyms, Abbreviations, and Symbols xliii

PTFE Polytetrafluoroethylene RSF Relative sensitivity factor


P-TIMS Positive ion thermal ionization mass spectrometry RST Reverse spectral transform
PTP p-Terphenyl s Seconds
PUR Pileup rejector SAF Subantarcticfront
PUREX Plutonium URanium EXtraction SAH S-adenosyl-homocysteine
PVC Polyvinyl chloride SalSa Salt sensor array
PVD Physical vapor deposition SAM Standard analysis method, S-adenosyl-methionine
PVDF Polyvinyldifluoride SAMAD Surface area mean aerodynamic diameter
PVT Polyvinyl toluene SAS Semiconductor a-spectrometry
PWR Pressurized water reactor SBD Surface barrier detector
PXE Phenyl-ortho-xylylethane SCA Single channel analyzer
Q Q value of nuclear reactions SCC Software coincidence counting, squamous cell carcinoma
QA Quality assurance SCI Science Citation Index
QC Quality control SCR Sample channels ratio, solar cosmic rays
QC-CPM Quench-corrected count rate SCX Strong cation exchange
QCD Quantum chromodynamics SD Standard deviation
QD Quadrupole SDCC Simplified digital charge comparison
QDC Charge-to-digital converter SDD Silicon drift detector
QE Quantum efficiency SDP Silicon drift photodiode
QIP Quench-indicating parameter SDT Shared dead time
QWBA Quantitative whole-body autoradiography SE Single escape, secondary electron
R Roentgen (1R ¼ 2.58  104 C/kg) sec Seconds
RAC Radon activity concentration SEC Size exclusion chromatography
rad Radiation-absorbed dose (1 rad ¼ 10 mGy ¼ 100 erg/g) SEGe Standard electrode coaxial Ge detector
RAD Radon-in-air monitor SEM Scanning electron microscopy
RAST Radioallergosorbent test SF Spontaneous fission
RBE Relative biological effectiveness SFC Supercritical fluid extraction
RDC Remote detector chamber SFD Scintillation fiber detector
RDD Radiological dispersal device (“dirty bomb”) SF-ICP-MS Sector fieldeinductively coupled plasma mass
RE Recovery efficiency spectrometry
REE Rare earth elements SFU Stacked filter unit
REFIT Radialelectron fluence around ion tracks SGD Submarine groundwater discharge
REGe Reverse-electrode coaxial Ge detector SHE Superheavy elements
REL Restricted energy loss SHOTS Southern Hemisphere Oceans Tracer Studies
rem Roentgen equivalent mammal (1 rem ¼ 10 mSv) SHRIMP Sensitive high mass resolution ion microprobe
RF Radiofrequency SI International System of Units, sequential injection, spray
RF Feedback resister ionization
RFQ Radiofrequency quadruple SIA Sequential injection analysis
RH Relative humidity SIE Spectral index of the external standard
r Density (g cm3), neutron absorption cross section, resistivity s Reaction cross section, thermal neutron cross section
RIA Radioimmunoassay Si(Li) Lithium-compensated silicon
RICE Radio Ice Cherenkov Experiment SIMS Secondary ionization mass spectrometry
RICH Ring imaging Cherenkov (counters/detectors) Si PIN Silicon p-i-n diode
RIMS Resonance ionization mass spectrometry SiPM Silicon photomultiplier
RIS Resonant ionization SIR International Reference System (Système Internationale de
RM Reference material Référence)
RMS Rosette multibottle samplers SI-RSC Sequential injection renewable separation column
RMT Radiometric technique SIS Spectral index of the sample
RNA Ribonucleic acid SJD Silicon junction detector
Ro5 Ring of Five (European radionuclide monitoring labs) SLAC Stanford Linear Accelerator Center
ROI Region of interest (spectral) SLIM System for Laboratory Information Management
ROSEBUD The Rare Objects Search with Bolometers Under- SLM Standard laboratory module
grounD collaboration SLSD Scintillator-Lucite sandwich detector
ROV Remotely operating vehicle SMAD Surface median aerodynamic diameter
RPC Resistive plate chamber SMDA Specific minimum detectable activity
RPH Relative pulse height S/N Signal-to-noise
RSC Renewable separation column, relative sensitivity coefficient SNAP Systems Nuclear Auxiliary Power
RSD Relative standard deviation SNICS Source of Negative Ions by Cesium Sputtering
xliv Acronyms, Abbreviations, and Symbols

SNF Spent nuclear fuel TDCR Triple-to-double coincidence ratio (method)


SNM Special nuclear material TDS Total dissolved solids
SNMS Secondary neutral mass spectrometry TEA Triethylamine
SNO Sudbury Neutrino Observatory, Canada TEM Transmission electron microscopy
SNR Signal-to-noise ratio TENORM Technologically enhanced naturally occurring radioac-
SNS Spallation neutron source tive materials
SNTS Semipalatinsk nuclear test site, Eastern Kazakhstan TEPC Tissue-equivalent proportional counter
SOA Secondary organic aerosol TES Transition edge sensor
SOI Silicon-on-insulator TBAB Tetrabutylammonium bromide
SOP Standard operating procedure TeV Teraelectron volts (1012 eV)
SPA Scintillation proximity assay Tf Transfer factor (radionuclide)
SPC Single photon counting TFTR Tokamak fusion test reactor
SPD Self-powered detector TFWT Tissue-free water tritium
SPE Single photon event, solid phase extraction, solid polymer THGEM Thick gas electron multiplier
electrolyte THM Traveling heater method
SPECT Single photon emission computed tomography tHM yL1 Metric tons of heavy metal per year
SPME Solid phase microextraction TI Transfer instrument
SQM Strange quark matter w Approximately
SQP(E) Spectral quench parameter of the external standard TIMS Thermal ionization mass spectrometry
SQP(I) Spectral quench parameter of the isotope TINCLE Track-in-cleavage (technique)
SQS Self-quenched streamer TINT Track-in-track (technique)
SQUID Superconducting quantum interference device TIOA Triisooctylamine
SR Superresolution, synchrotron radiation TL Thermoluminescence
sr Steradian TLA Trilaurylamine
SRAM Static random access memory TLC Thin-layer chromatography (chromatogram)
SRM Standard reference material TLD Thermoluminescence dosimeter
SRS Savannah River Site TMA Trimethylamine
SSB Silicon surface barrier detector TMI Three Mile Island
SSDD Segmented silicon drift detector TMOS Tetramethoxysilane
SSE Single site events TMS Tetramethylsilane
SSM Standard service module, selective scintillating microsphere TNOA Tri-n-octylamine
SSNTD Solid-state nuclear track detector TNSA Target normal sheath acceleration
ST Supersensitive TNT Trinitrotoluene
STD Shared dead time concept TOA Top of the atmosphere, trioctyl amine
STE Self-trapped excitation TOF Time-of-flight
STF Subtropical front TOP Time-of-propagation
STM Scanning tunneling microscope TOPO Trioctylphosphine oxide
STNTD Solid-state nuclear track detection (detectors) torr 133.3224 Pa
STP Standard temperature and pressure TP p-Terphenyl
STS Semipalatinsk test site TPPS Triphenylphosphine sulfide
STUK Radiation and Nuclear Safety Authority, Finland TR Tritium sensitive
Sv Sievert (1 Sv ¼ 1 Gy ¼ 100 rem ¼ 1 J/kg) TRACOS Automatic system for nuclear track evaluations
SVOC Semivolatile organic carbon TRE 12-O-Tetradecanoyl phorbol-13-acetate responsive element
t Ton(s) TRI Toxic release inventory
t½, T½ Half-life TR-LSC Time-resolved liquid scintillation counting
T Particle kinetic energy TR-PDA Time-resolved pulse decay analysis
T Tritium, tesla ¼ 1 V s/m2 TRPO Trialkyl phosphine oxide
TAEK Turkish Atomic Energy Authority TSC Task sequence controller
TALSPEAK Trivalent ActinideeLanthanide Separation by Phos- TSCA Toxic Substance Control Act
phorus Extractants and Aqueous Komplexants process TSEE Thermally stimulated exoelectron emission
TAR Tissueeair ratio tSIE Transformed spectral index of the external standard
TAT Targeted alpha therapy tSIS Transformed spectral index of the sample
TBP Tributyl phosphate TSP Total suspended particle
TBq Terabecquerel (1012 Bq) TTA Tenoyl-tri-fluoro acetone
TC Total carbon TTL Transistoretransistor logic
TCA Trichloroacetic acid TU Tritium unit (0.119 Bq 3H kg1 H2O or 7.14 DPM of 3H L1
TCS True coincidence summing H2O or ratio of 1 atom 3H:1018 atoms of 1H)
TD Time discriminator
Acronyms, Abbreviations, and Symbols xlv

u Atomic mass unit (1/12 mass of 12C ¼ 1.66054  1027 kg), up WBA Whole-body autoradiography
quark WBEC Weak base extraction chromatography
u Antiup quark WCVB Waste concentration vapor body
u Particle speed WDS Wavelength dispersive spectrometer
unr Nonrelativistic particle speed WDX Wavelength dispersive X-ray (analyzer)
ur Relativistic particle speed WHO World Health Organization
UCN Ultracold neutrons WIMP Weakly interacting massive particle
UHE Ultrahigh energy WIPP Waste Isolation Power Plant
UL Upper level WM Weighted mean
ULB Ultralow background WMO World Meteorological Organization, Geneva
ULD Upper level discriminator WNO World Nuclear Organization, London
ULEGE Ultralow-energy Ge WOCE World Ocean Circulation Experiment
UNSCEAR UN Scientific Committee on the Effects of Nuclear WOMARS Worldwide Marine Radioactivity Studies
Radiation WRA Warfare radioactive agent
UOC Uranium ore concentrate WSF Wavelength shifting fiber
U.S.A.E.C. US Atomic Energy Commission (now NRC) WSOC Water-soluble organic carbon
U.S. DOE US Department of Energy wt% Weight percent
USEPA US Environmental Protection Agency XAF X-ray absorption spectroscopy
USN Ultrasonic nebulizers XANES X-ray absorption near edge structure
UV Ultraviolet XRD X-ray diffraction
V Volts XRF X-ray fluorescence
V0 Step voltage XtRA Extended range
VAX Digital Equipment Corporation trade name y Years
VCCI Variable configuration cascade impactor YAG:Yb Yb-doped Y3Al5O12
VHPLC Very-high-pressure liquid chromatography YAP:Ce Cerium-activated yttrium aluminum perovskite
VMEbus Versa Module Europa bus (Ce:YAlO3)
VSiPMT Vacuum silicon photomultiplier tube YG Yttrium glass
VUV Vacuum ultraviolet (spectral region) YSi(Ce) Cerium-activated yttrium silicate
VYNS Vinyl acetate and vinyl chloride copolymer Z Atomic number
W Watt (1 W ¼ 1 J/s) Z2 Average atomic number
w/w Weight/weight Zef or Zeff Effective atomic number
WAK Wiederaufarbeitungsanlage (nucleal fuel reprocessing plant), ZCH Central Analytical Laboratory, Jülich
Karlruhe ZnS(Ag) Silver-activated zinc sulfide
Chapter 1

Environmental radioactivity monitoring


Rudolf Engelbrecht
Radiochemistry, Seibersdorf Labor GmbH, Seibersdorf, Austria; Currently - Austrian Agency for Health and Food Security, GmbH, Vienna

Chapter outline
I. Introduction: objective of environmental monitoring 1 1. Wastewater 23
II. Types of monitoring programs 2 2. Rain 23
A. Routine monitoring 2 3. Groundwater 23
B. Emergency preparedness 3 4. Surface water 24
C. Emergency monitoring 3 5. Drinking water 24
III. Fundamentals of environmental monitoring 4 D. Foodstuff 24
A. Design of environmental monitoring programs 4 1. Milk 24
B. Sampling strategies 7 2. Meat and fish 25
C. Sample preparation 9 3. Vegetables, fruits, and cereals 26
D. Measurement and quantification 10 4. Mixed diet 26
E. Quality assurance/quality control 12 V. Monitoring for external exposure 26
IV. Monitoring for internal exposure 14 A. Dose rate monitoring 26
A. Air 14 B. Dose monitoring 27
1. Aerosols 14 VI. Mobile monitoring 27
2. Online versus offline systems 14 A. Aerial measurements 27
3. Gaseous effluents 15 B. Mobile laboratories 28
B. Soil, sediments, vegetation, and deposits 17 References 32
1. Laboratory based 17 Further reading 40
2. In situ gamma spectroscopy 19 Rudolf Engelbrecht 40
C. Water 20

I. Introduction: objective of water, agricultural products, and natural foodstuffs, as well


as in bioindicators that concentrate radionuclides and pro-
environmental monitoring vide a measure of trends in activity levels.
As recent history (e.g., IAEA, 2011; UNSCEAR, 2014; Thus, environmental monitoring can be described as the
IAEA, 2015; IRSN, 2018) has shown to scientists and the exposition scenarioebased systematic sampling and anal-
public, transparent and comprehensible dose assessments, ysis of air, water, soil, and biota to assess environmental
including estimation of doses as closely as possible to those conditions. The objective of such monitoring is to obtain
actually received, are a fundamental basis of managing solid information that will serve as the basis for measures
radiation protection. The most realistic assessment of doses and political decisions. Environmental monitoring assess-
is obtained by using measured activity concentrations in ments can involve establishing baseline quality, uncovering
environmental media and measurements of external dose environmental trends, identifying any variations, detecting
rates. Environmental monitoring provides data that permit new environmental issues, and determining the progress
the analysis and evaluation of radiation fields and radio- made to achieve environmental goals.
nuclide activity concentrations in environmental samples It is important to distinguish the specific aspects of
relevant to human exposure, primarily in air, drinking environmental monitoring data obtained under normal

Handbook of Radioactivity Analysis: Volume 2. https://doi.org/10.1016/B978-0-12-814395-7.00001-5 1


Copyright © 2020 Elsevier Inc. All rights reserved.
2 Handbook of Radioactivity Analysis: Volume 2

operating conditions from those obtained under emergency Once a monitoring program has been implemented, it
conditions since the criteria for evaluation are completely should be reviewed periodically to ensure that it continually
different. Under normal operating conditions, data are often fulfills the objectives.
important for the statutory control of releases, but the levels The purpose of routine environmental monitoring of
set are to be related to human tissue doses. In case of a airborne radioactivity is to monitor domestic and foreign
possible accidental release of radioactivity, the monitoring facilities. Sampling of soils, sediments, or deposits serves
program aims at answering questions, such as Has an as an indicator of long-term buildup of radioactivity in the
abnormal release occurred? Is there action to be taken? and environment. Measurement of ingredients in foodstuff and
Which remedial measures should be brought about? Thus, water is intended to complete the monitoring program for
distinction can be made between the following different the migration of radionuclides in the food chain or to check
situations: the contamination of the public at large by ingestion.
Monitoring locations for ground- and surface water, sedi-
Routine monitoringeemergency preparednesse
ment, biota, and foodstuffs are related to the potential
emergency monitoring.
migration pathways determined by preoperational studies,
For each of these situations, the type of monitoring and the frequencies of sampling and measurements are
program to be established is influenced by the source of specified with a view to the timely detection of significant
radioactivity as well as the scale of the spatial and temporal changes in the release rates and concentrations of radio-
boundaries of the environment to be monitored. In the end, nuclides and the associated levels of human exposure in
the goal of monitoring the environment always is to obtain accordance with the monitoring objectives.
a profound set of data that will serve as a basis that enables It has to be noted that radon monitoring, which forms
authorities to implement measures for either preserving the main exposure to radioactive sources to members of the
environmental values or preventing their deterioration. public (UNSCEAR, 2000b), is not implemented in envi-
ronmental monitoring programs but conducted in special
radon survey programs (e.g., Friedmann et al., 2007).
II. Types of monitoring programs Recent attention has been paid to radiation risk to the
A. Routine monitoring people and the environment caused by exposure to ionizing
radiation originating from naturally occurring radioactive
Routine monitoring programs aim at providing information
materials (NORMs). NORMs touch many aspects of life,
on the overall dose received by the population at large. The
starting with occupational risk, through some “contami-
setup of the monitoring is the result of an optimization
nated” goods, leisure activities including spa visits and
process in which the availability of measurement resources,
ending with a huge amount of bulk waste often dumped in
the relative importance of different exposure pathways, and
our vicinity (Kathren, 1998; IAEA, 2003). Such alterations
the levels of activity and dose in relation to the regulatory
to the natural state result in an increment of radiation risk to
constraints are taken into consideration. Routine environ- the people as well as to nonhuman biota. Each particular
mental radiation monitoring programs are designed spe-
type of NORM determines a unique scenario of exposure
cifically for each facility, taking into account site-specific
usually differing from those caused by the artificial radio-
factors, such as climate, site location, the design of the
nuclides (Martin et al., 1997).
facility and its barriers, geological and geomorphological
The measurements must be adequate to determine ra-
conditions, the off-site environment, and the population
diation levels and trends of environmental radioactivity at
distribution (IAEA, 2004); these programs are conducted
levels just detectable, the parameters needed for subsequent
both on and outside the site giving rise to potential expo-
dose assessment, and compliance with national or interna-
sure of the public to radionuclides in the environment. tional standards, constraints, or limits laid down for the
The life cycle of the routine programs for environmental
protection of the population. These limits and constraints
monitoring comprises preoperational studies, performed to
have values that are typically less than exposure due to
establish “baseline” environmental radiation levels and
natural background radiation. It is, thus, necessary to be
activity concentrations for the purpose of subsequently
able to identify the source and to circumscribe the extent of
determining the impacts of the source, monitoring during
the radioactive material with reasonable accuracy.
the operational phase, and decommissioning or post-
The objectives of routine monitoring programs are to
operation monitoring, performed as long as the facility re-
mains a potential source of radionuclides that could be l provide information to assess the adequacy of protec-
released to the environment. The complexity of the pro- tion of the public,
gram depends on the identities, quantities, and chemical l meet requirements of regulatory agencies,
and physical forms of radionuclides that may be released l verify radionuclide containment and/or waste manage-
and on the characteristics of the monitored environment. ment practices,
Environmental radioactivity monitoring Chapter | 1 3

l meet legal liability obligations, and l Early government and public information
l provide public assurance. l Planning of urgent population protection
countermeasures
B. Emergency preparedness l Planning of agricultural countermeasures and food
restrictions
Environmental monitoring may be conducted continuously
to serve as a detection system. Emergency preparedness
C. Emergency monitoring
monitoring is part of a strategy for data and information
acquisition. The overall emergency strategy includes two Under emergency conditions, environmental monitoring is
different modes of information, namely, (1) acquisition, as the most informative source of data. The measurements of
there are physical measurements of relevant data on one the radiation levels or the levels of radioactive contamina-
hand and (2) modeling of situations as a tool for interpo- tion are required for rapid assessments of the situation to
lation and extrapolation in time and space where mea- inform those responsible for controlling the emergency so
surement data are sparse on the other hand. It is usually that countermeasures can be put in hand as a matter of
more satisfactory to make provision for detecting an urgency. Monitoring in emergency situations is also a
emergency at its source, but detection by environmental valuable and fundamental tool to verify the effectiveness of
monitoring may be required in some situations, for the actions taken, for example, evacuation, closing the
example, near frontiers. In a nuclear accident, the prompt areas, use of stable iodine tablets, or banning the con-
monitoring of a large area may be needed. For this reason, sumption of foodstuffs or water from defined areas.
automatic measuring stations that will continuously mea- History has shown that the requirements for the emer-
sure the dose rate in the environment installed around major gency monitoring program and the nature of relevant data
facilities are capable of early monitoring. Continuously will evolve with time. The procedures used in emergency
operated off-site systems have the advantage that they can monitoring can conveniently be grouped into three phases,
provide rapid indication, not only that a release to the namely, detection, initial survey, and subsequent surveys.
environment has taken place but also of the direction in In the initial emergency response following an accident,
which the released material is moving. Off-site systems do where information is required with as little delay as
have the disadvantage that the detectors need to be possible, rapid and relatively simple, albeit crude, analytical
considerably more sensitive than if sited near to the methods may be preferred. This usually means a lesser
possible point of release and also need to be extremely sensitivity and thus a greater risk for errors. However, in
reliable if duplication is to be avoided. any emergency situation, it is important that the results can
All of these systems may include such devices as contin- be obtained relatively quickly. Under most conditions, this
uous air samplers capable of measuring concentrations of would amount to the use of dose rate and survey
airborne particles, gaseous iodine, and any other radionuclides instruments.
of particular concern or water samplers for continuously Nevertheless, it should be ensured that the types of in-
scanning the sky or bodies of water for radiation. If a facility struments available are suitable for the measurement pur-
may contain large amounts of tritium, some special device to poses. For example, if the released material consists of only
measure tritium may well be installed. In each case, the tritium or plutonium, then the typical betaegamma survey
readings being telemetered back to a control center. instruments are not of much use and appropriate special
Systems intended to detect airborne releases by the use instruments and/or monitoring techniques should be used.
of air samplers introduce complex techniques, if early At the early stage of an accidental atmospheric release,
warning is required, because of the presence of the natural external exposure includes the contribution of radiation
decay products of radon and thoron. However, if time can from the plume. Thus, initial surveys in the release phase of
be allowed for these to decay, a simple measurement of the accident will be focused on measurements of cloud
gross alpha- or gross beta-activity will indicate whether shine and on the sampling of radionuclides from the plume
conditions are seriously abnormal, although it must always to assess doses from external exposure and inhalation. In
be remembered that gross activity results cannot be inter- the postrelease phase, external gamma dose rate measure-
preted in terms of hazard to man. The intended use of the ments are attributable mainly to radiation from deposits on
resultant information gives guidance to the choice of the ground. Close to the installation, these measurements
monitoring priorities of such networks. may also include the contribution of radiation from the
The objectives of emergency preparedness monitoring source.
are as follows: The external dose rate measurements should be sup-
plemented as soon as possible by nuclide-specific analysis
l Detecting any release
of representative samples of mobile environmental media
l Predicting plume trajectory
and biota through which radionuclides could migrate and
4 Handbook of Radioactivity Analysis: Volume 2

reach the human habitat and thereby enter the human body. measured? How will these parameters be monitored? Where,
These are atmospheric air, soil water and groundwater, when, and how frequently will the parameters be measured. A
surface water, sediments, biota, and foodstuffs. Ground- monitoring program will be as valuable and effective as the
water should be monitored through monitoring wells questions identified are specific and focused and can be used to
located at a sufficient depth around and downstream of the guide the development of a monitoring plan.
facility. These measurements may be pursued over longer To be consistent with the objectives and the design of
periods of time. However, the assessment of the impact of any monitoring program, one has to consider types and
short-lived nuclides such as iodine and ruthenium isotopes characteristics of critical radionuclides, modes of their
will be possible only if measurements are performed within release to the environment, including mechanisms for the
a few weeks after the accident. transfer of radionuclides through environmental media,
Once a release has ceased and deposition levels have dispersion and reconcentration mechanisms, and their sea-
stabilized, nuclide-specific deposition densities of all sonal variation, existing levels of radionuclides in the
gamma-emitting radionuclides can be acquired rapidly by environment and their variability, and exposure pathways
the use of in situ gamma spectrometry. Nevertheless, lab- that make the major contributions to individual doses,
oratory analysis of a large number of samples of soil, leading to requirements in terms of sampling, sample
plants, water, agricultural products, and natural foodstuffs treatment, measurement technique, and the lower limit of
will be necessary to supplement the data provided by the in detection or minimal detectable activity (IAEA, 2005).
situ measurements. Moreover, the nature of the environment, as the location of
During such subsequent surveys, it also will be neces- the facility in relation to population centers and their
sary to perform a large number of measurements in composition and densities, surface waters, oceans,
different media in view of an accurate a posteriori assess- geological, meteorological, hydrological, and other natural
ment of the radiological impact. Such an assessment fulfills conditions, which might influence the dispersal of released
the need for adequate information of the public and may radionuclides, has to be taken into account.
serve also further scientific investigations. A key feature in designing environmental monitoring pro-
The specific objectives of emergency radiation moni- grams is the identification of potentially critical radionuclides,
toring in the environment are to pathways, and groups or individuals potentially affected.
In the considerations of the limitation of dose to the
l provide accurate and timely data on the levels, extent,
general public from ionizing radiation, doses to individuals,
and duration of radiation and environmental contamina-
to critical groups, and to the general population are
tion with radionuclides,
distinguished. As early as 1965, the ICRP (1965) defined a
l provide detail of the physical and chemical characteris-
critical group as that “whose exposure is homogeneous and
tics of the hazard,
typical of that of the most highly exposed individuals in the
l assist in preventing and controlling the spread of
exposed population.” In 2006, the ICRP introduced the new
contamination,
concept of a representative person, defining it as “an indi-
l assist decision-makers on the implementation of urgent,
vidual receiving a dose that is representative of the more
intermediate-, and recovery-phase population protection
highly exposed individuals in the population” (ICRP,
countermeasures, agricultural countermeasures, and
2006). The term “representative person” describes an in-
food restrictions
dividual with characteristics that reflect those of the group
l provide information for the protection of emergency
that receives the highest doses from a particular source,
and recovery workers,
known as the representative person for the radionuclide in
l provide information for the public on the degree of the
question, and replaces the “average member of the critical
hazard,
group” defined in previous publications of the ICRP. In any
l provide information needed to identify any people for
case, critical groups or the representative person may be in
whom long-term medical screening is warranted,
the vicinity of the installation or at some distant location.
l confirm the efficiency of protective actions.
To assess the annual effective doses for both critical group
and representative person, methods recommended by the
III. Fundamentals of environmental International Atomic Energy Agency (IAEA, 1982; IAEA,
2001) can be used. A more conservative concept to assess
monitoring doses to the public is given in US Regulatory Guide 1.109
A. Design of environmental monitoring and based on the individual of maximum dose (US NRC,
programs 1977).
Routes from a source of radionuclides and/or radiation
Monitoring design provides answers to the following ques- to a target individual or a population through media in the
tions: What will be monitored? What are the parameters to be environment are defined in the exposure pathways.
Environmental radioactivity monitoring Chapter | 1 5

There are two main categories of exposure pathway: Under conditions of normal discharges and chronic (pro-
longed) exposure, the pathways are usually permanent and
l External exposure from radionuclides present in the air
well defined. In case of emergency releases, the contributions
or in material incorporated in, for example, soils or sedi-
via different pathways to the doses received by workers and
ment, determined by direct measurements of external
the public may be different from the normal and transient.
dose or by soil analysis.
These differences should be considered when establishing the
l Internal exposure from the inhalation, ingestion, or im-
monitoring program. To protect the public and workers from
mersion of radionuclides present in air or incorporated
deterministic health effects following major accidents, radio-
in water or foods, respectively. Immersion and inhala-
logical criteria in emergencies may be different from those
tion are monitored by air sampling. Ingestion of radio-
applied under conditions of normal discharges (e.g., additional
activity is monitored by means of food sampling, for
monitoring data may be necessary).
example, milk, fish, and shellfish, or indicator organ-
Under normal operation conditions, that is, for routine
isms or materials.
environmental monitoring, those radionuclides are to be
Generally, a range of potential pathways that may be considered, which are limited in discharge permits or are
more complicated in reality need to be considered significant components of a group limit (e.g., strontium-90
(Table 1.1). The relative importance of different exposure limited under any other beta/gamma-emitting radionuclide
pathways will be dependent upon group limit). Other radionuclides may be required as a result
of international obligations or backgrounds. Proven surro-
l the magnitude of the discharge,
gate radionuclides may be used (e.g., where the radionuclide
l the route of discharge and factors affecting it (e.g., stack
fingerprint is relatively stable). Since routine monitoring
height, meteorological conditions, etc.),
programs are designed to verify compliance with environ-
l the physical state or properties (e.g., emission type, en-
mental standards at levels just detectable and which are for
ergy, physical half-life, gas, liquid, or solid),
records only by low-level measurements, it is essential to be
l the chemical characteristics (e.g., organic or inorganic
able to identify the source and to circumscribe the extent of
form, oxidation state, speciation, etc.)
the radioactive material with reasonable accuracy.
l the dosimetric importance of radionuclides,
Preoperational assessments of the expected inventories of
l environmental characteristics (e.g., climate, type of
radionuclides during operation of a facility, the possible
biota, agricultural production, etc.); locations, ages, di-
discharge pathways and the likely amounts that will be
ets, and habits of the exposed individuals or
discharged to the environment, with due consideration of the
population.

TABLE 1.1 Important exposure pathways to be considered in the monitoring program.


External exposure pathways
Source of radiation / human Direct exposure from a source
Source of radionuclides/ atmosphere or water body / human Exposure due to the plume or water
Source of radionuclides / atmosphere or water body / hu- Skin contact exposure
man skin
Source of radionuclides / atmosphere or water body / soil or Exposure from deposited radionuclides on the ground, on the
sediment or building surface or vegetation / human shores of rivers, lakes, or the sea; on walls, roofs, and floors; or on
trees, bushes, and grass
Internal exposure pathways
Source of radionuclides / atmosphere / human Inhalation of radionuclides in the plume;
Source of radionuclides / water body / human Ingestion of radionuclides in drinking water
Source of radionuclides / atmosphere or water body / (soil Ingestion of radionuclides in food or beverages
or sediment) / vegetation / meat, milk, eggs, vegetables, or
marine food / human
Soil or sediment / human Inhalation of resuspended radionuclides
Source of tritium / atmosphere / human Absorption of tritium oxide through the skin
6 Handbook of Radioactivity Analysis: Volume 2

effluent treatment systems that will be installed, will help to Radionuclides of particular concern in freshwater and
define spatial and temporal boundaries and select types and marine food chains include 54Mn, 55Fe, 59Fe, 60Co, 65Zn,
95
numbers of samples and measurement methods. A preop- Zr, 95Nb, 103Ru, 106Ru, 110mAg, 125Sb, 131I, 134Cs, 137Cs,
141
erational program intended to establish baselines might also Ce, 144Ce, and some of the transuranic elements.
identify suitable indicator organisms or indicator materials Many other radionuclides would be present in debris from
for particular radionuclides. Indicators such as seaweeds, a nuclear accident; their potential contribution to human
lichen, or suspended particulate matter are selected not exposure depends on the type of accident and the circum-
because they represent a component of the human diet but stances at the time of the accident. Since there are several types
because they concentrate radionuclides and provide a mea- of fuel, the spectra of radionuclides that would be present in
sure of trends in activity levels and hence may provide more accidental releases could be somewhat different.
sensitive information of environmental contamination. The levels of radionuclides in the environment and food
Environmental monitoring during the decommissioning and their variability have been extensively compiled by the
of a facility, such as uranium mines and mills, uranium United Nations Scientific Committee on the Effects of
enrichment plants, fuel fabrication facilities, nuclear re- Atomic Radiation (UNSCEAR, 2000b, 2000c). These re-
actors (IAEA, 1998, 1999; 2001, 2002a, 2002b), nuclear ports contain information about the transfer of radionu-
fuel reprocessing plants, and other radionuclide processing clides between atmospheres, waters, soils, biota, and person
facilities, will be similar to that for the operational stage, and about human exposure to the various nuclides
modified to take account of changes in the source term, all (UNSCEAR, 2000a, 2008).
materials exhibiting significant levels of activity (FAO, What site or environment will be monitored, what will
1996) are removed as decommissioning proceeds. For both be measured, where will it be measured, and when and
current and historical discharges, in-growth of daughters how frequently will it be measured are essential elements
may need to be considered (e.g., 241Am from 241Pu). of a monitoring design. However, as the development of
The most important radionuclides to be assessed the monitoring design almost always requires clarification
following a release of radionuclides from a uranium-fueled and prioritization, documenting the design, including
reactor to the environment are 134Cs, 137Cs(137mBa), 131I, rationale for decisions, is critical when the design is
and other gamma emitters; the beta emitters 89Sr, 90Sr, and implemented and when the collected data are used for
tritium; and the alpha emitters 238Pu, (239 þ 240)Pu, 241Am, reporting to national policymakers, international forums,
and 242Cm. This group of radionuclides is most likely to be and the public.
of concern due to internal exposure from inhalation and Identification and assessment of the potentially critical
ingestion of food and water and to the contamination of radionuclides, pathways, and groups or individuals is a
environmental materials, which are part of the immediate substantial prerequisite in designing environmental moni-
pathways, leading to contamination of food (Table 1.2). toring programs, directly affecting the nature and extent of
Biological concentration in freshwater and marine systems the measurements. The selection of the major contributing
can result in very rapid transfer and enrichment of specific radionuclides and their significant pathways to the pre-
radionuclides. Radionuclides that enter such systems can, defined target population or individual direct the moni-
in certain cases, be rapidly accumulated by plankton and toring programs to the most important subjects. The
algae, which serve as food for higher trophic levels; thus, following principles for the development of a practical
the radionuclides become concentrated in organisms such monitoring program involve steps that are reasonably in-
as oysters, clams, shrimp, etc. dependent of local circumstances:

TABLE 1.2 Radionuclides of interest and related media in case of a nuclear accident.

Samples Radionuclides
131 134 137
Air I, Cs, Cs
3 89 90 131 134 137
Water H, Sr, Sr, I, Cs, Cs
89 90 131 134 137
Milk Sr, Sr, I, Cs, Cs
134 137
Meat Cs, Cs
89 90 134 137
Other foods Sr, Sr, Cs, Cs
89 90 95 95 103 106 131 134 137 144
Vegetation Sr, Sr, Zr, Nb, Ru, Ru, I, Cs, Cs, Ce
89 90 134 137 238 (239þ240) 241 242
Soil Sr, Sr, Cs, Cs, Pu, Pu, Am, Cm
Environmental radioactivity monitoring Chapter | 1 7

l Define the objective. when it is possible to sample only a small percentage of the
l Evaluate sources of direct radiation and radionuclides, whole. This type of sampling involves a selection process
especially the composition, concentrations, release in which each element in the population has an equal and
rates, points of release, and physical and chemical forms independent chance of being selected. Five main methods
of nuclides. include the following:
l Identify the pathways leading to exposure to man from
1. Judgmental (sample is taken on the judgment of the
source data by the use of analytical models for the
sampling person)
possible pathways and by the use of experience gained
2. Simple random (arbitrary collection of samples, having
at other sites and data on local meteorology, hydrology,
the same probability of being included),
and population distribution and diet.
3. Stratified random (random sampling based on additional
l Select the significant pathways that may be critical in
information)
terms of their contributions to exposure and determine
4. Systematic random (random sampling within subdi-
the critical population groups.
vided smaller areas of the original area)
l Consider the available analytical methods to select the
5. Systematic grid (subdividing the area of concern and
most effective combination of in situ measurements,
collecting samples from the intersections of the grid
sampling, chemical separation, and radionuclide anal-
lines)
ysis, that is, one that yields the required information
with least effort. By using statistical methods, probabilistic sampling at-
l Determine the consequent measurement requirements to tempts to increase the probability that generalizations
provide data for dose assessment for both normal and derived from the sample will be correct. Of the many types
abnormal conditions. of sampling strategies described in the literature, all are
l Allow for flexibility in the design as operational experi- useful in certain situations, but none is perfect. For
ence is accumulated and indicates that other types of example, a significant danger of using only probabilistic
measurements or measurement frequencies may be sampling techniques in field survey is that a major site may
desirable as the pathways and the other program re- be overlooked, resulting in a skewed analysis and nonrep-
quirements become better defined. resentative result. In any kind of environmental monitoring
program, the sample representativeness is an important
B. Sampling strategies issue. Representativeness in this context means that the
sample should reflect the conditions in the environment
The term sampling refers to strategies in selecting a sub- from which it is taken. A representative sample may be
group from a larger group and then uses this subgroup as a defined as one being able to answer questions in terms of
basis for making inferences about the larger group. The radiological information for which the analyses are per-
sampling strategy designed and adopted must deliver the formed. To put it in a more mathematical way, a repre-
necessary confidence and power to allow the appropriate sentative sample parallels the key variables and
inferences to be drawn. To do that, a number of important characteristics under examination and allows the collected
factors should be considered, including the nature of the results to be generalized to a larger population of which it is
control measure, the contaminant concerned, the nature and a subset.
location of the inputs, and statistical aspects of sampling In general, nonprobability sampling is less likely to
and analysis. The resulting measurements made following produce a set of specimens that is representative of the
the strategy should meet the requirements for emergency or population than valid probabilistic sampling, but repre-
regulatory management, or simply for compliance pur- sentativeness of environmental samples is difficult to
poses. The theoretical sampling strategy provides, as a demonstrate and usually considered justified by the pro-
minimum, a plan of what and where to measure, how many cedure used to select the samples (Gilbert and Pulsipher,
sampling units to collect, the time frame over which sam- 2005). It is necessary to keep in mind that site-
pling units should be collected, and the sampling fre- representative samples are not necessarily representative
quency. The consultation of experienced statisticians in a statistical sense. Accuracy and precision, which are
during the sampling design process may be appropriate. quality requirements on the analysis process, are of not
Generally, sampling strategies can be classified as either much worth if the samples are not representative to char-
nonprobabilistic or probabilistic. Nonprobabilistic sam- acterize site conditions.
pling is used when the sampling location of most interest is The inherent variability of environmental samples ne-
already known or on suspected sites with no need to sample cessitates careful design of sampling strategy. Since under
elsewhere, that is, judgmental sampling by subjective se- monitoring conditions the reasons for the variability cannot
lection of sampling locations. Probabilistic strategies, based be fully understood, a predefined sampling strategy should
on statistical considerations, on the other hand are common be used that is closely connected with an appropriate
8 Handbook of Radioactivity Analysis: Volume 2

statistical evaluation of the measured activities. In general, scattered and qualitative, however, and no materials as
activity levels in terrestrial samples are subject to spatial appropriate to the entire spectrum of encountered radio-
and temporal variability caused by various factors such as nuclides are known.
inhomogeneous spatial distributions of the deposited To minimize losses during sample collection and stor-
radioactive material in soil, redistribution of radionuclides age, containers of appropriate composition should be used.
by wind or by water erosion, differences in soil conditions The liquid contents can be frozen, acidified, or otherwise
and agricultural practices, and the superposition of different modified, by adding a complexing agent or stable carrier.
exposure pathways such as foliar uptake and root uptake. While it is important to avoid losses to container walls
Although this may not eliminate the uncertainty associated during storage, it is also important that the pretreatment will
with activity levels in environmental samples, it may not induce a change in the distribution of the radionuclides
reduce the uncertainty and enable it to be quantified by between the liquid and particulate matter or induce vola-
statistical means. tility losses of radionuclides.
In the case of normal discharges from licensed facilities, The sampling frequency will depend on the item to be
sampling locations should be selected close to points where measured and the variations with time in the activity con-
the maximum exposure or deposition is expected, prefer- centration in the media. In routine monitoring, the temporal
entially in the main wind direction for airborne discharges fluctuations are generally relatively low, so the frequency
or downstream from the release point for aquatic discharges may consequently be low. The time intervals between
and at the site boundary for direct radiation from the source measurements should reflect the half-lives of the radionu-
(Table 1.3). clides that are to be monitored. If the sampling time on a
Details of statistically based sampling designs, the filter is long in comparison with the half-life of the radio-
process of identifying survey unit sizes, laying out sys- nuclide concerned, this radionuclide may not be detected
tematic or random measurement grids, and methods for and the purpose of the monitoring is missed.
collecting samples are given in existing guidelines Samples are either taken manually from the environ-
(e.g., NRC, 1998a; NRC, 1998b; NRC, 1992; CIRIA, ment or accumulated in unattended devices and analyzed in
2000; BSI, 2001; MARSSIM, 2002; IAEA, 2005; USEPA, the laboratory or possibly in the field. Some collection
2006; ICRUM, 2006), in international standards (e.g., ISO devices have detector and recording systems that measure
18589-2, 2007), and in classic statistical sampling text- sample emissions during collection. Depending on the time
books, including Cochran (1977), Thompson and Seber response, online and off-line sampling/measuring devices
(1996), Thompson (2000), and Barnett (2002). are distinguished. For continuous monitoring systems,
There are some considerations in sampling radionu- sampling and counting times are identical, thus providing
clides beyond those shared with other types of environ- the information nearly real time. A reduction of sampling/
mental sampling. The type of radiation emitted by a counting time of online systems is tied to an expense of
radionuclide affects sample selection and eventual treat- statistical error, which in turn would demand an increase in
ment, because relatively nonpenetrating radiation such as the alarm levels. Shortcomings of online sampling systems
alpha particles must be measured in very small amounts of are in the limited possibilities of physical or radioanalytical
material, while gamma rays can be conveniently detected in sample preparations used to accumulate the radionuclides
bulk or unprocessed material. or for nuclide-specific techniques, thereby leading to lower
A common problem in collecting and storing a sample limits of detection, which are higher compared with off-line
of gas or liquid is loss of the radionuclide to the apparatus sampling and measurement.
and container surfaces. Selection of relatively nonretentive Nevertheless, determination of radionuclide concentra-
materials and minimization of areas and collection and tions in environmental materials collected and brought into a
sample transition times are recommended. Information on laboratory for analysis is the primary approach in environ-
the magnitude and rate of uptake by surfaces is widely mental radioactivity measurement. Samples that yield

TABLE 1.3 Pathways and related samples to be taken.

Release Pathway Samples


Atmospheric Inhalation Air
Ingestion Foodstuff
External Soil, direct measurement of ambient dose equivalent
Liquid Ingestion Marine food
External Water, direct measurement of ambient dose equivalent
Environmental radioactivity monitoring Chapter | 1 9

information most directly on radiation exposures of pop- activity so that the radionuclides can be measured with
ulations such as air, food, and water are of greatest interest in improved sensitivity or accuracy, and to reduce self-
monitoring programs. In some circumstances, field mea- absorption in the sample matrix for measurement of alpha
surements are sufficient, as there are a wide variety of in situ and pure beta emitters and low-energy photons.
measurement techniques available, including box counters, Sample preparation without recourse to special chemi-
portal monitors, in situ gamma spectroscopy systems, and cal separations is limited to total alpha-, beta-counting and
direct measurements with handheld instruments. In situ gamma spectrometry, but the samples have to be brought in
surveys are able to determine the radiation field properties, suitable form for measurement, which means a uniform
identify radionuclides, and determine their approximate distribution of the radioactive substances throughout the
concentrations but characterized by limited numbers of sample and the same sample size, thickness, and configu-
measurements with relative long count times. Thus, they ration within each group of samples. The question of ho-
may be combined with sampling and laboratory analysis. mogeneity becomes even more important as the range of
Laboratory determinations usually yield better descriptions the radiation becomes shorter, since self-absorption and the
of the analyzed material, greater analytical accuracy, and the sample detector geometry may vary in different parts of the
required sensitivity for radionuclides that do not emit sample. Calibration of these samples is usually performed
penetrating radiation. On the other hand, sampling requires with locally made standards having the same physical
greater efforts, provides information less promptly, and re- properties and known quantities of the appropriate radio-
quires additional interpretation for relating analytical results nuclides, in addition to traceable standards.
to the required environmental information. Any radiochemical analysis usually starts with obtain-
The general principles that apply to all sampling ac- ing a solution by the destruction of organic material in the
tivities include the following: sample. Materials that contain little organic matter can be
dissolved directly, since the dissolution treatment with
l The selection of types and location of in situ measure-
oxidizing acids will also remove the organic portion. Most
ments or sample collections and analyses, as well as
samples, however, must be oxidized first by wet ashing
the sample size and collection frequency to identify
(reaction with oxidizing agents in solution), dry ashing,
the radionuclides of interest, is to be based on informa-
with oxygen, or at room temperature with electrically
tion sources and modes of transfer through the environ-
excited oxygen. When samples are heated, care is to be
ment of radionuclides.
taken to avoid loss of the desired constituents by volatili-
l The radionuclide concentration, the sensitivity of the ra-
zation and splatter. For example, samples to be analyzed for
diation instruments, the capability of analytical
radioiodine cannot reliably be heated in the dry state but
methods, and the coordination of sampling and labora-
should be wet-ashed unless iodine is in one of its more
tory schedules define the numbers of samples.
highly oxidized states.
l All necessary parts of the sample are to be collected,
When igniting samples containing much organic matter,
and the samples have to be adequately preserved, so
such as food, the temperature should be raised gradually
that loss of radioactivity between the time of sampling
over an extended period to avoid flame-burning and to
and analysis is known or negligible.
minimize glow-burning. Losses of small particulates by
l Sufficient background samples are needed to provide in-
spattering can occur under these conditions. A partial
formation on preexisting nuclides from those under
oxidation of biological samples with nitric acid, followed
consideration.
by ashing in a muffle furnace, allows a lower final tem-
l Sufficient replicate samples should be collected to
perature (400e450 C) and will oxidize some of the volatile
determine variability of concentrations.
elements to less volatile forms.
Destruction of organic matter does not complete the
C. Sample preparation sample preparation process if chemical separations are to be
performed and the inorganic ash must also be dissolved.
High-sensitivity environmental analyses share common Complete dissolution of the sample is not necessary if it can
technologies, methods, processes, and information needs be shown that the desired nuclide is completely leached.
regardless of whether they are being used under normal Incompletely oxidized samples (gray ash) will be
operation conditions or in emergency situations. acceptable for gamma spectroscopy and many subsequent
Generally, sample preparation may include, but is not dissolution procedures. Usually, the dissolution process of
limited to, removing extraneous material, homogenizing, residues will oxidize small amounts of organic matter
splitting, drying, compositing, and final preparation of remaining after ashing, such as the gray ash. The samples
samples, to distinguish the desired radionuclides from may be entirely or almost entirely dissolved in nitric or
others that interfere with the final measurement by pro- hydrochloric acids, or in their mixtures. Substances not
ducing a response in a detector, to increase the specific easily dissolved with acids must be fused with appropriate
10 Handbook of Radioactivity Analysis: Volume 2

fluxes to obtain a solution. The higher temperature in- 2007; Maxwell and Culligan, 2009; Maxwell et al., 2010;
creases the reaction rates but may vaporize some radionu- Michel et al., 2008; Łokas et al., 2010; Spry et al., 2000;
clides. A combination of acids and fusion, such as that as Lee et al., 2011; Wand et al., 2004; Berlioz et al., 2005;
much as possible of the sample, is first dissolved by mineral Thakkar, 2002; Tavcar and Benedik, 2005; Martin and
acids, including hydrofluoric acid, and the insoluble residue Odell, 1998; Hrnececk et al., 2005; Srncik et al., 2008).
dissolved by fusion is often convenient. Typically combined procedures are starting with the
Any dissolution procedure should also include steps to separation of Pu and Th by anion exchange resins from
ensure that any added carrier or tracer is in the same concentrated HNO3 solution from Sr and Am, which are
chemical form as the nuclide being analyzed. Whatever collected together with other sample components in the
method is used to measure the recovery of a chemical effluent. Following preconcentration, Am can be separated
separation procedure, isotopic exchange or chemical and using a TRU column. Additional purification from lantha-
physical equivalency between the radionuclide in the nide impurities may be based on an anion exchange resin or
sample and the added carrier or tracer is essential. Isotopic the TEVA resin, whereas Sr is separated on a Sr resin
exchange such as converting multivalent elements to their column. Recently, three review papers about the analytical
highest or lowest oxidation states (e.g., hypochloride methodologies for the determination of plutonium as well
oxidation of iodine or ruthenium, sulfite reduction of as 241Am and 90Sr/90Y have been published (Vajda and
plutonium), or complexing or dissolving radium and Kim, 2010a,b,c).
barium sulfates (diethylene triamine pentaactetic acid Attention must be paid to some important details. For
[DTPA] or sodium carbonate fusion), should be under- example, the concentration of 239Pu in surface or ocean
taken, as early as possible in the analysis, before any water from fallout is of the order of 20 mBq/L, or about
chemical or physical operations are performed that might 5$1017 M, and this concentration is obtained with 2$107
result in loss of the desired nuclide. For many nuclides, atoms. In soil, a common plutonium concentration from
dissolution in mineral acids is sufficient to effect isotopic fallout is about 2 mBq/g. This activity can be obtained from
exchange. one plutonium oxide particle with a diameter of 0.1 mm. At
Attention must also be paid to the chemical and physical the very low concentrations frequently encountered,
form, that is, the ionic or nonionic form and oxidation state, contamination of the sample with extraneous radionuclides
of the radionuclide aside from the isotopic exchange during processing must be avoided, and the blank value
question, even when the carrier or tracer is not used. To put must be known and kept low and constant. In addition to a
it in a simple way, the radionuclide must be brought into a low blank, high radiochemical purity in the separation is
form in which it undergoes the expected reactions in the also needed for good accuracy and sensitivity. Reagents
separation process. must be carefully checked for radioactivity. For example,
The fundamentals of the conventional radiochemical the environmental concentration of thorium is approxi-
methods are precipitation, coprecipitation, ion exchange, mately 103 times that of the chemically similar plutonium;
and solvent extraction (ISO 18589-4, 2009; ISO 18589-5, thus, decontamination from thorium by a factor of 105 or
2009). A great variety of methods have been developed in more is required for a satisfactory plutonium analysis.
the past, but the most valuable development of the past These difficulties encountered as a result of very low
years has been the development of extraction chromato- concentrations can be avoided by adding macroquantities of
graphic materials, such as Sr-specific crown ether-based inactive isotopes of the same element, or of similar elements
material, Sr resin, or the transuranium elementespecific if no stable isotope exists. This procedure, the use of carriers
extraction chromatographic materials, (UTEVA, TRU, for radioactive tracers, is frequently used for measuring the
TEVA resins), developed by Horwitz et al. (1991, 1992a, chemical yield of a separation procedure. The chemical
1992b, 1993, 1995). These materials have become separations are greatly simplified since now the element can
commercially available as the registered products of be expected to exhibit its normal behavior, and the analytical
Eichrom Technologies, Inc. and TrisKem International problem is no longer one in ultratrace chemistry.
SAS, and these have replaced conventional methods based
on a series of precipitations. D. Measurement and quantification
In addition to procedures for the individual determina-
tion of the nuclides, a great variety of combined procedures For a long time, the outstanding measurement method in
for the simultaneous determination of actinides and radio- environmental monitoring has been the determination of
strontium isotopes in a variety of environmental substances gross alpha- and gross beta activities applying gas-flow
based on different combinations of ion exchange separation proportional counters after preparing a solid sample of
and extraction chromatography or the even pure extraction known thickness and area. The sample can be the residue
chromatography have been developed (Moreno et al., 1997; remaining after evaporation of a water sample, soil, sedi-
La Rosa et al., 2001; Mellado et al., 2001; Maxwell, 2006, ment, ashed vegetation, or other solid material. Since the
Environmental radioactivity monitoring Chapter | 1 11

samples generally contain an unknown radionuclide is not as efficient as the NaI detector, but it is capable of
mixture, an arbitrary choice must be made in selecting a distinguishing between very closely spaced energies. The
standard for calibration of the counting system and deter- energy resolution measured as the full width at half the peak
mining the conversion of sample counting rates to disin- maximum (FWHM) for typical coaxial germanium detectors
tegration rates. The arbitrary but necessary choice of a is between 1.6 and 2.1 keV for 1.33 MeV gamma rays,
standard nuclide introduces the largest uncertainty in the depending on the size and quality of the detector. The peak-
disintegration rates inferred from counting rates of thick to-Compton ratio is generally 40e100, again depending on
samples, since correction factors are energy dependent, but the size and quality of the detector.
by convention, the same alpha counting efficiency is Alpha spectrometry systems, typically, consist of the
assigned for all the alpha emissions and the same beta silicon diode surface barrier detector housed in a light-tight
counting efficiency is assigned for all the beta emissions vacuum chamber, a bias supply, amplifier, analog-to-digital
(ISO 18589-6, 2009). converter, multichannel analyzer, and computer. The bias is
Advances in gamma spectrometry, in alpha spectrom- typically 25e100 V. The vacuum is typically less than 0.1
etry and in liquid scintillation counting (LSC) and spec- millitorr. Since the sample and detector are in a vacuum,
trometry for alpha and beta emitters, have obviated many of most commonly encountered alpha energies will be detec-
the reasons for measuring total activity, but low-cost gross ted with approximately the same efficiency, provided there
measurements, preferably applying alpha/beta, separated is no self-absorption in the sample. The system is appro-
LSC measurements (Sánchez-Cabeza, and Pujol, 1995; priate for all alphas except those from gaseous radionu-
Zapata-García et al., 2009; Palomo et al., 2011; Schu- clides. Samples have to be prepared by means of chemical
macher et al., 2014) may still serve as a rapid and cost- separation. A known amount of a (diluted) standard solu-
effective screening procedure. tion (tracer) may be added before separation to determine
A very effective tool for measuring the concentration of the overall recovery of the sample from the chemical pro-
radionuclides in soil, water, air filters, and swipes is pre- cedures and/or quantification by isotope dilution.
sented by LSC. Samples or an aliquot may be placed Following conversion to a particulate having very little
directly into an LSC vial of cocktail and counted without mass and collection on a special filter (micropreciptation),
further preparation or first processed by ashing, radio- or collection from solution by electroplating onto a metal
chemical, or solvent extraction, or pulverizing to place the disk, the sample is then placed in the vacuum chamber at a
sample in intimate contact with the LSC cocktail. Actions fixed distance from the diode and analyzed. For environ-
such as bleaching the sample may also be adequate to make mental levels, counting times are in the order of
the cocktail solution transparent to the wavelength of light 80,000 seconds or more, providing detection limits in the
it emits. Additionally, very-high-energy beta emitters order of 1 mBq/g or below. Typical energy resolutions are
(above 1.5 MeV) may be counted using liquid scintillation in the range of 10e20 keV.
equipment without liquid scintillation cocktails by use of Alpha counting procedures are capable of sufficient
the Cerenkov light pulse emitted, as high-energy charged sensitivity to determine levels for monitoring and dose
particles move through water or similar substances. The use assessment. However, the potential of long-term buildup of
of pulse shape discrimination has allowed increases in long-lived radionuclides indicates that more sensitive
sensitivity by electronic discrimination against beta and methods may be required to determine the routes and rates
gamma emitters. However, beta energy spectra are 10e100 of movement through the environment. For these purposes,
times broader than gamma spectrum photopeaks so that mass spectrometry provides a unique and valuable tool
quantitative determination of complex multienergy beta (Ross, 2008 and Becker, 2007, 2010).
spectra is hardly possible. For the determination of 239Pu and 240Pu, which can
Environmental samples containing gamma-emitting ra- give direct information on the content of fissionable 239Pu,
dionuclides can be measured by means of gamma spec- mass spectrometric methods such as inductively coupled
troscopy. Although scintillation counters using a sodium plasma mass spectrometry (ICP-MS) and accelerator mass
iodide crystal with a thallium activator, NaI(Tl), have been a spectrometry (AMS) are necessary (Povinec et al., 2001).
mainstay of gamma ray spectrometry since 1948, they are ICP-MS has been widely applied for this purpose, although
superseded by semiconductor-based assemblies with the care must be taken to remove interferences like 238UHþ,
detector of choice for most applications to be a high- which can influence the determination of 239Pu (Hrnecek
resolution hyperpure germanium crystal (HPGe), whereas et al., 2002; Chiappini et al., 1996; Muramatsu et al., 1999,
silicon detectors are used for gamma spectrometry at low 2001). A partial review of how to overcome spectral
energies. Germanium has the advantages with respect to overlaps in elemental ICP-MS was presented by Vanhaecke
silicon of a smaller bandgap (Ge: 0.665 eV vs. Si: 1.12 eV at and Moens (2004).
77 K) for better energy resolution and a higher Z (32 vs. 14) For plutonium isotopes, the main advantage of AMS
for better photoelectric absorption. The germanium detector compared with conventional MS (TIMS, ICP-MS) is the
12 Handbook of Radioactivity Analysis: Volume 2

complete destruction of molecular isobars (e.g., 238UHþ for procedure for accreditation of analytical laboratories
239
Pu) by stripping to high positive charge states in the ter- through national accreditation bodies is a proper means to
minal of the tandem accelerator (Oughton et al., 2001). enhance acceptance and legal recognition of analytical re-
Additionally, this method permits the determination of higher sults worldwide. The global quality standard for analytical
mass plutonium isotopes such as 242Pu and 244Pu in envi- laboratories is the ISO/IEC 17025 (ISO, 2017). These
ronmental samples (Fifield et al., 1996; Hrnececk et al., 2005). standards set out specific management and technical
Mass spectrometric methods have been reviewed for the requirements.
determination of transuranium elements, for example, by While management requirements are mainly related to
Betti et al. (2006). Hou and Ross (2008) extensively the operation and effectiveness of the quality management
compared radiometric and mass spectrometric methods for system and more or less identical to ISO 9001 re-
long-lived radionuclides. They concluded that mass spec- quirements, technical requirements focus on the qualifica-
trometric techniques, although susceptible to isobaric tion and competence of staff, testing methodology,
interference and the need of extensive equipment and infrastructure and equipment, and reporting of results.
infrastructure, are valuable rapid analytical methods for the The sampling, sample handling and preparation,
determination of many long-lived radionuclides, including analytical procedures, and other factors, which might have
99
Tc, 237Np, and isotopes of uranium, thorium, and pluto- an influence on the result, have to be documented carefully,
nium (Table 1.4). for example, as standard operating procedures (SOPs), to
allow reevaluation of results if doubts about their reliability
E. Quality assurance/quality control come up. SOPs detail the work processes that are con-
ducted or followed within an organization and document
As the results of environmental monitoring are of funda- the way activities are performed. The benefits of a valid
mental importance not only to assess environmental condi- SOP are reduced work effort combined with improved data
tions but also to support decision-making, policy comparability, credibility, and legal defensibility and pro-
development and prioritization of policies based on solid moted quality through consistent implementation of a
information, the application of quality assurance and quality process even if there are changes in personnel.
control measures during the data collection process, data In addition, particular attention should be paid to the
storage and access is a fundamental component of any requirements on method validation, in terms of accuracy,
effective environmental monitoring program to ensure repeatability and reproducibility, the use of calibration
quality and comparability of the analytical results. As a standards that are traceable to national or international
minimum, an adequate quality assurance program satisfies standards, instrument calibration, and performance testing.
the general requirements established by the regulatory body. In providing robust and sound analytical results, it is
To minimize laboratory incidents, such as the mislabeling of inevitable to understand that every measurement will al-
samples or biased analyses, quality control and quality ways be subject to a certain amount of uncertainty. Un-
assurance concepts have been developed to assist the labo- certainty is a measure giving the quality and accuracy not
ratory personnel to achieve a higher degree of transparency only of a sample analysis but of the measurement program.
of procedures, minimize potential sources of error, stan- Uncertainty in environmental monitoring results arises
dardize the handling of samples, instruments, and data, and primarily from design errors, the nonrepresentativeness of
in the end, decrease the rate of nonconformance results. samples and/or measurements, human errors, and mea-
Particularly in the case of sensitive materials, this has surement uncertainty. These uncertainties cannot be fully
been recognized as early as the 1950s in the nuclear in- eliminated but can be reduced as far as possible.
dustry, and concepts have been developed to assure trace- Nonrepresentativeness occurs when the sampling or
ability of materials, and of course, reliability of results. field measurement is unable to capture the complete extent
Many different branches of industry have adopted, refined, of variability that exists for the radionuclide distribution in
and further developed these concepts, because it has been a survey unit. Since it is impossible in every situation to
realized that a formal quality control and quality assurance measure the residual radioactivity at every point in space
system helps achieve a stable level of high-quality output. It and time, the results will be incomplete to some degree. It is
was only in the late 1980s that similar strategies became also impossible to know with complete certainty the re-
attractive to research laboratories and, in particular, EUR- sidual radioactivity at locations that were not measured, so
ACHEM and ISO started to set up guidelines and norms for the incomplete survey results give rise to uncertainty. The
the implementation of these measures (e.g., the ISO 9000 greater the natural or inherent variation in residual radio-
series). Finally, the idea of a formal accreditation of labo- activity, the greater the uncertainty associated with a de-
ratories following quality guidelines was developed and cision based on the survey results. Representativeness in
now is widely accepted thatdthrough the advent of inter- sampling and/or in field measurements can be optimized by
national trade and exchangedan internationally agreed
TABLE 1.4 Detection limits, separation, and counting times for radionuclides of interest in environmental media.
Detection limit
Nuclide Method (mBq/Sample) Preparation time Count time Reference
239þ240
Pu, Alpha spectrometry 0.02 2e4 days 5 days Varga et al. (2007)
238
Pua
241
Pu LSC 11 2e3 days 5 hours Liong Wee Kwong (2004)
224
Ra Gamma spectrometry 70 - 1000 minutes Parekh et al. (2003)
226 Gamma spectrometry 80 - 2400 minutes Parekh et al. (2003)
Ra
222
LSC 0.3e1.4 2h (þ30 days ingrowth of Rn) 6 hours Sanchez-Cabeza and Pujol (1998)

Alpha spectrometry 0.2e0.5 2e4 days 2 days Purkl S and Eisenhauer (2003); Karamanis et al.,
2006
228 Gamma spectrometry 110 - 2400 minutes Parekh et al. (2003)
Ra

Environmental radioactivity monitoring Chapter | 1


228
LSC 0.1 1e2 days (þ48 h ingrowth of Ac) 60 minutes Nour et al. (2004)
228
LSC (Cerenkov 0.3 1e2 days (þ48 h ingrowth of Ac) 100 minutes L’Annunziata and coworkers (see Aleissa et al.,
counting) 2008)
Alpha spectrometry 0.2 2e4 days (þ12 months ingrowth 3 days Purkl and Eisenhauer (2003)
of222Rn)
90
Sr/90Y LSC (Cerenkov) 10 1e2 days (þ20days ingrowth of90Y) 3hours Suomela et al. (1993)
90
LSC 10 1e2 days (þ20days ingrowth of Y) 3hours Popov et al. (2006)
a
Same detection limits are achievable for all other actinides.

13
14 Handbook of Radioactivity Analysis: Volume 2

means of an appropriate sampling and measurement good measuring efficiency. Electrostatic precipitators,
scheme as described above. cyclone collectors, and cascade impactors are in use to
Whereas incorrect calibration may be detected and collect particles and classify them according to size.
corrected at a later stage, errors in the treatment of the Since the radionuclide concentrations are reported per
samples cannot readily be detected and corrected. unit volume of air (Bq/m3), the air should be drawn through
Furthermore, the storage of samples allows the repetition of the filter at a known rate for a known period of time,
measurements on the samples that are obviously not cor- preferably using an integrating flow meter to give the total
rect. Regular training and exercises should be conducted for volume. When high dust concentrations occur during
the staff to maintain the experience of personnel as an sampling, it may not be possible to maintain a constant air
important precondition for high-quality work, especially flow through the filter. The collection efficiency may
under stress in emergencies. change during operation if too many solids accumulate.
Human errors may give rise to, for example, improper Several types of filter material (glass fiber, paper, cel-
recording, loss of samples, incorrect labeling, cross- lulose) are used for collecting aerosol materials. The type of
contamination during sample preparation, and contamina- filter is selected according to the needs for high collection
tion of measurement devices. Adequate training of efficiency, particle size selectivity, retention of gaseous
personnel and quality assurance procedures should be used iodine with the particles, and ease of radiochemical anal-
to reduce human errors, even in emergency conditions. ysis. It may be desirable to change filter media for specific
purposes or to use several filters in series.
Lozano et al. (2011) propose the use of quartz filters to
IV. Monitoring for internal exposure collect alpha-emitting natural radionuclides.
A. Air Pure cellulose papers are useful for samples to be dis-
solved and analyzed radiochemically, but the analytical
Monitoring of airborne radioactive material in either par-
filter papers used to filter solutions are inefficient collectors
ticulate or gaseous form in air is of particular importance to
for aerosols and clog easily. Of particular value for samples
estimate radiation exposures from external radiation or
to be analyzed radiochemically are filters composed of
inhaled radionuclides; it provides the first opportunity to polystyrene fibers. They are efficient and capable of sus-
identify the spectrum of radionuclides making up the
taining high air flow rates without clogging, are readily
contamination and transfer of the deposited radionuclides
destroyed in analysis by ignition at low temperatures
through the food chain. Except for radon, the noble gases
(w300 C) or by wet ashing with oxidizing agents, are also
are not of great concern for internal exposure but contribute
soluble in many organic liquids, have the disadvantage of
to the external exposure (Mück and Henrich, 2001).
very low mechanical and tensile strength, and must be
Since the natural radioactivity concentrations under
handled carefully. Fiberglass filters can function efficiently
normal conditions are significantly higher than the artificial
at high flow rates but require fluoride treatment for disso-
activity concentrations, accumulation methods are required. lution and generally contain some radionuclides, for
If the concentration is needed, the volume of air is
example, 40K, to complicate low activity analysis. Over-
measured in terms of flow rate. When the radionuclide
views of filter media, classification, performance data,
activity per total amount of the element is to be determined,
collection efficiencies, and practical selection tables are
a passive device, such as a bag of silica gel or zeolite
available (e.g., Purchas and Sutherland, 2002; Ruzer and
suspended in air to collect tritiated water, may be
Harley, 2005; and Papastefanou, 2008).
satisfactory. Retention efficiency must be tested under
operating conditions, and possible adverse effects on the
2. Online versus offline systems
collection efficiency by other gases at various concentra-
tions should be tested. The chemical form of the radionu- Aerosol filtration can be accomplished by either moving
clide especially influences the collection efficiency. Data on filter bands in online systems or offline with fixed filter
atmospheric stability, wind speed, and wind direction under sheets. Both solutions have their advantages and draw-
which the samples were collected should be noted. backs, and obviously, they require different measuring ar-
rangements and different data evaluation algorithms.
The concept of moving filter bands means that the
1. Aerosols
adsorbing surface is (partially or totally) renewed from
Aerosol monitoring includes sampling and measuring units measurement to measurement. Thus, the sampled volume is
that collect dust by drawing air through a filter material. relatively less than that of a fixed filter sheet with the same
The filters coupled to air pumps are capable of accumu- air rate (w25 m3/hour compared with 100e1000 m3/hour),
lating particulates from a large volume of air onto a small and so does the accumulation of a suspected artificial
surface; their radioactive content can be determined with radiocontamination as well. On the other hand, the amount
Environmental radioactivity monitoring Chapter | 1 15

of accumulated natural radioactivity will also be less in this done very effectively by simultaneous coincidence
case. Radionuclides on air filters are dominated by the counting of alpha decay and by assuming that there is
naturally occurring, short-lived particulate decay products no contribution of artificial alpha emitters. In this
of radon (1e20 Bq/m3 in outdoor air) and will also include way, concentrations of artificial radioactivity down to
cosmogenic 7Be. 0.1 Bq/m3 can be detected. One may also perform a sec-
The moving band concept has significant advantage ond delayed beta-counting after, for example, 12 h
over the fixed filter systems if the concentration of artificial (most short-lived daughters will then have decayed,
radioactivity in the sampled air steeply increases. This step- except 212Pb).
function-like phenomenon can occur in local monitoring l Gross alpha: That is, total alpha minus natural alpha
systems where the possible source of contamination is close radioactivity. The measurement is done by gas flow pro-
to the sampling station. In regional systems, the activity portional counters, with or without anticoincidence or
concentration of artificial radionuclides may increase due to passivated, ion-implanted planar silicon detectors
atmospheric dispersion of radioactivity emitted from a (PIPS). Lower detection limits range between 1$105
(probably) distant source. This dispersion process is gov- and 4$102 Bq/m3.
erned by laws of long-distance diffusion so the increase l Nuclide specific: To ensure optimum early warning,
cannot be as vivid as it is assumed for cases of local these instruments are designed to allow the simulta-
monitoring. Therefore, a slow buildup rate is expected so neous alphaebeta measurement and the nuclide-
the “early warning” requires accumulation of specific measurement. In the automatic mode, modern
radioactivitydthis condition means the supremacy of fixed instruments are capable of reaching low detection limits
(or slowly moving) filter systems over those of fast filter by means of high-purity Ge detectors.
increment. Moving filter facilities allow automatic opera-
General aspects pertaining to online monitoring systems
tion up to 6 months and are particularly used in automatic
(IEC, 2002a, 2002b) and regarding both continuous and
monitoring networks. One automatic station design of the
discontinuous sampling (ANSI, 1999; ISO-2889, 1975) of
IMS (International Monitoring System) Radionuclide
discharges to the atmosphere can be found in international
Network uses a small robot to cut the filter in pieces after
standards.
the collection process, which are afterward stacked into a
neat pile for gamma measurement. The cutting edge works
well on glass fiber filter material but badly on organic ones 3. Gaseous effluents
(Medici et al., 2004).
Effluents can be present in air in gaseous forms that are not
Fixed filter devices only permit sampling periods of
collected on particulate filters. Thus, special cartridges of
maximum 1 week and thus require considerable operational
activated charcoals or zeolites, both of which also may be
service. High sampling rates are achieved with high capacity
silver impregnated, are necessary for efficient collection. Flow
blowers and large area filters. The filters are usually com-
pressed to provide a standard counting geometry and are rates through these cartridges are normally lower than those
for normal aerosols. Drawback of these filters is that,
measured by gamma spectrometry. Most institutes perform
depending on the concentration, they become saturated and
correction from natural radioactivity by waiting 2e5 days
have to be replaced. However, silver zeolite cartridges are very
before measuring the filter. Detection levels of a few mBq/m3
expensive, and charcoal cartridges are more commonly used.
can be obtained, for example, 10e30 mBq/m3 for 140Ba with
Radioactive gases can be measured in many types of
an airflow of 1000 m3/hour (Schulze et al., 2000). Subse-
counters with suitable sample chamber or the gas being
quently the filters may be dry- or wet-ashed for radio-
placed inside the detector and spectrometers, including
chemical analysis of pure alpha or beta emitters (e.g., 239Pu
and 90Sr) using alpha spectrometry or LSC, respectively. coincident detection of different radiation types. To prepare
a gas sample for counting, it should be separated from the
Widely used measuring methods of online systems are
air and purified. This process consists of separations by
as follows:
charcoal and molecular sieve columns and purification by
l Gross beta: That is, total beta radioactivity with correc- drying and chemical reactions to remove the impurities
tion for natural radioactivity (mostly influenced by (Cummings et al., 1971; Stevenson and Johns, 1971; Johns,
radon daughters). The measuring instruments used are 1973; Medici et al., 2004; Bowyer et al., 2002).
GeigereMüller, gas flow proportional counter with 3
H and 14C gas samples are usually not counted as
different active surfaces, and plastic scintillators with gases, as 3H is usually converted to water and 14C gas
ZnS coating, mostly in anticoincidence configuration. samples are converted into benzene or similar liquid for
Depending on the methods used, the lower detection counting in liquid scintillation counters. To use the liquid
limits range between 5$105 and 1 Bq/m3. Distinction scintillation technique for radioactive gases, they must be
between natural and artificial radioactivity can be soluble in the liquid scintillation medium.
16 Handbook of Radioactivity Analysis: Volume 2

a. Iodine measurement Ionization chambers provide a theoretical sensitivity in


Iodine in air can be bound to aerosols or in the gaseous the order of 1014 A/becquerel at equilibrium. The detection
state, each requiring special measuring techniques. Iodine limit is variable with the volume of the ionization chamber
sampling is carried out by means of “traditional” filter pa- and the measuring time, which is in the order of 30 minutes
pers or charcoal drums. The filter paper captures the iodine to hours. Typically using a 1-L ionization chamber, one can
attached to aerosols, the charcoal captures the gaseous detect about 5 Bq/m3 with an uncertainty of 10%e20%
iodine, and the combination of the two measures the total (Pohl and Pohl-Rueling, 1976; Friedmann, 1983).
amount of iodine in air. Lucas cells are containers coated inside with ZnS(Ag)
Filter sheets containing charcoal and iodine-specific and having a quartz window transparent to scintillation
impregnated material are available. The advantage of the photons. The container is filled with radon containing air,
latter is obvious: the filters can be replaced easily and and scintillation photons are measured after equilibrium with
automatically, and their measuring geometry provides the short-lived radon progenies is reached. Since each alpha
much better counting efficiency. particle emitted from a decaying radon atom is followed by
As far as regional monitoring is concerned, the “ex- two others from the decaying radon progenies, the theoret-
pected” iodine radioisotopes are the relatively long-lived ical conversion factor is 3 pulses/becquerel. Practically, this
fission products 131I, 132I, and 133I. All of them are beta factor is between 2 and 2.5 scintillations/becquerel.
and gamma emitters, so iodine filter sheets are coupled to For time-integrated measurements mainly passive
the appropriate detectors described above. If further instrumentation, such as adsorption on charcoal, diffusion
radiochemical processing of filter sheets is possible and chambers with and without filters, thermoluminescent de-
required, the extremely long-lived 129I can also be analyzed tectors, or solid-state nuclear track detectors are used
(Hou et al., 2009). 131I concentrations in the order of currently. Solid-state nuclear track detectors are made of
hundreds of mBq/m3 can be measured in 1 hour. In the case materials such as cellulose nitrate (LR115), polycarbonate
of an accident, the ratio of gaseous 131I to 131I attached to (Makrofol, Lexan), or allyldiglycol polycarbonate (CR39).
particulate matter can vary between 2 and 20. The reading of these types of detectors is done after an
(electro-)chemical etching process by optical devices, for
b. Radon measurement example, as track density, changes in optical transparency,
or by scintillation technique. As etching agent a solution of
There are many different methods available for the mea-
mainly potassium hydroxide or sodium hydroxide in
surement of radon and its short-lived decay products, active
different concentrations and varying ratios of ethanol are
as well as passive, short term as well as continuous or time
used, depending on the detector quality, the kind of etching
integrating monitors. Some of them are very sophisticated
process, and alpha energies to be detected.
and promise an accuracy of the measurement in the order of
Excellent reviews on solid-state nuclear track detectors
a few percent. Many of those are very sensitive not only to
are given by an OECD/NEA group of experts, published in
radon but also to environmental parameters and therefore
OECD (1987), by Ilic and Durrani (2003), Guo et al.
fail, for example, in a wet environment. Others are less
(2012), and in Chapter 3, Volume 1 of this book.
accurate, but they give reliable information on radon under
difficult conditions. Instruments are called active, when any
kind of external or internal power supply is needed for c. Noble gases other than radon
operation. Instruments are passive, when no external power Krypton and xenon are inert noble gases and, therefore,
supply is necessary for operation. usually one of the first radionuclides that can be emitted in
For the detection of radon gas, only the instrument has processes that produce fission products. Due to their inert
to be designed in a way that the noble gas, separated by nature, krypton and xenon radioisotopes are unlikely to
means of an aerosol filter from its decay products and other contribute significantly to internal exposure but are parts of
aerosols present in air, is permitted to enter the sensitive the external exposure due to the plume after an accidental
volume where the radon is allowed to decay for a defined release to the air.
period of time. Thus, the radon measurement is basically a Furthermore, krypton and xenon do not have a major
radon and radon progeny measurement. In that case, all deposition rate from the atmosphere and therefore can
suitable detectors are applicable to detect charged particles travel long distances following a release and be detected
and photons emitted from the decaying radon and its decay with sufficiently sensitive instruments. In addition, the half-
products. For reasons such as the selected alpha and / or lives of some of their isotopes (85Kr half-life: 10.8 years
beta particles and the insensitivity to photons, only ioni- and 133Xe half-life: 5.3 days) are nearly optimal for
zation chambers, alpha spectrometers and scintillation detection, because they are short enough that they do not
methods (e.g. Lucas Cells) are used for the active mea- build up in the atmosphere from decay of geological ura-
surement of radon gas. nium or anthropogenic sources, yet they are long enough to
Environmental radioactivity monitoring Chapter | 1 17

survive windborne travel distance from the source at xenon gas into a favorable counting geometry. Several
detectable levels. sources explain the state-of-the-art for this process in some
The major sources of 85Kr are nuclear fuel reprocessing detail (e.g., Stockburger et al., 1977; Ringbom et al., 2003).
plants located in the northern hemisphere. Due to its long Mainly, four automatic xenon measurement systems
radioactive lifetime, 85Kr has spread out all over the globe; have been developed: the Automatic Radioanalyzer for
typical background levels in the northern (southern) Isotopic Xenon (ARIX), from the Khlopin Radium Institute
hemisphere are currently about 1.3 Bq m3 of air. The (KRI), Russia; the Automated Radioxenon Sampler-
yearly global release rate of 85Kr to the atmosphere exceeds Analyzer (ARSA), from the Pacific Northwest National
the removal rate by radioactive decay, resulting in a slow Laboratory (PNNL), United States; the Swedish Automatic
but continuous increase of atmospheric concentrations Unit for Noble Gas Acquisition (SAUNA), from Total-
worldwide, which has been of some scientific concern försvarets Forskningsinstitut (FOI), Sweden; and the Sys-
(WMO, 1996). The well-known source term and its tème de Prélèvement d’Air Automatique en Ligne avec
chemically inert properties make 85Kr a useful tracer for l’Analyse radioXénons atmosphériques (SPALAX) from
studies of the regional and the global air circulation (Jacob Departement Analyse, Surveillance, Environnement du
et al., 1987; Zimmermann et al., 1989; WMO, 1996). CEA (CEA/DASE), France. An overview of the system
Monitoring of 85Kr may have some importance for nuclear features can be found in Bowyer et al. (2002); Ringbom
safeguards (Kalinowski et al., 1998). Clandestine produc- et al. (2003); and Fontaine et al. (2002).
tion of plutonium for nuclear weapons can be detected by
the monitoring of 85Kr in the air. B. Soil, sediments, vegetation, and deposits
About 20 radioactive isotopes of xenon are formed in
fission of heavy elements such as uranium or plutonium. Sampling of soils, deposits, and vegetation and subsequent
Most of these isotopes decay within seconds, but a few measurement of radionuclide concentration is an appropriate
have half-lives of several hours to several days and, thus, method for evaluation of levels of ground contamination due
are detected in the environment near nuclear facilities such to dry or wet deposition, the contribution to the evaluation of
as medical isotope production facilities (Saey et al., 2010), levels of total deposition per unit area on all surfaces, the
near operating nuclear reactors, and also following nuclear prediction of dose rates, and time dependence of dose at the
explosions. This is one of the basic reasons why monitoring location, and with use of transfer coefficients, a rough esti-
of radioactive noble gases in the atmosphere has been mate can be obtained for the future contamination of vege-
performed for decades. Radioxenon backgrounds range tables. Additionally, ground contamination may be a source
from well below 1 mBq m3 in much of the southern of resuspension of radioactivity that may cause inhalation
hemisphere (Bowyer et al., 1997) to 1000 mBq/m3 near hazards and additional dispersion of radioactivity.
medical isotope production facilities. However, most of the
world has backgrounds in the range of 1e100 mBq/m3. 1. Laboratory based
Radioactive xenon has four isotopes that are commonly
a. Soil and sediments
detected by many groups and by the International Moni-
toring System (IMS) of the Comprehensive Nuclear-Test- Soil sample analysis is a common method of environmental
Ban Treaty (Saey and De Geer, 2005). These isotopes are monitoring. Sampling depths vary with the purpose of the
131m
Xe (t½ ¼ 11.9 d), 133Xe (t½ ¼ 5.2 d), 133mXe study and the soil characteristics. The conventional sam-
(t½ ¼ 2.2 d), and 135Xe (t½ ¼ 9.1 h). pling technique of soils is core sampling. Because the
The basic techniques for measuring radioactive krypton concentration of deposited radionuclides usually decreases
or xenon isotopes in the atmosphere have been available for rapidly with depth in undisturbed soil, one may have to
a number of years using a variety of methods (Ludwick, sample as a function of depth, with both the collection area
1966; Schölch et al., 1966; Bernstrom and DeGeer, 1983; and the depth noted. For radionuclide availability studies,
Kunz, 1989; Bowyer et al., 1996). Sensitive detection of samples should be taken in crop areas with a coring tool to
krypton and xenon isotopes is commonly performed after a depth of 5 cm or to the depth of the plow line.
separation of the gas from large volumes of air from the Migration in the soil depends on the radionuclide and its
major interfering constituents of air, such as N2, O2, Ar, chemical form and the soil type, but most artificial radio-
CO2, H2O, Rn, etc. by collecting the gas on adsorbents nuclides are found in the upper 30 cm soil layer. Because of
(e.g., through activated charcoal under reduced pressure at the possibility of large microscale variations of deposition,
liquid nitrogen temperature) followed by the use of gas it is very important to take a sufficient amount of soil
chromatography using CH4 as a carrier gas to both further samples to obtain a reasonable estimate of the deposition of
separate the xenon from radon and to insert the krypton or radioisotopes at a given site. The sample should also be
18 Handbook of Radioactivity Analysis: Volume 2

defined according to soil characteristics, agricultural status, mesh size of 2 mm. Activity in soil samples is reported on a
and vegetation cover. The latter should be analyzed sepa- dry weight basis in Bq/kg and on an area basis in Bq/m2.
rately. Sampling tools vary, but any device that will cut a The question of complete dissolution versus leaching of
straight core will be satisfactory. Samples should be taken soils is still being debated for certain analyses. Plutonium
with coring tools of known diameter so that the ground area from worldwide fallout can be successfully leached with
represented by the sample is accurately known. In general, acids, if a plutonium tracer in the same chemical form is
about 10 cores (or a total surface area of at least 200 cm2) used to monitor the yield. Other forms of plutonium, such
are taken and composed to make a single sample. as those produced in a laboratory or fuel reprocessing plant
Sediment is an indicator and accumulator of radionu- by high temperature ignition, require digestion methods
clides that are insoluble and adsorbed on insoluble material (e.g., high-pressure microwave, plasma, etc.) or repeated
in the aquatic system. Conventional collection is by a treatments with hydrofluoric and mineral acids for complete
dredge dropped from a boat. The dredge mechanism is dissolution.
activated by contact with the benthos. For river sediments, In typical radiochemical procedures to analyze for Pu,
it is of interest to describe the stream flow conditions that Am, and Sr in soils, 10 g of ashed material is taken for the
lead to benthal deposition and the movement of the sedi- analysis. If no stable strontium is present in the sample,
ment, as well as the characteristics of the sediment such as 10 mg of strontium carrier and spikes of 243Am and either
236
particle size distribution, soil type, ion-exchange capacity, Pu or 242Pu tracers are added. The selection of the
and organic content. Collected samples are treated similarly amount of the spikes depends on the expected activity
to soil samples except that the accumulation from and concentrations present in the sample, but typically
interaction with the aquatic environment must be consid- 10e50 mBq of each are added. The use of HF will be
ered rather than deposition from air and uptake by grass. recommended for sample dissolution to facilitate the total
Drying at low temperatures (50 C) to avoid the loss of decomposition of the matrix, since 90Sr might be contained
radionuclides from the soil and hand mixing of soils or in the lattice of the silicate material or in refractory oxides.
sediments prior to subsampling should be acceptable for The sequential treatment with mineral acids usually results
gamma spectroscopy where a relatively large subsample is in the dissolution of greater than 99% of the sample, and
used (e.g., 150e500g). However, drying, grinding, and the resulting solution is filtered through a 0.2-mm poly-
sieving prior to subsampling should be carried out where a propylene membrane filter. The leachate solution is used
small subsample (e.g., 5e10g) is to be taken for radio- for the radiochemical separation of Pu from Am and Sr by
chemical analysis. Commercially available grinders, mills, anion exchange followed by the preconcentration of Am
pulverizers, mixers, and blenders are suitable. Hardened and Sr by coprecipitation with calcium oxalate. Am is
metals are best for the grinding surfaces, and it is not likely separated from Sr by extraction chromatography using
that radioactive contamination will be introduced into a TRU resin. For further purification of the Am fraction
sample with this equipment, except by cross-contamination (separation from rare earth elements), anion exchange
from a high radioactive sample. To prevent this, thorough chromatography is used. The final Sr separation and puri-
cleaning of equipment between samples is advisable. At this fication is performed by extraction chromatography using
stage, a portion may be taken for gamma ray spectrometry. Sr resin (Vajda et al., 1992; Moreno et al., 1997). The
If vegetation and organic debris are not discarded, the measurement of the 90Sr activity is performed by LSC us-
roots, mat, and vegetation should be cut into very fine ing a low-energy window, which includes the entire 90Sr
particles so as to be distributed evenly; if they are to be spectrum plus some tailing from any ingrown 90Y, and a
discarded, these materials should be collected and weighed. high-energy window chosen above the 90Sr maximum
Stones should be collected, weighed, and discarded. It can b-energy, which is used to measure 90Y to correct the 90Y
be assumed that the large rocks contain an insignificant tailing in the 90Sr window. The recovery factor for 90Sr
fraction of the activity and are in effect voids in the sample. (assuming a total isotopic exchange between the stable
This has been shown experimentally for plutonium (Krey strontium isotopes and the measurand 90Sr) is determined
and Hardy, 1970). The mass of the discarded material by gravimetry, and the calculation is based on a standard-
should be taken into account, but not in calculating the ized strontium carrier solution. The quantification is per-
specific activity of the soil. It provides, however, additional formed by isotope dilution alpha spectrometry using 242Pu
information to indicate the overall makeup of the growing or 236Pu and 243Am tracers.
area. In either case, the soil should be crushed, ground, or
pulverized to a particle size predetermined by the analytical b. Vegetation
requirements. The need for preparing the material will also Analysis of vegetation, such as grass and leaves, animal
depend on the nature of the soil; for example, beach sand feeds, especially forage and field corn, provides important
may not need grinding. In general, the soil should pass a data for determining radionuclide concentrations in food
Environmental radioactivity monitoring Chapter | 1 19

chains. Some materials have particular utility for identifi- space for the data from a number of sampling locations are
cation: Spanish moss on trees being a natural filter for gradual. For this reason, daily, weekly, or even monthly
airborne particles, ground mosses, and lichens integrating variations per sample location are not of radiological
radionuclide deposition over many years, and the leaves of significance.
perennial plants being useful for identifying nuclides The container or collector surface should be washed to
collected in a particular growing season. collect radionuclides that tend to adhere to surfaces or lined
The vegetation cover from at least 1 m2 of ground with a plastic sheet that is analyzed with the container
should be collected. The aim should be to obtain at least contents. Water may be funneled through a filter or ion
0.5 kg. Smaller samples may be collected whenever the exchange system for collecting some radionuclides. Dry
required radionuclide detection limit can be attained. Grass deposition is determined separately on material such as
should be cut at the appropriate height (1e5 cm) to obtain gummed paper or fibers that simulate grass. The same ra-
an estimate of what a grazing animal would consume by dionuclides are usually deposited in rain and collected with
simulating its grazing behavior. In drier climates or during airborne particles, but relative amounts depend on the
sparse growing seasons, it may be necessary to sample initial vertical distribution, particle sizes, and other
nearer to the soil surface. Care must be taken to prevent the characteristics.
cut material from being contaminated with soil. It should be Collectors intended to measure representative deposi-
recognized that samples of vegetation cut this way will not tion should be placed so as to avoid effects by local factors,
represent exactly what the grazing animal consumes. for example, air turbulence, shielding by buildings and
The vegetation may be analyzed in a fresh state, or if vegetation, and sources of dust, fumes, and moisture.
time permits and the loss of radioiodine is not of concern, it
may be dried. Generally, grass is dried at temperatures not 2. In situ gamma spectroscopy
exceeding 105 C for 24 hours. The dried matter should be
Introduced in the 1960s to determine natural background
ground so that all particles pass through a 2-mm sieve.
and weapons test fallout emitters in soil, the relevant
Samples must be weighed in a consistent manner so that the
gamma dose rate in the air above, and the relative contri-
concentrations can be compared among samples. Activity
on grass is reported on the basis of two weights (Bq/kg wet bution of the 238U and 232Th series and 40K to the dose rate
(Lowder et al., 1964a, 1964b; Beck, 1966; Beck et al.,
mass or Bq/kg dry mass) and area (Bq/m2); hence, sample
1964), in situ (i.e., field) spectrometry soon appeared as a
mass should be determined at collection and air-dried,
powerful tool to provide rapid and spatially representative
oven-dried, or ashed. There is general agreement that
estimates of environmental radioactivity. In essence, this
vegetation requires complete dissolution.
technique consists of the collection of gamma spectra using
If samples are collected to derive transfer coefficients or
a field-portable detector mounted on a tripod above the
to represent certain exposure pathways, sample selection
ground surface (typically 1 m) and subsequent elaboration
must be guided by factors such as growth patterns, wind
direction frequencies, soil types, and farming practices. The of the full absorption peak areas multiplied by ad hoc co-
efficients calculated according to two fundamental
amounts required for such analyses may refer to the entire
assumptions:
sample, to the edible part, or to the part that collects or
concentrates the radionuclides of interest. One should l The sourcedin this case the soildcan be modeled as an
consider the pathway of radionuclides to the analyzed infinite half-space (thus within the field of view of the
fractions, such as surface deposition, root uptake, and detector, the ground surface should be relatively flat
translocation from other parts of the plant. and free of any large obstacles, and the radionuclide ac-
tivities are assumed to be uniform within this zone).
c. Deposits l The vertical distribution of radionuclides can be
reasonably assumed to take account of attenuation by
Dry and wet depositions of radionuclides are measured to
the soil matrix (typically uniform distribution for natu-
follow the movement of radionuclides from air to terrestrial
ral radionuclides and exponential distribution for artifi-
and aquatic media. In principle, a collector with an open
cial ones).
surface ranging from 0.05 to 10 m2 accumulates dust or
precipitation for a specified time, and this material is Under these conditions, it is possible to use a standard
analyzed for radionuclide content. The materials used for point source calibration performed in the laboratory (Beck,
the collecting areas vary (stainless steel, plastic, polyester, 1972; Beck et al., 1972; Cutshall and Larsen, 1986; Miller
PVC). To obtain concentration as well as deposition values, and Shebell, 1995). The calibration based on the relation of
the amount of rainfall is measured after each collection. the absorption peak counting rate registered by the detector
Typical sampling periods range from daily, over weekly to (Nf) to the exposure rate in air (I) above the ground, or the
monthly. In normal circumstances, variations in time and concentration or inventory of a particular nuclide (A) is
20 Handbook of Radioactivity Analysis: Volume 2

Nf N0 Nf F Nf N0 Nf F obtained following two approaches: Monte Carlo simula-


¼ , , or ¼ , , tion and the use of algorithms aimed to the direct elabo-
I F N0 I A F N0 A
ration of spectra. A parametric calibration was elaborated,
where based on the efficiency and geometric dimensions of the
N/F is the counting rate from a particular spectrum ab- detector (Helfer and Miller, 1988). Another improvement
sorption peak due to a unit primary photon flux density was the introduction of a stripping method that subtracts
of energy E incident on the detector along the detector partial absorption and the contribution from cosmic ray
axis (normal to the detector face). events from a collected spectrum. An important step for the
Nf /N0 is the correction required to account for detector diffusion of this technique was the publication of ICRU
angular response, Report 53 (ICRU, 1994), which addressed the main aspects
F/I is the primary photon flux density with an energy E of in situ gamma spectroscopy.
at the detector resulting from the decay of a particular Hence, since the pioneering work of Beck et al. (1972),
radionuclide per unit exposure rate at the detector the use of in situ gamma spectrometry measurements has
from all primary and scattered photons originating become a well-established technique for documenting
from this nuclide and any others present from its radio- levels of environmental radioactivity in soils (e.g., Miller
active decay series. and Helfer, 1985; Helfer and Miller, 1988; Miller et al.,
F/A is the total photon flux density at the detector loca- 1994; Zombori et al., 1992; Lettner et al., 1996; Abelquist
tion per unit concentration or inventory of the nuclide. et al., 1996; Tyler et al., 1996), power reactor plumes
(Gogolak, 1984), forests (Gering et al., 2002; Plamboeck
The first two terms depend on the particular detector; F/ et al., 2006), urban areas (Medeiros and Yoshimura, 2005;
I and F/A values depend only on the source composition Clouvas et al., 2001, 2003; 2006; Svoukis and Tsertos,
and geometry and can be used for any spectrometer cali- 2007), large areas (Cresswell et al., 2006; Tyler, 2004;
bration. The factors are derived from g-ray transport cal- Guillot, 2001; Hendriks et al., 2001), indoor gamma dose
culations. Tabulations of these data along with other rate estimates (Miller, 1984; Miller and Beck, 1984;
pertinent information on the makeup of the environmental Clouvas et al., 1998, 2000), and building materials (Risica
g-radiation field can be found in Beck et al. (1972), Beck et al., 2001; Risica and Nuccetelli, 2001; Bochicchio et al.,
and de Planque (1968), and Beck (1972). A complete set of 2004).
exposure rate values (I/A) close to 200 common fission and
activation radionuclides at various exponential depth dis-
tributions in the soil can be found in Beck (1980). C. Water
With this calibration and the coefficients elaborated In addition to potential contamination with anthropogenic
following Beck’s method, the dose ratedproduced by the radionuclides, radium isotopes, 222Rn, several short-lived
unscattered and scattered fluence of gamma raysdcan be daughter products of radon, and finally, two longer-lived
estimated, and the radionuclide inventory calculated. decay products, 210Pb and 210Po, and to some extent ura-
Minimum detectable concentrations using a typical 25% nium are of some concern in natural waters. Due to its low
relative efficiency p-type germanium detector and a 10- solubility, thorium is not generally considered to be a major
minute count time at typical background radiation levels environmental hazard. Radiological water quality guide-
for 60Co, 137Cs, 152Eu, 226Ra (based on measurement of lines have been developed regionally (ANZECC/ARM-
progeny), and 228Ac (to infer 232Th) are all reported to be in CANZ, 2000; NHMRC, 2004; USEPA, 2000; EU, 1998)
the order of 1.8 Bq/kg (NRC, 1995). and globally (WHO, 2008; WHO, 2011) for potable, live-
The original method cannot be used for all kinds of stock, watering irrigation, and recreational uses.
source geometry, for example, indoors or urban outdoors, Sampling and preparation of water samples for analysis
because it is not feasible to elaborate the buildup factors or presents a number of problems not shared by other sample
produce calibration curves from which to derive the types and for which clearly defined answers are not avail-
radionuclide activity concentrations in the source. Further able. The problems are caused principally by two situa-
limitations of the technique are mainly associated with the tions: the samples are two-phase systems (i.e., the water
need of a priori assumptions about the distribution of nu- contains some insoluble material) and the sometimes un-
clides in the soil, an important source of uncertainties of predictable behavior of many substances at very low con-
activity concentration estimates and dose rate evaluations, centration. The variable composition of natural waters adds
since dose rate is obtained as a sum of different radionu- to the problem.
clide contributions to unscattered and scattered gamma flux Because a radioactive element of interest often is pre-
at the detector. sent in submicrogram quantities, a significant fraction may
Indoor and outdoor buildup factors and the estimate of no longer exhibit their expected ionic behavior and be lost
the actual radionuclide distribution in soil have been by adsorption on the surface of suspended particles or on
Environmental radioactivity monitoring Chapter | 1 21

the surface of containers used in the examination. Even an occur if finely divided species become fixed on the
ion as simple as cesium can be lost in trace amounts in glass container walls during counting. Such samples can be
containers by exchange with the potassium in the glass. filtered, evaporated, or acidified, if the suspended material
Radionuclides at low activities may also exhibit many is soluble in dilute acid.
properties of colloids, and the term “radiocolloid” has been For gross activity measurements applying gas flow
applied to such mixtures. For a discussion of radiocolloids, proportional counters, the water sample is dried by oven
in general, see Crouthamel and Heinrich (1971), Olofsson evaporation just below the boiling temperature or on a hot
et al. (1981, 1983), or Vilks and Bachinsk (1997). To plate. The sample should be less than 3 mg cm2 in
reduce the effect of radiocolloid adsorption, an appropriate thickness. The main error in this procedure is the loss of
amount of the corresponding nonlabeled compounds (car- particles, which might become airborne during the drying
rier) should be added to the system to lower the radio- process.
colloid formation by the chemical dilution of the Although there are a number of international standards
radioactivity (Keller, 1993). describing test methods for gross alpha and/or gross beta
To reduce the possibility of the loss of radionuclides on determination in water samples, for example, ISO 10704
the walls, the sample is usually acidified. Most environ- “Water qualitydGross alpha and gross beta activitydTest
mental water is close to neutral, and acidification to method using thin source deposit” (ISO 10704, 2018); ISO
0.1e0.5N is adequate. At this acidity, radioactive sub- 9696 “Water qualitydGross alpha activitydTest method
stances in particles in the sample can be leached (perhaps using thick source” (ISO 9696, 2017); ISO 9697 “Water
slowly) and appear in the solution, resulting in a consid- qualitydGross beta activitydTest method using thick
erable increase in the original soluble radioactivity. Also, source” (ISO 9697, 2018), the gross activity method is
iodine ions will slowly oxidize to iodine, and radioiodine in considered to be a screening procedure at best. For
solution may be lost by volatilization if nitric acid is used. example, Oural et al. (1988) have shown that gross-alpha
To prevent sorption of radionuclides on container walls activity can underestimate actual activity because of par-
between sampling and analysis, freezing may be a suitable tial volatilization of radon, short-lived radon daughters, and
method, but this is practical for small samples only, and the polonium during evaporation on the planchet. Until the
treatment of the insoluble portion still remains. If the short-lived radon daughters decay to a level supported by
sample has been stored before analysis, particularly at its radium in the water, a time-dependent alpha activity results,
natural acidity, it is advisable to transfer the sample to a which has little correspondence with actual water chemistry
second container with a solutiondusually an aciddin (Oural et al., 1987, 1989). Although nuclide-specific mea-
which the sought-for activity is soluble. The wash solution surements are preferable in environmental monitoring,
can be added to the original solution or analyzed separately. there are some attempts of gross counting applying LSC
The effectiveness of the washing procedure must be veri- (Happel et al., 2004; Kleinschmidt, 2004; Wisser et al.,
fied experimentally. 2006, Zapata-García et al., 2009), as it provides a rapid
So, it would appear that the safest pretreatment pro- screening method with the ability to give at least hints of
cedure, if the suspended and dissolved fractions are desired the radionuclide that has to be analyzed in the case of an
separately, is to filter the water through membrane filter unknown contamination.
paper while collecting the sample in the field and acidify Various methods have been described for the mea-
the sample immediately thereafter. The acid can be present surement of radium isotopes and 222Rn. Besides gamma
in the receiving flask during filtration. In this way, the water spectroscopy (e.g., ISO 13164-2, 2013; ISO 13165-3,
is not in contact with the container walls until after acidi- 2016), liquid scintillation techniques are most common.
fication. If this procedure is impractical, the sample should The classical reference method for radon in water mea-
be filtered as soon as possible after collection and the surements has used a radon bubbler and the Lucas cell.
sample acidified immediately prior to filtration. Any inac- Liquid scintillation techniques for 222Rn in water, first
tive carriers or radioactive tracers used in the analyses described by Prichard and Gesell (1977), have the advan-
should be added as soon as possible, preferably before tages of minimal sample preparation time, small sample
acidification, filtration, or evaporation. sizes, and automatic sample changing, with achievable
An efficient method for separating traces of actinide detection limits in the order of 0.37 Bq/L (Spaulding and
elements from solution introduced in the 1960s by Eakins Noakes, 1992), actually depending on the background,
and Gomm (1968) utilizes filtration through glass fiber counting time, and acceptable degree of uncertainty. LSC
paper at pH 5. Most actinides are absorbed almost instruments capable of alpha/beta discrimination are being
completely on the glass fibers, indicating that silica in so- used in the determination of radon and its daughters in
lution can adsorb many ions from solution. ground water and drinking water since the 1990s
A precaution observed in direct gamma spectrometry of (e.g., Schönhofer, 1989; Chalupnik and Lebecka, 1993;
water samples is the change in counting geometry that will Irlweck and Wallner, 1993; Prichard et al., 1991) as well as
22 Handbook of Radioactivity Analysis: Volume 2

in surface water (Salonen, 1993). A standard method based direct evaporation (Katzlberger et al., 2001) of large vol-
on a two-phase extraction to determine 222Rn in water umes is very time-consuming and susceptible to losses of
samples is given in ISO 13164-4 (2015), the detection limit polonium (Oural et al., 1988).
of which is 0.5 Bq/L at a measuring time of 1 hour and for a Therefore, coprecipitation with iron hydroxide followed
test sample of 10 mL. by a solvent extraction step with an extractant such as
Liquideliquid extraction, ion exchange chromatog- diisopropyl ether to remove Fe from the sample solution
raphy barium sulfate, and barium carbonate precipitation (Narita et al., 1989) or MnO2 (Carvalho, 1997; Martin and
are the usual separation techniques used for radium. Spe- Hancock, 2004) has commonly been used. Additional
cific extractants especially for use with alpha LSC, such as chemical purification using Sr resin (Vajda et al., 1997;
extractive scintillators (RADAEX) (McDowell and Miura et al., 2000; Vrecek et al., 2004) or various solvent
McDowell, 1994) or impregnated filter papers (Empore extractions prior to the final autodeposition of Po may be
Radium Rad Disks) (Smith et al., 1997) for radium, have applied.
been developed. The extractive scintillator consists of an Besides gamma spectroscopy of evaporated water
organic extractant solution, such as toluene, xylene, or samples, analysis of 210Pb in water samples can be based on
mesitylene solution of a high-molecular-weight neo- autodeposition of the Pb-210 decay product Bi-210 on
carboxylic acid together with the crown ether (dicyclo- nickel according to the electrochemical series of metals.
hexano-21-crown-7), used in a mole ration 2:1 combined Due to its electrochemical characteristic, Po-210 is
with a flour, PBBO, and naphthalene as energy transfer collected as well. The method consists of a chemical acid
agent. This extractant separates radium from barium, pulping, followed by a decay products buildup, the depo-
strontium, and calcium by factors of 9.3, 12, and 58, sition and the measurement of the 210Bi beta radiation. The
respectively (McDowell and McDowell, 1994). deposition from HCl is more smoothly and quantitative to
Analysis for 226Ra may involve inferring the radium HNO3 or H2SO4 (Figgis, 1961). In 1982, Richard J. Velten
activity from a measurement of the ingrown daughter, and Betty J. Jacobs developed a standard method for 210Pb
222
Rn (Parks and Tsuboi, 1978; Prichard et al., 1980; determination in drinking water (EPA, 1982) for LSC or
Cooper and Wilks, 1981; Horiuchi and Murakami, 1981; low background end window counting. The method con-
Nobrega et al., 1987; Chu and Khalique, 1990; Schönhofer sists of a precipitation as chromate, purification from 210Bi
et al., 1991), or applying pulse shape analysis to the by selected dissolution of lead sulfide from a hydrochloric
determination of 226Ra alpha particles (Cross and McBeth, acid solution (1.5 N), and conversion of lead to the
1976; Coombs, 1980; Noguchi et al., 1984; Burnett and carbonate.
Tai, 1992; Blackburn and Al-Masri, 1992; Saarinen and Activity concentrations in the range of less than
Suksi, 1992). 20 mBqe50 mBq/L can be achieved with measuring times
228
Ra determination may be based on counting 228Ac between 3 and 12 hours with the standard method of ISO
(Petrow et al., 1964; Nour et al., 2004, L’Annunziata and 13163, 2013 “Lead-210dTest method using liquid scin-
coworkers (see Aleissa et al., 2008)) or the 228Th alpha- tillation counting” (ISO 13163, 2013). The sample volume
emitting daughter, liquid scintillation betaegamma coin- needed for this method is 0.5e1.5 L.
cidence spectrometry, and 220Rn emanation (Orr, 1988), Tritium, produced during atmospheric thermonuclear
which is similar to 222Rn emanation techniques used for tests, is used as a global transient tracer for studying dy-
226
Ra. However, the latter approaches are limited by the namics in the hydrological cycle, recharge, renewal rate,
slow ingrowth of the 228Th (T1/2 ¼ 1.9 years). flow velocity, and in conjunction with radiocarbon to
A time-saving method for the measurement of 226Ra, determine groundwater age (Libby, 1953; Bergmann and
228
Ra, and 210Pb in drinking water by applying Empore Libby, 1957; Fontes, 1983; Günay, 2006; Lloyd, 1981;
Radium Rad Disks and low-level liquid scintillation spec- Sanchez-Cabeza and Pujol, 1999; Lehmann et al., 1993;
trometry has been developed by Schönhofer and Wallner Yurstsever, 1983; Wen et al., 2005, 2008; Borio et al.,
(2001). Radium is concentrated by filtration of the sample 2005).
through a membrane loaded with element-selective parti- Because natural levels of tritium are only marginally
cles. The extracted nuclides are eluted with 0.25 M alkaline measurable by direct b-counting methods, the water sam-
EDTA solution, which is then mixed with the LSC cocktail. ples are purified by distillation, followed by an isotopic
Lead is coextracted, and therefore, 210Pb interferes with enrichment procedure using electrolysis through direct
228
Ra to a certain extent. The collection efficiency for both current (Florkowski, 1963, 1992; Morgenstern et al., 1992).
lead and radium isotopes is about 100% (Schönhofer and After the neutralization procedure by addition of PbCl2, or
Wallner, 2001; Wallner, 2002). CO2, a new distillation is performed. Afterward, one
To determine low-level activity concentrations of 210Po aliquot of 8 mL is withdrawn to a scintillation vial with
in water samples, large volume samples (>1 L) have to be 12 mL of Ultima Gold LLT scintillation cocktail (Perki-
provided. The samples have to be preconcentrated since nElmer, Inc.) at a sample pH value ranging from 5 to 7.
Environmental radioactivity monitoring Chapter | 1 23

Tritium (and its daughter 3He) can also be measured uranium mills; the 90Sr titanate waste from a radioisotope
using mass spectrometry, but other dissolved gases (H2O, heat source is quite insoluble compared with most other
CO2, O2, N2, etc.) must be removed first (Faure, 1986; strontium wastes. Valuable information on the chemical
Clark and Fritz, 1997). composition of wastes, the behavior of radioelements, and
Due to the specific characteristics of tritium (gas, rela- the quantity of radioisotopes in use appears in the literature
tively easily oxidized to HTO), combined with omnipotent (e.g., Ghiloufi, 2009.)
presence of water vapor, the assay of low levels of tritium
requires consideration of various types of contamination, 2. Rain
the magnitude of which is depending strongly on specific
procedures of sample handling, on the ambient tritium The rainwater may be directly fed to a bottle or to an ion
exchange column where the nuclides are fixed. Measure-
concentrations during sampling, storage and analysis, and
ment of the activity in the collected rainwater and of the
the type of containers used to store the samples before the
amount of rainfall allows the calculation of the average
analysis. Sample contamination may originate from some
total deposition during the sampling period.
types of watches with fluorescent tritium dials, tritium
Contamination of rain water samples by airborne soil
sources used in gas chromatography, targets used in
and surface dust can be minimized by locating the sampling
neutron generators, or medical experiments where tritium is
stations on the roofs of buildings. Overhanging vegetation
used as a tracer (Okada and Momoshima, 1993).
Tritium activity concentration is commonly reported in should be avoided. The most suitable size for the collector
depends on the amount and frequency of precipitation in
Tritium Units (TU). The TU is the ratio of tritium atoms to
the area, as well as the frequency of collection. For areas
stable hydrogen-1 atoms or [3H]/[1H], prior to weapons
receiving 5e25 cm precipitation per month, a collecting
testing, and represents the number of tritium atoms per
area of 0.1e0.2 m2 is suggested. All materials in the col-
1$1018 hydrogen atoms. Hence, one TU is equivalent to
lector must be transferred with great care to ensure that all
0.118 Bq kg1 of water. With the electrolytic enrichment
the radioactive material is collected. The sides and bottom
technique, detection limits in the order of 0.1e0.01 TU
of the container should be scrubbed several times with a
(11.8e1.18 mBq/kg) are achievable. If detection limits in
the order of 10 Bq/kg (Bq/L) are to be achieved, distillation rubber spatula and rinsed with distilled water. If the con-
tainers are reused, care must be taken to avoid a buildup of
(probably multiple distillations) will suffice using low-level
contamination that will influence subsequent samples.
LSC instruments.

1. Wastewater 3. Groundwater
For most people, the source of water for domestic con-
Wastewater often contains larger amounts of nonradioac-
sumption and other uses is groundwater, often obtained
tive suspended and dissolved solids than water, and often,
from shallow, private wells, but more often obtained from
most of the radioactivity is in the solid phase. At the
sampling of radioactive industrial wastes or similar mate- public, community wells tapping the aquifer.
Besides possible contamination from effluent dis-
rials, the high possibility of deposition of radioactivity on
charges, groundwater is prone to naturally occurring ra-
surfaces of glassware, plastic containers, and equipment,
dionuclides. If valid judgments are to be made about the
which may cause a loss of radioactivity and possible
hazards and management of the radionuclides in ground
contamination of subsequent samples collected in inade-
water, it is necessary to understand the specific behavior of
quately cleansed containers, has to be considered.
these radionuclides in the aquifer chemical systems, and
Generally, the use of carriers in the analysis is inef-
that requires detailed knowledge of groundwater pH,
fective without prior conversion of the solid phase to the
soluble phase, since the radioelements may exhibit unusual reductioneoxidation potentials, with rock materials (Foss
and Brooker, 1991). Chemical reactions, such as ion ex-
chemical characteristics, because of the presence of com-
change, chemical complexing, and equilibration reactions
plexing agents or the method of waste production. For
with minerals and physical processes, such as alpha recoil
example, tritium may be combined in an organic compound
(Osmond and Cowart, 1976; Osmand et al., 1983, 1984),
when used in the manufacture of luminous articles; radio-
can cause considerable departures from decay equilibrium
iodine from hospitals may occur as complex organic
within the uranium decay series.
compounds, compared with elemental and iodide forms
Because of their greater mobility, uranium and 226Ra are
found in fission products from the processing of spent
nuclear fuels; uranium and thorium progeny often exist as usually depleted relative to 230Th on the surfaces of soil or rock
particles (e.g., minerals and particulate organics). 238U, 234U,
inorganic complexes rather than oxides after processing in
24 Handbook of Radioactivity Analysis: Volume 2

and 226Ra are, therefore, present in greater abundance in D. Foodstuff


ground water than 230Th. 222Rn enters water by alpha recoil
Samples of food are of greatest interest because their
and/or leaching and migrates. 210Po and 210Pb also migrate to a
analysis yields values of the radionuclide intake that
lesser extent and are in disequilibrium to other isotopes in the
contribute directly to dose. Foods that contribute 5% or
U-238 series (Upchurch et al., 1991).
more to the total diet intake should be collected for ana-
lyses. Food sampling should be undertaken first at the
4. Surface water
producer’s and subsequently at the retail market. In general,
Surface water comprises river, lake, or sea water and is one food products should be prepared as for home use, bearing
of the environmental compartments to which radioactive also in mind that like vegetation, all foodstuffs require
effluents from nuclear installations are authorized to be complete dissolution. Analysis of individual foodstuffs can
discharged. Radionuclides in surface waters can be found in indicate whether and which countermeasures should be
the water phase or associated with suspended particles and taken to reduce doses, whereas food sampling of mixed
can eventually become incorporated into sediments and diets provides an estimation of total uptake. If, however,
living species. Natural radionuclides in river water include mixed diet samples are to be used, a separate mixed diet of
3
H at levels of 0.02e0.1 Bq/L, 40K (0.04e2 Bq/L), radium, baby foods should also be analyzed.
radon, and their short-lived decay products (<0.4e2 Bq/L). Following an emergency, it is important that specific
The main fraction of 3H in surface water, however, is due to food types are continued to be monitored, particularly
human activities. foodstuffs coming from areas with high contamination and
Some of the sampling methods are automatic and those accumulating radionuclides of interest, such as ce-
continuous and are designed to give an early warning in case sium or strontium.
of an accidental release. In all cases, additional information
on the river flow rate is very important. Samples can be
taken continuously (or daily) and are then bulked into 1. Milk
monthly or quarterly analysis, or alternatively, spot samples Consumption of milk and dairy products has been shown to
are taken periodically and analyzed individually. The time be one of the most important pathways for uptake of ra-
and frequency of sampling is very important for rivers with dionuclides from environment to man, as milk is likely to
large differences in seasonal hydrological variations. be contaminated by radioactive iodine and cesium within
Treatment of the water may consist of filtration, the the first days after a release of volatile radionuclides. Milk
filtered water and the suspended material being measured can be collected from individual farms or from individual
separately, ion exchange and subsequent washing of the ion animals, raw milk at farms at processing centers, or bottled
exchange column, or evaporation (for direct measurement milk at the supermarket. It is, of course, essential to note the
of the residue). Chemical separations are needed for 90Sr, date of collection of the milk. At large processing centers,
whereas 3H is measured after multiple distillation or elec- milk is pooled from several sources with different collec-
trolytic enrichment. Usually, residual beta (total beta less tion days at the local farms. The date of processing should
40
K activity) contamination is reported, although there is a therefore be taken as the reference date for sampling.
clear tendency to perform nuclide-specific measurements Liquid milk must be preserved for long-time storage.
by means of gamma spectrometry and LSC. For periods of 1e2 weeks, milk is usually stored in a
refrigerator near the freezing point. Storage at frozen-food
5. Drinking water temperatures (about 15 C) is suitable for longer pe-
Drinking water is monitored because of its vital importance riods. A preservative, such as formalin or sodium azide
for human consumption, even though a severe radioactive (3.5 mL of 5% aq. solution per liter), can be added to
contamination of this medium is rather improbable. Sam- prevent souring if a longer period of storage is anticipated.
ples may be taken from ground or surface water supplies, Before gamma spectrometric analysis, the milk samples
from water distribution networks, mineral waters, etc. Spot are dried at low temperatures with stirring to avoid the
samples are taken a few times a year and analyzed indi- formation of a protein skin on the surface, by adding milk
vidually or samples are taken daily and bulked for monthly in small quantities to the container in which evaporation
or quarterly analysis. occurs so only a small quantity is being heated at any one
Sample treatment usually consists of sample evaporation time, by coagulating the protein before evaporation, by
for direct measurement of the concentrate or separation on heating the milk with rennin, or by freeze-drying. Chemical
ion exchange columns. More elaborate chemical separations separation is applied for the determination of 90Sr activity
are required for 90Sr determination, whereas 3H is generally and separation of the water phase with subsequent distil-
measured following multiple distillation of the sample. lation for the separation of 3H.
Environmental radioactivity monitoring Chapter | 1 25

In an emergency situation, the rapid analysis of 89Sr and Where the sample includes considerable water, it must be
90
Sr in milk is essential to protect humans from radiation weighed at uniform water content. Because radionuclide
exposure due to the intake of contaminated milk. Some concentrations in animal tissue tend to range widely, a
methods using ion exchange resins have been attempted for sufficient number of animals must be collected to define the
rapid determination of radiostrontium in milk to avoid the normal range of radionuclide concentrations.
usual process of drying, ashing, and acid leaching (Vaney Following an accidental release, meat becomes one of
et al., 1989; Baratta, 2000). Brun et al. (2003) summarized the main sources of radiocesium for humans. Contamination
rapid methods of radiostrontium analysis in milk, compared of meat is mainly the result of animal grazing, but contam-
several methods in terms of analysis time, and reported a inated drinking water might also be an important pathway,
procedure combining cation exchange resin, Sr-resin, oxa- while inhalation is not likely to be a significant pathway to
late, and BaCrO4 precipitations to be appropriate for the meat. Meat sampling should normally be done in such a way
analysis of 90Sr within 48 hours (2002). However, it was that the composite sample is representative of a large number
difficult to apply this method to milk samples containing of animals, although after heavy fallout, screening mea-
both 89Sr and 90Sr. surements of individual animals may be necessary.
There have been some efforts to measure 89Sr and 90Sr Another pathway for the uptake of radiocesium by man
simultaneously, such as using spectrum-unfolding methods following an accident constitutes contamination of fish,
(Hong et al., 2001), other full spectrum methods (Heilgeist, especially those from nutrient-deficient lakes. Obtaining a
2000), the three energy window approach (Eikenberg et al., representative sample from an area containing many lakes
2005), and the constrained optimization function in three may require some compromise since collection of samples
energy windows with MATLAB software (Chobola et al., from a large number of the lakes may be impracticable.
2006). All of these approaches tend to fail when the 89Sr/90Sr Ocean fish will not take up as much radiocesium as
activity ratio is reasonably high, since small variations in the freshwater fish, because of the dilution through the depth of
quenching level shifts the spectrum toward the low energy the ocean and the effective dilution associated with the high
region, leading to significant counting errors in the 90Sr potassium content in the water, but particulate-associated
energy region. Using two energy windows, Kim et al. (2009) radionuclides can be enriched to high levels.
reported relative bias due to spectrum shifting higher than In a detailed program, fish are collected by species; in a
20%, when the 89Sr/90Sr activity ratio exceeded 10. less detailed program, fish typical of categories such as
Cerenkov counting procedures for the determination of bottom feeders, insect eaters, and predators may be
89
Sr and 90Sr have been reported by Melin and Suomela collected. Again, numerous replicate samples are desirable
(1995), who applied an additional step to separate 90Y after because of the usual difficulty in knowing whether a fish
measuring 89Sr, and Heckel and Vogl (2009). Both caught at a location had lived there for an extended period.
methods only have been demonstrated for low 89Sr/90Sr Thus, the presence or absence of a radionuclide does not
activity ratios, which would be exceeded likely in samples permit any definite conclusion concerning the presence of
collected under emergency conditions. the radionuclide in water at that location. For some fish,
Kim et al. (2010) introduced a combined counting more specific information concerning their location may be
method using Cerenkov and liquid scintillation where the available; for example, dams, salinity gradients, and tem-
sample was sequentially measured in Cerenkov and scin- perature gradients can be effective barriers in their move-
tillation counting modes. 89Sr and 90Sr activities in milk ment. Besides their origin, fish are sorted per species and
samples of 89Sr/90Sr activity ratios as high as 35 could be size (Saxen, 1990).
measured within 1 day with less than 20% and 40% relative Shellfish such as clams or oysters, some species of mac-
biases, respectively. A review paper on the analytical roalgae, and other filter feeders quickly take up the contami-
methodologies for the determination of radiostrontium nants from the seawater and can also be used as biological
isotopes has been published by Vajda and Kim (2010). indicators, having the advantage of being relatively stationary.
The shells, meat, and, in some case, the fluid are analyzed
2. Meat and fish separately. However, shellfish being filter feeders contain
much sediment in the intestine. If this material is not also
Animals whose meat is consumed by the public can be separated, the results can be seriously misleading.
collected at the normal time of slaughter. It is strongly rec- The samples should be cleaned, and the edible portions
ommended that rare wildlife (e.g., endangered species) should should be retained for analyses. Masses are determined by
not be used in environmental sampling and measurement. subtracting the inedible portion from the total since loss of
The animal usually is dissected to separate the edible moisture from the edible portion during the time of prep-
portions of those tissues that are to a degree specific for aration may amount to a sizable fraction of the mass. For
radionuclides of interest. Unless the animal is very small, fish, poultry, and meat samples, the bones are easily
tissue from each animal is considered as a separate sample. separated after heating for 1 hour at 150 C. The mass of the
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133. Anansi seeks his Fortune. [Note]

Stanley Jones, Claremont, St. Ann.

Anansi was very poor and he went out to seek his fortune, but he had
no intention of working. He clad himself in a white gown. And he met a
woman. She said to him, “Who are you, sah? an’ whe’ you from?”—“I
am jus’ from heaven.” The woman said, “Did you see my husban’
dere?” He said, “Well, my dear woman, heaven is a large place; you will
have to tell me his name, for perhaps I never met him.” She said his
name was James Thomas. Anansi said, “Oh, he is a good friend of
mine! I know him well. He is a big boss up there and he’s carrying a
gang. But one trouble, he has no Sunday clo’es.” The woman ran away
and got what money she could together and gave it to Anansi to take to
her husband.

But he wasn’t satisfied with that amount; he wanted some more. He


went on a little further and saw a man giving a woman some money
and telling her to put it up for ‘rainy day’. After the man had left, Anansi
went up to the woman and told her he was “Mr. Rainy Day.” She said,
“Well, it’s you, sah? My husband been putting up money for you for ten
years now. He has quite a bag of it, and I’m so afraid of robbers I’m
glad you come!” So Anansi took the money and returned home and
lived contentedly for the rest of his days.

[Contents]
134. The Pannier-jar. [Note]

Vassel Edwards, Retirement, Cock-pit country.

There was a man at slave time had a wife, and the wife kept two other
men. The husband of that wife was working out. One night, one came
first and then the house-master came home. And they had a big jar
called a pannier-jar, and the wife took the man and put him into the
pannier-jar. Afterward the other man came [164]in, and when he saw the
house-master was frightened and he told the house-master he had
come to borrow the pannier-jar. The house-master told him he could
take it, and the woman helped him up with the pannier-jar. And when
he got part of the way, he said, “Poor me bwoy! if it wasn’t for this
pannier-jar, I would be dead tonight!” The other man in the pannier-jar
said, “Brar, same meself!” And he got frightened and heaved down the
pannier-jar, mashed it up and killed the man in there.

[Contents]
135. Anansi kills his Grandmother. [Note]

William Cooper, Mandeville.

Anansi an’ Tiger were travelling. Anansi kill him old grandmother, him
put him into a little hand-cart was shoving him t’ru de town. After him
catch to a shop jes’ like out here, de shop-keeper was a very hasty-
temper man; an’ went in de shop an’ call fe some whiskey an’ give it to
one of de shopkeeper carry it to his grandmother. An’ said he mus’ go
up to de han’-cart an’ call twice. An’ de ol’ lady did not hear. So Anansi
said to de shop-keeper him mus’ holla out to de ol’ lady; him sleeping.
So de ol’ lady didn’t hear, he fire de glass in de ol’ lady face, an’ de ol’
lady fell right over. Then the shop-keeper get so frighten he cry out to
Anansi, say Anansi mustn’t mek no alarm in de town; he will give him a
bushel of money to mek him keep quiet.

So dem was going along an’ borrow a quart can from Tiger an’ was
measuring dis money. Tiger said, “Where you get all dat money?”
Anansi say, “I kill my ol’ grandmother.” Tiger, him went home an’ kill his
grandmother an’ put her up in a little hand-cart an’ was goin’ along t’ru
de town hollerin’ out to all de people, “Who want a dead body to buy?”
So Anansi said to Tiger he shouldn’t do anyt’ing like dat; too foolish!

[Contents]
136. White Belly and Anansi. [Note]

Richard Morgan, Santa Cruz Mountains.

White Belly plant some peas. Hanansi come a White Belly yard and
say, “Brer White Belly, dem peas not fat an’ you know what you do? if
you want ’em to be fat, mek up little fire at de root.” Tomorrow morning
when White Belly were come, every peas dead!

White Belly is a carpenter. He mek a box. He mek bargain wid de


mudder; he say, “Ma, I gwine put you in dis ’ere box, [165]put some
money in de box; den I will holla out “Me mudder died!” White Belly put
de han’ ’pon de head, say, “Me mamma dead o-o-o!” Hanansi run
come. White Belly say, “Ma, what you have to give me? Let good an’
bad see!” De box turn up an’ t’row out all de money. Hanansi go back
home an’ say, “Ma, I wan’ a little water to wash me foot.” Mother carried
the water come. He dip him feet in dere, say, “Good Lord, ol’ lady, you
give cramp me!” Tek de mortar stick, lick ’im in de head. An’ cobb’e one
box an’ put his mudder in an’ call out, “Me mudder dead!” White belly
come. Hanansi said, “Ma, what you have to give me? Give me back
good an’ bad see!” De box raise up an’ ’tamp him down flat. So
Hanansi kill him ma, an’ White Belly mudder save.

[Contents]
137. Monkey hunts Anansi. [Note]

Richard Morgan, Santa Cruz Mountains.

Hanansi borrow Monkey money, so him tell Monkey fe come


Wednesday. When Monkey come, Hanansi knock in ’tomach, say,
“Broad enough you can knock, oh!” Monkey ketch him, beat him. Nex’
day when Monkey come he say, “Mudder Hanansi, whe’ you son?” Him
say, “Brer Monkey, fe you murder him yesterday, don’ know if you him
dead!” Monkey call one roos’ cock an’ cut de craw an’ tek out Hanansi
an’ beat him.

When him gone, Hanansi say, “Ma, you goin’ mek Brer Monkey kill me?
You know wha’ you do, Ma? Put on yo’ pot, dig de fire ashes, put me in
deh, mek up de fire, put on de pot. I will see if dat fellah, Monkey, wi’ fin’
me when him come!” Nobody knew Monkey was a Obeah man. When
Monkey come he say, “Mo’nin’, Mudder Hanansi; wha you son?”
Mudder Hanansi said, “Massa, dis two day you beat him, an’ don’ know
wha’ he do?” Monkey gwine a kitchen, tek off de pot an’ dig out de fire-
ashes an’ tek out Hanansi an’ beat him.

Anodder Obeah woman tell Mudder Hanansi said, “You gwine to let
Monkey kill yo’ son? Yo’ can twis’ rope?” De ol’ woman said, “No me
trade?” 1 She said, “Twis’ one rope. When you look out o’ one en’, you
see horse you t’ink o’ ants.” Put Hanansi upon it. When Monkey come,
Hanansi deh ’pon de rope. When Monkey go up ’pon de rope, holla till
Hanansi cut de rope. Me’while de rope cut, Monkey tumble down broke
hi’ neck. So Hanansi come down, clean up Monkey. [166]

1 It is my trade. ↑
[Contents]
138. Anansi and the Pig coming from Market. [Note]

Moses Hendricks, Mandeville.

Anansi took the job to sweep the market. After he swept the market and
got the pay, he bought a pig called ‘wee pig’. On his way home he had
to cross a stream. He couldn’t get the pig across. He wouldn’t carry it
himself and he wouldn’t pay anyone to assist him,—wanted free help.
So he saw a dog coming along. He said, “Br’er Dog, I beg you bite this
pig, make this pig jump over the river, make Anansi get home.”

Dog said no, couldn’t do it.

He saw a stick coming along, said, “Do, Br’er Stick, I beg you lick this
dog, make this dog bite this pig, make this pig jump over this river,
make Anansi get home.”

Stick said no, couldn’t do it.

He see Fire, say, “Do, me good Fire, burn this stick, make this stick lick
this dog, make this dog bite this pig, make this pig jump over this river,
make Anansi get home.”

Fire says no.

He sees Water. “Do, me good Water, I beg you out this fire, make this
fire burn this stick, make this stick lick this dog, make this dog bite this
pig, make this pig jump over the river, make Anansi get home.”

Water said no.

He saw a cow coming. “Do, Br’er Cow, drink this Water, make this
water out this fire, make this fire burn this stick, make this stick lick this
dog, make this dog bite this pig, make this pig jump over this river,
make Anansi get to go home.”

Cow said no.

He saw a butcher coming. “Do, me good butcher, I beg you butcher this
cow, make this cow drink this water, make this water out this fire, make
this fire burn this stick, make this stick lick this dog, make this dog bite
this pig, make this pig jump over this river, make Anansi get home!”

Butcher said no, wouldn’t do it.

He sees Rope coming along. “Do, Br’er Rope, I beg you hang this
butcher, make this butcher kill this cow, make this cow drink this water,
make this water out this fire, make this fire burn this stick, make this
stick lick this dog, make this dog bite this pig, make this pig jump over
the river, make Anansi get home!”

Rope said no.

Saw Grease coming along. “Do, me good Grease, grease this rope,
make this rope hang this butcher, make this butcher kill this [167]cow,
make this cow drink this water, make this water out this fire, make this
fire burn this stick, make this stick lick this dog, make this dog bite this
pig, make this pig jump over the river, make Anansi get home!”

Grease said no.

He saw a Rat. Said, “Do, me good Rat, gnaw this grease, make this
grease grease this rope, make this rope hang this butcher, make this
butcher kill this cow, make this cow drink this water, make this water out
this fire, make this fire burn this stick, make this stick lick this dog, make
this dog bite this pig, make this pig jump over this river, make Anansi
get home!”

Rat says no.


Saw Puss coming along. “Do, Br’er Puss, I beg you kill this rat, make
this rat gnaw this grease, make this grease grease this rope, make this
rope hang this butcher, make this butcher kill this cow, make this cow
drink this water, make this water out this fire, make this fire burn this
stick, make this stick lick this dog, make this dog bite this pig, make this
pig jump over this river, make Anansi get home!”

Puss says, “Yes, I will kill your rat!”

Rat says, “Before you kill me, I will gnaw the grease!”

Grease says, “Before you gnaw me, I will grease the rope!”

Rope says, “Before you grease me, I will hang the butcher!”

Butcher says, “Before you hang me, I will kill the cow!”

Cow says, “Before you kill me, I will drink the water!”

Water says, “Before you drink me, I will out the fire!”

Fire says, “Before you out me, I will burn the stick!”

Stick says, “Before you burn me, I will lick the dog!”

Dog says, “Before you lick me, I will bite the pig!”

Pig says, “Before you bite me, I will jump over the river!”

So away went the pig over the river; and him and Anansi went home
safe and without expense.
[169]
DANCE AND SONG.

[Contents]
139. The Fifer. [Note]

Richard Roe, Maroon Town, Cock-pit country.

There’s a boy once, mother got only the one boy an’ ’he love him so
much that ’he give him a flute. So one day they go to far groun’ an’
coming back the boy leave the flute at the groun’. When he catch half-
way, he remember it an’ he tell him papa. Papa say to go back for it, but
he mus’ be careful not to blow it coming back because he got a lot of
wil’ beasts to pass. So as he come home he begin to blow, 1

[MP3 ↗️ | MusicXML ↗️]

♩ = 72

Minnie, Minnie, wa-yo da Lim-ba, Minnie, Minnie, wa-yo da Lim-ba.


Minnie, Minnie, wa-yo da Lim-ba, Minnie, Minnie, wa-yo da Lim-ba.

Wild beast rush out, say, “Who’s dat blowing de pipe, sah?”—“Oh, no,
not me blowing!” An’ go ’way, blow again. Wil’ beast rush out. “Ha!
you?”—“No, grandpapa, not me blowing!”—“Den who blowing?”—“He
gone on befo’, massa; not me blowing!”—“Blow, let me see.”—“Flee
flitty flee, flee flitty flee.”
Wil’ beast go away. He commence the right tune now,

“Minnie Minnie, wa-yo da lim-ba,


Minnie Minnie, wa-yo da lim-ba,
Minnie Minnie, wa-yo da lim-ba.”

(Wild beast rush out, catch him, compel him to play.)

“Ah, I catch you now, sah! Play de tune now, sah! blow, sah!”

Then he began to blow the right tune, both dance. Different [170]wil’
beasts—Tiger, Asoonah, all the wil’ beasts come out an’ dance. An’ the
father get frightened, come shoot all the wild beasts, all drop save him
boy. An’ flog the boy.

1 The song was sung by Alfred Williams. ↑

[Contents]
140. In Come Murray.

William Forbes, Dry River, Cock-pit country.

It was said when you go you see a man going to play dat Nansi story.
Get anodder wid a pint a water, den him gwine to turn a drunkard,
begin to totter, say, “Tiger, tiger, lie down”—

[MP3 ↗️ | MusicXML ↗️]

♩ = 84

Zin come Murray. I take drink, lay down, Zin come Murray.
Murray, ah, lay down, Zin come Murray. I take drink lay down,
Zin come Murray. Oh, poor Murray. Zin come Murray.
I take drink, lay down, Zin come Murray.
[Contents]
141. Tacoomah makes a Dance. [Note]

William Forbes, Dry River, Cock-pit country.

Tacoomah make a dance, get Anansi for de fiddler, an’ Grass-quit was
coming as a fiddler too. Robin Redbreast was to play de music,
Monkey was to blow de bugle. Well, after de night de dance
commence. Anansi gwine to play,

“Queena bunna, ring-ki-ting,


You sen’ fe great Grass-quit,
You don’ sen’ fe me!
Anansi draw bow so sweet, ring-ki-ting,
Anansi draw bow so sweet, ring-ki-ting.”

Tacoomah say,

“You ya, you ya, so ya, me ya,


Wid a fort tumba like a tenky bunna,
Wid a jump, wid a jump, like a tenky bunna.” 1

[171]

Robin Redbreast say,

“Jock, Jock, when you coming home?”

Jock said,

“Tomorrow evening.”
“What in your right?”
“Boot an’ spur.”
“What in your left?”
“Bow an’ arrow. 2”
Jock 3 said,

“Robin redbreast
Was pretty well dressed,
And he was into his nest,
And a puppy went into his nest
And broke his neck t’ru distress.”

Well, den, Turtle an’ Duck goin’ in de river fe go an’ swim, an’ dem is to
run to a hill-side in de river. An’ Cock is de judge. Den Cock went to
sing fe dem—

“Co co re co.”

Duck an’ Turtle swim—

“Shekey, shekey, shee-e-e.”

1 The tune is that of the Devil in the Cock and Corn story, number 85. ↑
2 The dialogue is taken from a popular game. ↑
3 I asked, “Who is Jock?”—“Jock man dora.” ↑

[Contents]
142. Anansi makes a Dance. [Note]

William Forbes, Dry River, Cock-pit country.

Again, Anansi make a dance. Him playing de fiddle,


[MP3 ↗️ | MusicXML ↗️]

♩ = 84

Kelly bam bom ba, Kelly bam ya Morree! Kelly bam bom ba, Kelly
bam ya Morree! Kelly bam bom ba, Kelly bam ya Morree!
Dem dat kyan’ run, dey no hearie! etc. 1

Kelly bam bom ba, Kelly bam ya Morree! Kelly bam bom ba, Kelly
bam bom ba, Kelly bam bom ba, Kelly bam ya Morree! Kelly[172]
bam bom ba, Kelly bam bom ba, Kelly bam ya Morree! Kelly
bam bom ba, Kelly bam bom ba, Kelly bam bom ba, Kelly
bam ya Morree! — — — — — — — — — —

Goat dere a dance, say,

“Me kyan’ run, but me cunnie do!”

Dog begin to sing,

“Na way you lie, Samedy,


Pussy no dead at all!”

Den Puss an’ Rat begin to dance an’ say,

“Massa Puss an’ Massa Rat a jump shandelay, 2


[MP3 ↗️ | MusicXML ↗️]

♩ = 160

Oh, jump shandelay, jump shandelay, den a jump shandelay.


Oh, oh, jump shandelay—Missa Rat a jump den a jump shandelay!
Oh, oh, jump shandelay. Jump shandelay, will you jump shandelay!
Oh, oh, jump shandelay, oh, Missa Rat a jump, will you jump, shandelay!
Den she went an’ jump it, den she went an’ jump it, den she went an’ jump it,
den she went an’ jump it, den she went an’ jump it, den she went an’ jump it.

Well, Anansi boy was blowing de fife,

“Ti-li-harry-ham, handsome ben-in-ben!”

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