Table Of ContentThermally and Optically Stimulated
Luminescence
Thermally and Optically Stimulated Luminescence: A Simulation Approach, First Edition. Reuven Chen and Vasilis Pagonis.
© 2011 John Wiley & Sons, Ltd. Published 2011 by John Wiley & Sons, Ltd. ISBN: 978-0-470-74927-2
Thermally and Optically
Stimulated
Luminescence
A Simulation Approach
REUVEN CHEN
Raymond and Beverly Sackler School of Physics and Astronomy,
Tel Aviv University, Tel Aviv, Israel
VASILIS PAGONIS
McDaniel College, Westminster, MD, USA
Thiseditionfirstpublished2011
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LibraryofCongressCataloging-in-PublicationData
Chen,R.(Reuven)
Thermallyandopticallystimulatedluminescence:asimulationapproach/ReuvenChenandVasilisPagonis.
p. cm.
Includesbibliographicalreferencesandindex.
ISBN978-0-470-74927-2(hardback)
1. Thermoluminescence.2. Thermoluminescencedosimetry.3. Opticallystimulatedluminescencedating.
I.Pagonis,Vasilis.II.Title.
QC479.C472011
612(cid:2).014480287–dc22
2010053722
AcataloguerecordforthisbookisavailablefromtheBritishLibrary.
PrintISBN: 9780470749272
ePDFISBN: 9781119993773
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eMobi: 9781119995777
Setin10/12ptTimesRomanbyThomsonDigital,Noida,India
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FrontcoverimagecourtesyofHerbYeates,http://superfluorescence.com/.Copyright(2007)withpermission.
Contents
AbouttheAuthors ix
Preface xi
Acknowledgements xiii
1 Introduction 1
1.1 ThePhysicalMechanismofTLandOSLPhenomena 1
1.2 HistoricalDevelopmentofTLandOSLDosimetry 2
1.3 HistoricalDevelopmentofLuminescenceModels 5
2 TheoreticalBasisofLuminescencePhenomena 7
2.1 EnergyBandsandEnergyLevelsinCrystals 7
2.2 TrappingParametersAssociatedwithImpuritiesinCrystals 9
2.3 CaptureRateConstants 10
2.4 ThermalEquilibrium 12
2.5 DetailedBalance 14
2.6 ArrheniusModel 15
2.7 RateEquationsintheTheoryofLuminescence 18
2.8 RadiativeEmissionandAbsorption 19
2.9 MechanismsofThermalQuenchinginDosimetricMaterials 20
2.10 AKineticModelfortheMott–SeitzMechanisminQuartz 23
2.11 TheThermalQuenchingModelforAluminabyNikiforovetal. 26
3 BasicExperimentalMeasurements 29
3.1 GeneralApproachtoTLandOSLPhenomena 29
3.2 ExcitationSpectra 32
3.3 EmissionSpectra 34
3.4 BleachingofTLandOSL 35
4 Thermoluminescence:TheEquationsGoverningaTLPeak 39
4.1 GoverningEquations 39
4.2 OneTrap-OneRecombinationCenter(OTOR)Model 44
4.3 General-orderKinetics 45
4.4 Mixed-orderKinetics 47
4.5 QandP Functions 51
4.6 LocalizedTransitions 55
4.7 SemilocalizedTransition(SLT)ModelsofTL 57
vi Contents
5 BasicMethodsforEvaluatingTrappingParameters 63
5.1 TheInitial-riseMethod 63
5.2 Peak-shapeMethods 65
5.3 MethodsofVariousHeatingRates 66
5.4 CurveFitting 69
5.5 DevelopingEquationsforEvaluatingGlowParameters 71
5.6 ThePhotoionizationCrossSection 73
6 AdditionalPhenomenaAssociatedwithTL 79
6.1 PhosphorescenceDecay 79
6.2 IsothermalDecayofTLPeaks 81
6.3 AnomalousFadingandAnomalousTrappingParametersofTL 82
6.4 CompetitionBetweenExcitationandBleachingofTL 94
6.5 AModelforMid-termFadinginTLDating;ContinuumofTraps 100
6.6 Photo-transferredThermoluminescence(PTTL) 109
6.7 TLResponseofAl O :CtoUVIllumination 116
2 3
6.8 DependenceoftheTLExcitationonAbsorptionCoefficient 118
6.9 TLVersusImpurityConcentration;ConcentrationQuenching 121
6.10 CreationandStabilizationofTLTrapsDuringIrradiation 129
6.11 DuplicitousTLPeakduetoReleaseofElectronsandHoles 131
6.12 SimulationsoftheDuplicitousTLPeak 140
7 OpticallyStimulatedLuminescence(OSL) 143
7.1 BasicConceptsofOSL 143
7.2 DoseDependenceofOSL;BasicConsiderations 144
7.3 NumericalResultsofOSLDoseDependence 146
7.4 SimulationoftheDose-rateDependenceofOSL 148
7.5 TheRoleofRetrappingintheDoseDependenceofPOSL 150
7.6 Linear-modulationOSL(LM-OSL) 153
7.7 UnifiedPresentationofTL,PhosphorescenceandLM-OSL 156
7.8 TheNewPresentationofLM-OSLWithintheOTORModel 158
7.9 TL-likePresentationofCW-OSLintheOTORModel 168
7.10 DependenceofLuminescenceonInitialOccupancy;OTORModel 169
7.11 TLExpressionWithintheUnifiedPresentation 171
7.12 PseudoLM-OSLandOSLSignalsunderVarious
StimulationModes 173
7.13 OSLDecayandStretched-exponentialBehavior 174
7.14 OpticallyStimulatedExoelectronEmission 180
7.15 SimulationsofOSLPulsedAnnealingTechniques 186
8 AnalyticalandApproximateExpressionsofDoseDependence
ofTLandOSL 193
8.1 GeneralConsiderations 193
8.2 CompetitionDuringExcitation 196
8.3 CompetitionDuringHeating 198
8.4 ThePredose(Sensitization)Effect 205
Contents vii
8.5 SensitizationandDe-sensitizationinQuartz 207
8.6 Dose-rateDependence 210
8.7 SublinearDoseDependenceofTLandLM-OSLinthe
OTORSystem 211
8.8 Dose-dependenceandDose-rateBehaviorsbySimulations 222
8.9 SimulationsoftheDose-rateEffectofTL 225
8.10 NonmonotonicDoseDependenceofTLandOSL 229
8.11 NonmonotonicDoseDependenceofTL;Simulations 231
8.12 NonmonotonicEffectofOSL;ResultsofSimulations 239
9 SimulationsofTLandOSLinDatingProcedures 245
9.1 ThePredoseEffectinQuartz 245
9.2 SimulationofThermalActivationCharacteristicsinQuartz 247
9.3 TheBaileyModelforQuartz 256
9.4 SimulationofthePredoseDatingTechnique 261
9.5 TheSingleAliquotRegenerativeDose(SAR)Technique 266
9.6 ThermallyTransferredOSL(TT-OSL) 272
10 AdvancedMethodsforEvaluatingTrappingParameters 279
10.1 Deconvolution 279
10.2 Monte-CarloMethods 282
10.3 GeneticAlgorithms 287
10.4 ApplicationofDifferentialEvolutiontoFittingOSLCurves 291
11 SimultaneousTLandOtherTypesofMeasurements 297
11.1 SimultaneousTLandTSCMeasurements;ExperimentalResults 297
11.2 TheoreticalConsiderations 301
11.3 NumericalAnalysisofSimultaneousTL-TSCMeasurements 310
11.4 ThermoluminescenceandOpticalAbsorption 313
11.5 SimultaneousMeasurementsofTLandESR(EPR) 318
11.6 SimultaneousMeasurementsofTLandTSEE 323
12 ApplicationsinMedicalPhysics 327
12.1 Introduction 327
12.2 ApplicationsofLuminescenceDetectorsinMedicalPhysics 328
12.3 Examplesofin-vivoDosimetricApplications 332
12.4 Radioluminescence 334
13 Radiophotoluminescence 341
13.1 DevelopmentandUseofRPLMaterials 341
13.2 TheSimplestRPLModel 344
14 EffectsofIonizationDensityonTLresponse 347
14.1 ModelingTLSupralinearityduetoHeavyChargedParticles 347
14.2 DefectInteractionModel 351
14.3 TheUnifiedInteractionModel 352
viii Contents
15 TheExponentialIntegral 357
15.1 TheIntegralinTLTheory 357
15.2 AsymptoticSeries 358
15.3 OtherMethods 362
PreviousBooksandReviewPapers 363
AppendixA Examples 365
A.1 SimulationofOSLExperimentsUsingtheOTORModel 365
A.2 SimulationofOSLExperimentsUsingtheIMTSModel 366
A.3 SimulationofTLExperimentUsingtheBaileyModel 369
References 371
AuthorIndex 395
SubjectIndex 411
About the Authors
ReuvenChen
ProfessorReuvenChenisaProfessorEmeritusatTelAvivUniversity.Hehasbeenworking
onthermoluminescence,opticallystimulatedluminescenceandotherrelatedtopicsoverthe
last 48 years. Professor Chen has published approximately 170 scientific papers and two
books. He has been a Visiting Professor at several universities in the USA, UK, Canada,
Australia,Brazil,FranceandHongKong.Atpresent,heisanAssociateEditorofRadiation
Measurementsandrefereeforseveralinternationaljournals.
VasilisPagonis
Professor Vasilis Pagonis is a Professor of Physics at McDaniel College. His research
involves working on modeling properties of dosimetric materials and their applications
inluminescencedatingandradiationdosimetry.ProfessorPagonishaspublishedapprox-
imately 70 scientific papers, as well as the book Numerical and Practical Exercises in
Thermoluminescence, published in 2006. He currently holds the Kopp endowed chair
inthephysicalsciencesatMcDanielCollege.
Preface
Thermoluminescence (TL) and optically stimulated luminescence (OSL) are two of the
mostimportanttechniquesusedinradiationdosimetry.Hundredsofpapersarepublished
every year in the scientific literature on different aspects of TL and OSL. These cover a
wholespectrumofsubjects,fromexperimentalpapersdescribingvariousaspectsofthese
phenomenaindifferentmaterialsunderdifferentexperimentalconditions,manytimeshav-
inginmindthepotentialapplications,topublicationsinterestedonlyinthedatesreached
bythesemethodsandtopublicationsondosimetrymeasurementsindifferentenvironments
(e.g.,inspaceships).Ontheothersideofthespectrum,onecanfindworkonthephysical
basisofTLandOSL,inwhichresearcherstrytoobtainbetterunderstandingoftheunder-
lyingprocesses.Theseincludethedosedependenceoftheeffects(whichmaybelinearor
nonlinear),possibledose-ratedependence,thestabilityoftheeffectsatambienttemperature
(whichmayincludenormalandanomalousfading),thedependenceoftheseeffectsonthe
relevantdefectsandimpurities,andthenatureoftheemissionspectrum.
ThetheoreticalworkonTLandOSLconsists,inmostcases,ofthestudyofthesimultane-
ousdifferentialrateequationsgoverningthetransitionsofchargecarriers,usuallyelectrons
and holes, between the different trapping states associated with impurities and defects in
thestudiedsample,andtheconductionandvalencebands.Theseequationsarenotlinear
andtherefore,inmostcases,cannotbesolvedanalytically.Inmanycases,approximations
concerningthetrappingparametersandfunctionsaremadetoreducethecomplication,and
explicitequationsforsimplifiedmodelssuchasthefirst-andsecond-orderkineticscanbe
written and solved analytically. Here, general solutions are reached from which one can
considerhowdifferentphenomenamaytakeplace,e.g.howthesignalfadeswithtimeat
room temperature under first- or second-order kinetics, and to what extent these predic-
tions agree with specific luminescence experiments for a given material. Obviously, this
approachhasastronglimitationsinceonedoesnotknowwhethertheassumptionsmade
holdallalongthetemperatureandtimerangeofaTL/OSLmeasurement.
Thisbookconcentratesonanalternativeapproach,inwhichwesimulatevariousexper-
imental situations by numerically solving the relevant coupled differential equations for
chosensetsofparameters.Usingthisapproach,severalcomplexsituationscanbedemon-
strated such as superlinear and nonmonotonic dose dependencies, dose-rate effects, the
occurrence of abnormally high frequency factors and others. Obviously, the shortcoming
ofthisapproachisthatitdoesnotprovideuswithgeneralsolutionsbutratherwithresults
associatedwithspecificsetsoftrappingparameters.However,thiskindofdemonstration
that certain behaviors are commensurate with our understanding of the underlying pro-
cesses is of great importance. With the present availability of strong computing power
andadvancednumericalmethods,thisapproachhasbecomeverypopularduringthepast
20years.Asecondapproachthatisemphasizedthroughoutthisbookisdemonstratingthe
possibilityofobtaininganalyticalsolutionsofthesystemsofdifferentialequationsbyusing
thequasi-equilibriumapproximation.Numerousexamplesaregiveninwhichthisapproach
xii Preface
leadstoexactanalyticalsolutionswhichdescribeaccuratelytheexperimentalresults.This
book is designed for practitioners, researchers and graduate students in the field of radi-
ation dosimetry. It is a synthesis of the major developments in modeling and numerical
simulationsofthermallyandopticallystimulatedprocessesduringthepast50years.
Chapter1ismostlyahistoricaloverviewofthedevelopmentsinTLandOSLdosimetry
duringthepast50years,followedinChapter2byanoverviewofthetheoreticalbasisand
severalquantumaspectsofluminescencephenomena,whichisbasedontheenergy-band
modelofsolids.Chapter3dealswithanumberofbasicexperimentalmeasurementsrelevant
tothestudyofTLandOSL.InChapter4wepresentthebasickineticequationsgovern-
ing the TL process, including simple kinetic models based on first- second- general- and
mixed-orderkinetics.Inaddition,someaspectsoflocalizedversusdelocalizedelectronic
transitionsduringtheluminescenceprocessarediscussed.Thebasicmethodsofevaluat-
ing kinetic parameters in TL and OSL experiments are the main topic of Chapter 5, and
Chapter6addressesavarietyofphysicalphenomenacommonlyencounteredduringTLand
OSLmeasurements.ThebasictheoreticalaspectsandexperimentaltechniquesusedinOSL
dosimetryarepresentedinChapter7,withaspecificemphasisontherelationshipbetween
thevariousmodelsusedinobtainingOSLdata(LM-OSL,CW-OSL,pseudoLM-OSL,etc.).
Chapter8addressesatopicofprimeimportanceforradiationdosimetryresearchers,namely
thedosedependenceofTL/OSLsignals.Differenttypesofexperimentallyobserveddose
behaviors are examined using both an analytical approach and approximate expressions
obtained using certain approximations. The topic of TL and OSL simulations for dating
applicationsispresentedinChapter9,includingsimulationsofrecentmajordevelopments
in TL/OSL dating protocols. Chapter 10 examines the use of several alternative methods
forevaluatingtrappingparameters,basedonavarietyofadvancednumericalmethodslike
Monte-Carlo techniques, genetic algorithms and advanced curve-fitting methods. Chap-
ter 11 contains a more general approach to thermally stimulated phenomena, and several
methodsofanalyzingsimultaneousthermalmeasurementsarepresented.Theprocessesof
thermallystimulatedconductivity(TSC),thermallystimulatedelectronemission(TSEE),
optical absorption (OA) and electron spin resonance (ESR) are briefly discussed, in par-
ticular in cases where their simultaneous measurements with TL can produce additional
informationandcanbesimulatedalongwiththesimulationofTL.Chapter12dealswith
applicationsofluminescenceinmedicalphysicsandChapter13withtheassociatedphe-
nomenon of radiophotoluminescence. Chapter 14 summarizes theoretical developments
andsimulationresultsontheeffectsofionizationdensityonTLresponse,whichisatopic
ofmajorinterestinradiationdosimetryforparticlesofvaryingionizationdensity.Finally
Chapter15presentsvariousnumericalapproachestotheexponentialintegralwhichappears
commonlyinTLapplications.Inadditiontothecomprehensivelistofreferences,covering
all the subjects discussed in the book, we have also included a list of books and review
articlespublishedintheliteraturefrom1968onwards.Finally,inAppendixA,wepresent
somesimpleexamplesofcomputercodethatsimulatethreeimportantmodelswhichappear
frequentlyinthebook,namely,theonetrap-onerecombinationcenter(OTOR)model,the
interactivemultipletrapsystem(IMTS),andthewidelyusedBaileymodelforquartz.
