Self-attenuation

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Self-attenuationMarie-Christine LépyLaboratoire National Henri Becquerel - LNE / CEA-DRT-LISTCEA Saclay – F-91191 GIF-SUR-YVETTE Cedex - FRANCEE-mail : marie-christine.lepy@cea.fr

Self-attenuation Introduction Attenuation coefficients Self-attenuation– Simple analytical formula– Generalisation– Practical tools Examples

Introduction Emission of photons attenuated through thesample If sample different from the calibration (size,shape, density, chemical composition)– Reduction of the photon beam– « False » peak areas– Correction factor required to get the true activity Homogeneity ?

Calibration sources

Attenuation coefficients Definition – Beer-Lambert law Tables Experimental measurement

Attenuation coefficientsBeer-Lamber law : attenuation of a narrow parallell photon beamµ ρxI(x) I0 e µx I0 e ρAbsorbingmaterialMonochromaticphoton sourceI0Ixρ density (g.cm-3)µ total linear attenuation coefficient of material i for enegy E (cm-1)ρ x mass thickness (g.cm-2)µ / ρ mass attenuation coefficient (cm2.g-1)µ depends on E and ZDetector

Attenuation coefficients (2)Practical parameter : attenuation coefficientPartial interaction coefficients:Photoelectric absorption:Compton scattering:Pair production effect:τi(E)σi(E)κi(E)τ const. Z4.5 E 3(major at low energies)σ const Z E 1κ const Z2(only if E 1022 keV)Linear attenuationcoefficient (cm-1)Mass attenuationcoefficient (cm2.g-1)Photoelectricττ/ρComptonσσ/ρPair productionκκ/ρµ τ σ κµ/ρ τ/ρ σ/ρ κ/ρInteractionTotalDepend on the energy, E, and the material (Z)For practical use : tables function of Z and ETables : cross sections (1 barn 10-24 cm2) or mass attenuation (cm2.g-1)

Attenuation coefficients (3)Photoelectric absorption coefficient sum of photoelectric effect ineach electronic shell (subshells):τ τΚ (τ L1 τ L2 τ L3 ) (τ M1 τ M2 τ M3 τ M4 τ M5 ) .If E binding energy of shell i, τ i 0For E Ei : absorption discontinuity: maximum ionisation probability in shell iτ variation versus the energy shows discontinuities corresponding to binding energies ofelectrons shells and subshells K, L, M.Ln(τ)Since µ τ σ κµ has the same discontinuities, function ofthe material atomic structure (Z)Ln(E)

Germanium mass attenuation coefficientAttenuation coefficients (4)Ge bindingenergies :L1: 1.4143L2: 1.2478L3: 1.2167K: 11.1031

Lead mass attenuation coefficientAttenuation coefficients (5)Pb bindingenergies :M1: 3.8507M2: 3.5542M3: 3.0664M4: 2.5856M5: 2.4840L1: 15.8608L2: 15.2000L3: 13.0352K: 88.0045

Mass attenuation coefficients Composition known - calculation Composition unknown - measurement Calculation: Attenuation coefficient table– XCOM (NIST Database)– Example for HCl 1N

XCOM : mixture Defining the mass fraction of each compound for HCl 1N: Matrix : HCl 1N 1 mole of HCl in 1 liter of solution HCl 1N density 1.016 (1L 1016 g) Mass of one HCl mole 1 35.45 36.45 g Resulting input parameters for XCOM Compound 1: HCl Mass fraction: 36.45 Compound 2: H2O Mass fraction 1016 – 36.45 979.55

xcom1.html

XCOM input-output

XCOM Results

Experimental measurementPrinciple : Use the unknown matrix and a collimated photon beamPhotonbeamPb ntainerN1(E)N2(E)Two successive measurements- Empty container- Container filled with unknown matrix with thickness x

Experimental measurementPhotonbeamPb collimatorsFor each energy:N2(E) N1(E) . exp (-µ(E) . nerN1(E)1 N 2 (E ) µ ( E ) ln x N1 ( E ) N2(E)Associated relative uncertainty:u 2 (µ) u2 ( x ) 22µx u 2 ( N 0 (E) ) u 2 ( N ( E ) ) 22 N(E)NE ()N(E)020 ln N (E) 1

Experimental arrangement

New experimental arrangementSourceSampleCollimatorDetector

Experimental measurementProblems:- Single line gamma emitters should be used to avoidcoincidence summing effects- At low energy – small angle Compton scatteringcontribution the collimated source and the sample far fromdetector High intensity sources required – storage problem ?- Time consuming

Measured linearattenuation coefficientx 2.5 cm-1Energy/keVFEP counting rate(spectrum 1) N1/t1FEP counting rateµm (cm ) (spectrum 2) N2/t2 (1/x) 1063837.255.630.10166260.0648.780.083

Mass attenuation coefficients/ cm2.g-110Standard solution HClStandard solution HClPhosphogypsum10,10,01101001000Energy/keV10000

Interpolated attenuation coefficientExample: attenuation in a 10 cm thick matrix for 300 keV energyMesurement of µ for some energies:Energy/keV100200500N1 (s-1)1000600200N2 (s-1)18016073N1 / N20.1800.2670.365µ (cm-1)0.1710.1320,101Interpolation for E 300 keV:0.1800.170Measured valuesInterpolated value0.160Linear interpolation: µ 0.122 cm-1Logarithmic interpolation: µ 0.117 cm-1µ 200300Energy (keV)400500600

Software for visualization of the dependence ofinteraction coefficients on element and energyEPICSHOW (NEA databank)EPICSHOW is part of the EPIC (Electron Photon Interaction Code) system.The program allows interactive viewing and comparison of data in the EPICdata bases.Plots and listings can be obtained.The EPIC electron, photon, and charged particle data bases are availablewith this package.The data bases include data for elements hydrogen (Z 1) to fermium(Z 100) over the energy range 10 eV to 1 GeV.

Self attenuation Simple formula Generalisation

Self-attenuation in a volume sampleIntrinsic photon flux: I0 (What you wish to know to derive the activity)Emitted photon flux: I (What is recorded by the detector)For a thin layer, with thickness de:I0dI 0 dexThis partial photon flux is attenuated through thickness e:I0dI exp( µ e ) dexOnly true if thesample ishomogeneous !xSampledeµ linear attenuation cofficient (cm-1)For the whole volume with thickness x :xe0de1 exp( µ x )I I 0 exp( µ e ) I0 xµ x0

Self-attenuation in a volume sampleI I0 1 exp( µ x )µ xIntrinsic photon flux: I0 (What you wish to know to derive the activity)Emitted photon flux: I (What is recorded by the detector)Self-attenuation:Catt1 exp( µx ) µx Approximation for a thin source (µx 1) : µ x I I0 1 2 Catt 1 µ x2

Interpolated attenuation coefficientExample: self-attenuation in a 10 cm thick matrix for 300 keV energy0.180Interpolation for E 300 keV :0.170Measured valuesInterpolated value0.160Linear interpolation: µ 0.122 cm-1Logarithmic interpolation: µ 0.117 cm-1µ 200300400500600Energy (keV)Self-attenuation at 300 keV :1 exp( µ300 x) 1 exp( 0.117 10)Catt 0.589µ300 x0.117 10

Self-attenuation in a volume sampleSelf-attenuation: Catt If the measured sample is subject to attenuation and the calibrationsource is not, a correction factor must be applied to the peak area that is:1/CSattCself Catt 1 exp( µx )µx 1µx 1 exp( µx )If both are subject to self-attenuation, the corrective factor is the ratio ofthe self attenuation for each materialCself 1Catt mes 1Catt cal[[]] µx 1 exp( µx ) mes µx 1 exp( µx ) calMes measuredsampleCal : calibrationsource

Self-attenuation in a volume sample Can also be computed as a transfer factor from anefficiency calibration established reference material tomeasure a different mateial (in the same geometry)ε mes ε cal fSelf Thus the efficiency transfer factor is:fSelf [Catt ]mes[Catt ]cal 1 exp( µx ) µx mes 1 exp( µx ) µx calMes measuredsampleCal : calibrationsource

Transfer from an efficiency calibration established with a liquid source(filled with 10 cm HCl) for matrixes silica and sand:ε mes ε cal fSelf ε cal[C ] [C ]att mesatt calDensities:water/HCl 1.016silica 0.25sand/resin 1.54Energy (keV)µ HCl (cm2.g-1)µ HCl (cm-1)[Catt ]calµ silica 0874µ silica (cm-1)0.0420.0310.0270.022[Catt]fSelf (silica)µ sand (cm2.g-1)µ sand .510.1130.1740.8981.410.09190.142[Catt]fSelf (sand)0.3540.750.4290.790.4740.820.5340.84

General formula Realistic if the source is far from the detector (parallel beam - normalincidence) - small source Not true for environment measurements (d’, d" » d)dSampled’dGecrystald’’d’SampleGecrystal

General formula Must consider all possible trajectories for each point of the volumesample - integration over solid angle and sample volumeP (r , t )Samplee dV exp( µ(E ) e(r , t ))dΩCatt VΩ dV dΩVΩΩPoint P with position r, and emissiondirection te: path in the sample matrixAdd the container absorption and probabilityof full-absorption of the photon in thedetector active volume

General formulaP (r , t )Sample dV exp( µ(E ) e(r , t )) T (E, r , t ) P (E, r , t ) dΩCatt VeΩ dV T (E, r , t ) P (E, r , t ) dΩVΩΩDenominator « self attenuation » for a transparent sampleNµ(E) : attenuation coefficient of the sample material for theenergy Ee : trajectory through the sampleT : Transmission through absorbers (container, detectorwindow, )P : Probability of full-energy absorption in the detectorThis correction can be numerically computed (Gauss-Legendre integration)

Efficiency transfer factor Transfer factor from an efficiency calibrationestablished reference material to measure a differentmaterial (in the same geometry)[Catt ]mesfSelf [Catt ]calε mes ε cal fSelf ε cal[C ] [C ]att mesatt calThis transfer factor can be numerically computed (Gauss-Legendreintegration)

Self-attenuation in Marinelli geometrySample dV exp( µ(E ) e(r , t )) T (E, r , t ) P (E, r , t ) dΩCatt VΩ dV T (E, r , t ) P (E, r , t ) dΩVGecrystalΩThe general expression must be extended todifferent parts of the sample, according to thepath of the photonsNumerical integration using different volumesThis correction can be numerically computed (Gauss-Legendre integration)

Monte Carlo simulation Self attenuation can be computed usingMonte Carlo methods– General codes (GEANT, MCNP,PENELOPE, etc)– Dedicated software (DETEFF, GESPECOR,etc.) Any geometry (including non-cylindricalsymmetry) can be considered Time-consuming ? Dedicated sofwareare optimizedSampleGecrystal

Practical toolsMethods for self-attenuation correction Empirical methods – simplified computing Analytic approach– ANGLE– ETNA , etc. Monte Carlo methods– DETEFF– GESPECOR– General codes (GEANT, PENELOPE, MCNP)

Examples Importance of the material density Influence of the filling height Change of matrix

Self –attenuation in silica Silica low density (0.25 g.cm-3) Sand (mainly silica) (2.5 g.cm-3) Thickness 1 cmRadionuclideEnergy/keVMass 7730.9900.90940K1460.80.05260.9930.937

Self –attenuation in steel Fe (7.5 g.cm-3)RadionuclideEnergy/keVMass attcoefficient(cm2.g-1)Selfattenuation1 cmSelfattenuation1 mmSelfattenuation0.1 90.9730.99740K1460.80.04950.8350.9820.998For the low energies, only the very first thickness contributes

Influence of the filling height?

Influence of the filling heightPlastic vial filled with HCl 1N - Reference height 46,5 mm – diameter 39 mmAt 10 cm1,20At contact1,21,1540 mm filling height1,1542 mm filling heightFilling height 35 mm1,10Filling height 40 mmFilling height 43 mm1,05Filling height 45 mmFilling height 48 mm1,001,144 mm filling height45 mm filling height1,0547 mm filling height150 mm filling heightFilling height 50 000About 5 % variation for 10% change in filling heightMore important when the height is reducedMore sensitive for low-energiesMore sensitive at short source-to-detector distance2500

Influence of the filling heightPlastic vial at contact - Reference height 46,5 mm – diameter 39 mmSilica (d 0.24)Sand-resin (d 1.54)Efficiency transfer for sandEfficiency transfer for silica1,21,21,1540 mm42 mm1,142 mm44 mm1,0544 mm145 mm145 mm0,9547 mm0,9547 mm0,948 mm0,948 mm1,1540 mm1,11,050500100015002000250050 mm0500Energy/keV10001500Energy/keV40 mm – 500 keV: HCl 1.11; silica 1.10; sand 1.1250 mm – 500 keV: HCl 0.946; silica 0.951; sand 0.9442000250050 mm

Influence of the filling heightPlastic vial at contact - Reference height 20 mm – diameter 39 mmHCl (d 1.016)Sand-resin (d 2.54)20 mm /- 2 mm - Sand at contact1,061,041,02Filled 22 mm1Filled 18 mm0,980,960,940500100015002000Efficie nc y trans fer fac torE fficiency tyransfer factor20 mm /- 2 mm HCl at contact1,11,05Filled 18 mm1Filled 22 mm0,950,905002500Energy/keV18 mm – 500 keV: HCl 1.049; sand 1.05922 mm – 500 keV: HCl 0.955; sand 0.94710001500Energy/keV20002500

Efficiency calibration for different geometries0,10Source ponctuelle à 2 cmSource volumique (silice d 0,25) au contactSource volumique liquide (d 1,016) au contactSource volumique (sable/résine d 1,54) au contactSource ponctuelle à 5 cmSource ponctuelle à 10 cm (référence)Source ponctuelle à 20 cm0,08Experimental calibrationwith volume sourcesSilica low density (d 0.24)Rendement0,06HCl 1N (d 1.016)Sand-resin (d 1.54)0,040,020,00100Energie (keV)1000

Efficiency transferTransfer from an efficiency calibration established with a liquid source(filled with 4.65 cm HCl) for matrixes silica and sand:EnergyHClDensities:water/HCl 1.016silica 0.25sand/resin 1.54ε mes ε cal fSelf ε cal[C ] [C ]att mesSimple expression :[Catt ]mesfSelf [Catt 0,975f self20508010020050010002000µ (cm -1)0,5740,0670,0430,0380,0300,0210,0150,011µ 0,0860,4650,5650,6580,6530,7330,7940,849f self20508010020050010002000Silicaatt cal 1 exp( µx ) µx mes 1 exp( µx ) µx ,3910,7500,8360,9500,8830,9130,9340,952

Application exampleTransfer from an efficiency calibration established with a liquid source(filled with 4.65 cm HCl) for matrixes silica and sand:[Catt ]mesfSelf [Catt ]calComparisonof the generalised formula(ETNA code) with thesimple 0107Sand1,54 ,9480,963

Summary Self attenuation is of main importance for low energiesand high densities In case of high attenuation only a thin layer of thesample located close to the detector is important In case of homogeneous matrix, it can be computed ifthe attenuation cœfficient is knownMethods for self-attenuation correction Empirical methods – simplified computing Analytic approach Monte Carlo methods

Partial interaction coefficients: Photoelectric absorption: τi(E) (major at low energies) Compton scattering: σi(E) Pair production effect: κi(E) (only if E 1022 keV) Depend on the energy, E, and the material (Z) For practical use : tables function of Z and E Tables : cross sections (1 barn 10-24 cm 2) or mass attenuation(cm 2.g-1)

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