: IPREM/LCABIE, UMR VNRS Université de Pau et des Pays de l Adour (UPPA), F Pau Cedex 09 b. : CEA, DAM, DIF, F Arpajon, Cedex.

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Are polytomic interferences, cross contmintion, mixing-effect, etc., ostcles for use of Lser ltion - ICP-MS coupling s n opertionl technique for urnium isotope rtio prticle nlysis?

Instruments NBS 950 rnium prticles V-Femtosecond lser ltion High Resolution Sector-Field ICP-MS (LAMDBA, Amplitude system/nexey) Plese touch : frmes to ply nimtions Polycronte disk Optimiztion of

2 ng Ojectives Anlysis of environmentl smples which consists in dust collected with cotton clos wiped y inspectors on surfces inside declred nucler fcilities is key tool for sfegurds.

1 Are polytomic interferences, cross contmintion, mixing-effect, etc., ostcles for use of Lser ltion - ICP-MS coupling s n opertionl technique for urnium isotope rtio prticle nlysis? Arine DONARD,, Fien POINTRIER, Christophe PECHEYRAN : IPREM/LCABIE, MR VNRS niversité de Pu et des Pys de l Adour (PPA), F-6405 Pu Cedex 09 : CEA, DAM, DIF, F Arpjon, Cedex Smple preprtion / Instruments NBS 950 rnium prticles V-Femtosecond lser ltion High Resolution Sector-Field ICP-MS (LAMDBA, Amplitude system/nexey) Plese touch : frmes to ply nimtions Polycronte disk Optimiztion of signl cquisition to ccess detiled informtions Altion of single prticle 0.2 ng Ojectives Anlysis of environmentl smples which consists in dust collected with cotton clos wiped y inspectors on surfces inside declred nucler fcilities is key tool for sfegurds. Prticle nlysis, i.e. mesurement of urnium isotopic composition in single micrometer-size prticles, is crried out of few lortories, which use two estlished techniques: Secondry Ions Mss Spectrometry nd comintion of fission trcks technique nd Thermo-Ioniztion Mss Spectrometry (TIMS). Regulr poster The gol of this work is to explore potentil of Lser Altion HR-ICP-MS coupling s n lterntive technique for prticle nlysis. LA-HR-ICP-MS is promising techniques s its comines following dvntges: rpidity, very high sensitivity, nd very high signl/noise rtio. More precisely, study presented here is focused on : chrcteriztion of performnce of technique: ccurcy, reproduciility, detection limits identifiction of limittions of this technique in terms of Prticle during ltion process tht might ffect mesure of surrounding prticles Interferences due to non-urnium prticles from surrounding environment (P prticles)? Performnce Altion of 5 prticles of NBS 950 stndrd Altion of 4 prticles Mesurement of signl Interferences (P) Comprison of isotopic rtios for: NBS 950 urnium nd P prticles Imging of re-deposition of urnium round crter fter ltion Estimtion of detection limits NBS 950 urnium

2 Are polytomic interferences, cross contmintion, mixing-effect, etc., ostcles for use of Lser ltion - ICP-MS coupling s n opertionl technique for urnium isotope rtio prticle nlysis? Arine DONARD,, Fien POINTRIER, Christophe PECHEYRAN : IPREM/LCABIE, MR VNRS niversité de Pu et des Pys de l Adour (PPA), F-6405 Pu Cedex 09 : CEA, DAM, DIF, F Arpjon, Cedex NBS 950 rnium prticles Anlysis of environmentl smples which consists in dust collected with cotton clos wiped y inspectors on surfces inside declred nucler fcilities is key tool for sfegurds. Prticle nlysis, i.e. mesurement of urnium isotopic composition in single micrometer-size prticles, is crried out of few lortories, which use two estlished techniques: Secondry Ions Mss Spectrometry nd comintion of fission trcks technique nd Thermo-Ioniztion Mss Spectrometry (TIMS). V-Femtosecond lser ltion (LAMDBA, Amplitude system/nexey) Ethnol + Collodion (1/11) Polycronte disk,0% Rel. error from Reference vlue 2,44% 0,0071 0, se of mini-ltion cell (00 mm ) ICP-MS: Electrosttic scn Isotopes:,,,, H Triple mode (pulse counting, nlog nd Frdy) Jet interfce ddition of N2 to enhnce sensitivity Lser Resulting Altion dimeter: 100 µm Fluence: 10 J/cm2 To prevent some skewing effects, dwell time set up on ICP-MS is smllest possile to cquire lrge numer of points for n ltion. Durtion mesurement cycle (mesurement of 5 msses): 26 ms Becuse of this short dwell time : increse of numer nd of intensity of signl spikes, due to irregulr rrivl of ltion frgments into plsm. Dt tretment requires spike rejection filter. Externl correction of mss is (NIST 610) P prticles Comprison of isotopic rtios for: Altion of 4 prticles Mesurement of signl 24,1% Prticle numer #1 #2 # #4 1,8% 16,1% Percentge of redeposition fter ltion () 1.1% 2.6% 0.4%.5% -0,% 51,1% 1,5% Signl of ech isotope is integrted to clculte isotopic rtios Interferences First step : Altion of prticle: 50µm 50µm Second step :Altion of crter + surrounding re to study of re-deposition 00µm 00µm Altion of 5 prticles of NBS 950 stndrd / / / 5,4% Altion of single prticle 0.2 ng Performnce 0, Locliztion of urnium prticles y SEM (Scnning Electron Microscope) FEI Qunt D FEG Short/trnsient signl Instrument settings: More precisely, study presented here is focused on : chrcteriztion of performnce of technique: ccurcy, reproduciility, detection limits identifiction of limittions of this technique in terms of Prticle during ltion process tht might ffect mesure of surrounding prticles Interferences due to non-urnium prticles from surrounding environment (P prticles)? High Resolution Sector-Field ICP-MS The gol of this work is to explore potentil of Lser Altion HR-ICP-MS coupling s n lterntive technique for prticle nlysis. LA-HR-ICP-MS is promising techniques s its comines following dvntges: rpidity, very high sensitivity, nd very high signl/noise rtio. Averge (5 replictes) Externl reproduciility (RSD, 5 replictes) Internl reproduciility (RSD on v. vlue) Smple preprtion / Instruments Ojectives NBS 950 urnium nd P prticles NBS 950 urnium Signl on urnium isotopes during ltion of P prticles (rtio with respect to 208 P) Rtio / 206 P Interference t <LD 206 <LD P14N2? of urnium fter ltion Estimtion of detection limits Numers of counts in lnk disc < 70 counts Poisson s lw With B, verge of counts depending on integrtion time LOD* (s ) LOD* (s isotope) 5 pg 1 fg 1 pg 40 g 46 g 75 g 4 g 40 g Sptil resolution 40 µm *Clculted from NIST 610 ltion Detection of 400-nm dimeter N prticle (for ) Potentil for detection of 15-nm HE prticle (9% ) 11 novemre 2014 No systemtic direction for fll-out loctions. Limited mounts of urnium re re-deposited (% rnge). Consistent with results of previous study (Huert et l 2014) Very low signl recorded t mss of when P prticles re lted, possily due to interference of 206P14N2 No significnt influence of polytomic interferences with P on isotopic rtio mesurement for urnium prticles surrounded y led prticles

3 Are polytomic interferences, cross contmintion, mixing-effect, etc., ostcles for use of Lser ltion - ICP-MS coupling s n opertionl technique for urnium isotope rtio prticle nlysis? Arine DONARD,, Fien POINTRIER, Christophe PECHEYRAN : IPREM/LCABIE, MR VNRS niversité de Pu et des Pys de l Adour (PPA), F-6405 Pu Cedex 09 : CEA, DAM, DIF, F Arpjon, Cedex Smple preprtion / Instruments NBS 950 rnium prticles V-Femtosecond lser ltion High Resolution Sector-Field ICP-MS (LAMDBA, Amplitude system/nexey) Smple preprtion Plese touch following frmes NBS 950 rnium prticles to ccess detiled informtions Polycronte disc Altion of single prticle Dry for 24h Optimiztion of signl cquisition Ojectives 1 cm Anlysis of environmentl smples which consists in dust collected with cotton clos wiped y inspectors on surfces inside declred nucler fcilities is key tool for sfegurds. Polycronte disk Ethnol + Collodion (1/11) Prticle nlysis, i.e. mesurement of urnium isotopic composition in single micrometer-size prticles, is crried out of few lortories, which use two estlished techniques: Secondry Ions Mss Spectrometry nd comintion of fission trcks technique nd Thermo-Ioniztion Mss Spectrometry (TIMS). Instruments The gol of this work is to explore potentil of Lser Altion HR-ICP-MS coupling s n lterntive technique for prticle nlysis. LA-HR-ICP-MS is promising techniques s its comines following dvntges: rpidity, very high sensitivity, nd very high signl/noise rtio. V-Femtosecond More precisely, study presented here islser focusedltion on : High Resolution Sector-Field ICP-MS chrcteriztion of performnce of technique: ccurcy, reproduciility, detection limits LAMDBA, Amplitude system/nexey identifiction of limittions of this technique in terms of ser mesure of surrounding prticles Prticle during ltion process tht might ffect L Locliztion of urnium Interferences due to non-urnium prticles from surrounding environment (P prticles)? ( prticles y SEM (Scnning Electron Microscope) FEI Qunt D FEG Performnce Altion of 5 prticles of NBS 950 stndrd ) Glvnometric mirrors Altion of 4 prticles Mesurement of signl Virtul shping of ls er Imging of e re-deposition of urnium round m crter fter ltion Estimtion of detection limits Regulr poster Instrument settings: ICP-MS: Electrosttic scn Isotopes:,,,, H Triple mode (pulse counting, nlog nd Frdy) Jet interfce with ddition of N2 to enhnce Interferences (P) sensitivity Lser Femtosecond lser Comprison of isotopic rtios for: V : 257 nm Resulting spot: 50 *50 µm NBSµm 950 urnium nd PAltion prticles Fluence: 10 J/cm2 Repetition rte: 1 khz Scn speed: 1 mm/s

Instruments NBS 950 rnium prticles Smple preprtion V-Femtosecond lser ltion High Resolution Sector-Field ICP-MS (LAMDBA, Amplitude system/nexey) Plese touch following frmes NBS 950 rnium prticles to

4 Are polytomic interferences, cross contmintion, mixing-effect, etc., ostcles for use of Lser ltion - ICP-MS coupling s n opertionl technique for urnium isotope rtio prticle nlysis? Arine DONARD,, Fien POINTRIER, Christophe PECHEYRAN : IPREM/LCABIE, MR VNRS niversité de Pu et des Pys de l Adour (PPA), F-6405 Pu Cedex 09 : CEA, DAM, DIF, F Arpjon, Cedex Smple preprtion / Instruments NBS 950 rnium prticles Smple preprtion V-Femtosecond lser ltion High Resolution Sector-Field ICP-MS (LAMDBA, Amplitude system/nexey) Plese touch following frmes NBS 950 rnium prticles to ccess detiled informtions Polycronte disc Altion of single prticle Dry for 24h Optimiztion of signl cquisition Ojectives Anlysis of environmentl smples which consists in dust collected with cotton clos wiped y inspectors on surfces inside declred nucler fcilitiespolycronte is key tool for sfegurds. disk Ethnol + Collodion (1/11) Prticle nlysis, i.e. mesurement of urnium isotopic composition in single micrometer-size prticles, is crried out of few lortories, which use two estlished techniques: Secondry Ions Mss Spectrometry nd comintion of fission trcks technique nd Thermo-Ioniztion Mss Spectrometry (TIMS). 1 cm Virtul shping of lser em Regulr poster Instrument settings: The gol of this work is to explore potentil of Lser Altion HR-ICP-MS coupling s n lterntive technique for prticle nlysis. LA-HR-ICP-MS is promising techniques s its comines following dvntges: rpidity, very high sensitivity, nd very high signl/noise rtio. V-Femtosecond lser ltion 50 µm Instruments High Resolution Sector-Field ICP-MS More precisely, study presented here is focused on : chrcteriztion of performnce of technique: ccurcy, reproduciility, detection limits LAMDBA, Amplitude system/nexey identifiction of limittions of this technique in terms of ser mesure of surrounding prticles Prticle during ltion process tht might ffect L Locliztion of urnium Interferences due to non-urnium prticles from surrounding environment (P prticles)? ( prticles y SEM (Scnning Electron Microscope) FEI Qunt D FEG Performnce Altion of 5 prticles of NBS 950 stndrd ) Glvnometric mirrors 50 µm Altion of 4 prticles Mesurement of signl Imging of re-deposition of urnium round crter fter ltion Estimtion of detection limits ICP-MS: Electrosttic scn Isotopes:,,,, H Triple mode (pulse counting, nlog nd Frdy) Jet interfce with ddition of N2 to enhnce sensitivity Interferences (P) Lser Femtosecond lser Comprison of isotopic rtios for: V : 257 nm Resulting Altion spot: 50 *50 µm NBSµm 950 urnium nd P prticles Fluence: 10 J/cm2 Repetition rte: 1 khz Scn speed: 1 mm/s

Instruments NBS 950 rnium prticles V-Femtosecond lser ltion High Resolution Sector-Field ICP-MS (LAMDBA, Amplitude system/nexey) Plese touch following frmes to ccess detiled informtions Skew effect

5 Are polytomic interferences, cross contmintion, mixing-effect, etc., ostcles for use of Lser ltion - ICP-MS coupling s n opertionl technique for urnium isotope rtio prticle nlysis? Arine DONARD,, Fien POINTRIER, Christophe PECHEYRAN : IPREM/LCABIE, MR VNRS niversité de Pu et des Pys de l Adour (PPA), F-6405 Pu Cedex 09 : CEA, DAM, DIF, F Arpjon, Cedex Smple preprtion / Instruments NBS 950 rnium prticles V-Femtosecond lser ltion High Resolution Sector-Field ICP-MS (LAMDBA, Amplitude system/nexey) Plese touch following frmes to ccess detiled informtions Skew effect Polycronte disc se of mini-ltion cell (00 mm ) Insufficient numer of points to define signl Poor precision due to non representtive smpling Ojectives Optimiztion of signl cquisition Altion of single prticle To prevent some skewing effects, dwell time set up on ICP-MS is smllest possile to cquire lrge numer of points for n ltion. Anlysis of environmentl smples which consists in dust collected with cotton on surfces inside declred nucler fcilities is key tool for sfegurds. I I clos I inspectors I I1 I wiped I I1 y I Durtion of mesurement cycle (mesurement of 5 msses): 26 ms Prticle nlysis, i.e. mesurement of urnium isotopic composition in single micrometer-size prticles, is crried out of few lortories, which use two estlished techniques: Secondry Ions Mss Spectrometry nd comintion of fission trcks technique nd Thermo-Ioniztion Mss Spectrometry (TIMS). V The gol of this work is to explore potentil of Lser Altion HR-ICP-MS coupling s n lterntive technique for prticle nlysis. LA-HR-ICP-MS is promising techniques s its comines following dvntges: rpidity, very high sensitivity, nd very high signl/noise rtio. More precisely, study presented here is focused on : chrcteriztion of performnce of technique: ccurcy, reproduciility, detection limits identifiction of limittions of this technique in terms of Prticle during ltion process tht If might mesure of surrounding prticles >0ffect points Interferences due to non-urnium prticles from surrounding environment (P prticles)? Skew effect negligile y isotope Regulr poster Becuse of this short dwell time : increse of numer nd intensities of signl spikes, due to irregulr rrivl of ltion frgments into plsm. Dt tretment requires spike rejection filter. se of ll detectors Performnce Altion of of 5 prticles of NBS 950 stndrd singlealtion prticle 0.2 ng : Frdy cup or Anlog : Pulse counting Altion of 4 prticles Mesurement of signl : Anlog : Pulse counting Imging of of urnium round My inducere-deposition is (cross clirtion etween fter ltion Frdy cups ndcrter pulse couting mode difficult) Estimtion of detection limits For ech isotope: Interferences (P) Sutrction of lnk signl point y point Comprison of isotopic rtios for: Sum of ll intensities lnk corrected nd P prticles Externl correction of mss is (NIST 610)

Instruments NBS 950 rnium prticles Polycronte disc V-Femtosecond lser ltion High Resolution Sector-Field ICP-MS (LAMDBA, Amplitude system/nexey) Performnce Plese touch following frmes to/ccess

6 Are polytomic interferences, cross contmintion, mixing-effect, etc., ostcles for use of Lser ltion - ICP-MS coupling s n opertionl technique for urnium isotope rtio prticle nlysis? Arine DONARD,, Fien POINTRIER, Christophe PECHEYRAN : IPREM/LCABIE, MR VNRS niversité de Pu et des Pys de l Adour (PPA), F-6405 Pu Cedex 09 : CEA, DAM, DIF, F Arpjon, Cedex Smple preprtion / Instruments NBS 950 rnium prticles Polycronte disc V-Femtosecond lser ltion High Resolution Sector-Field ICP-MS (LAMDBA, Amplitude system/nexey) Performnce Plese touch following frmes to/ccess detiled informtions / / Altion of 5 prticles of NBS 950 stndrd Averge (5 replictes) 0, ,0071 0, Ojectives Optimiztion of signl cquisition Altion of single prticle Estimtion of detection limits Externl reproduciility 5,4% 1,5% 24,1% Anlysis of environmentl smples which consists in dust collected with cotton clos wiped y inspectors on surfces inside declred nucler fcilities isof key tool for sfegurds. (RSD, 5 replictes) Numers counts in lnk disc < 70 counts Prticle nlysis, i.e. mesurement of urnium isotopic composition in single micrometer-size prticles, is crried out of few lortories, which use two estlished techniques: Secondry Ions Mss Spectrometry nd comintion ofinternl fission trcks technique nd Thermo-Ioniztion Mss Spectrometry (TIMS). reproduciility,0% 1,8% 16,1% The gol of this work is to explore(rsd potentil of Lser Altion HR-ICP-MS coupling s n lterntive technique for prticle nlysis. LA-HR-ICP-MS is promising techniques s its comines on v. vlue) Poisson s lw Regulr poster following dvntges: rpidity, very high sensitivity, nd very high signl/noise rtio. More precisely, study presented is focused on : Rel.here error from 2,44% reproduciility, -0,% chrcteriztion of performnce of technique: ccurcy, detection limits 51,1% Reference vlue identifiction of limittions of this technique in terms of Prticle during ltion process tht might ffect mesure of surrounding prticles Interferences due to non-urnium prticles from surrounding environment (P prticles)? Numer of counts integrted for n ltion (exmple for 1 ltion) 2,E+04 2,E+06 Blnk (counts) 1 1 Performnce Numer of count intergrted NBS 950 (counts) 4,E+02 2,E Altion of 5 prticles of NBS 950 stndrd Cpility to detect in 90-nm dimeter in 400-nm dimeter N prticle. Altion of 4 prticles Mesurement of signl N prticle, nd to detect Imging of urnium round re-deposition prticle (9% of ) crter fter ltion Potentil for detection of in 15-nm dimeter HE nd of in 80-nm dimeter HE prticle (1.05% ). Estimtion of detection limits With B, verge of counts depending on integrtion time Interferences (P) LOD* (s isotope) 16 g Comprison of isotopic rtios for: 16 g nd P prticles *Clculted from NIST 610 ltion 12 g 40 g

7 Are polytomic interferences, cross contmintion, mixing-effect, etc., ostcles for use of Lser ltion - ICP-MS coupling s n opertionl technique for urnium isotope rtio prticle nlysis? Arine DONARD,, Fien POINTRIER, Christophe PECHEYRAN : IPREM/LCABIE, MR VNRS niversité de Pu et des Pys de l Adour (PPA), F-6405 Pu Cedex 09 : CEA, DAM, DIF, F Arpjon, Cedex Smple preprtion / Instruments NBS 950 rnium prticles V-Femtosecond lser ltion High Resolution Sector-Field ICP-MS (LAMDBA, Amplitude system/nexey) Polycronte disc Plese touch following frmes to ccess detiled informtions First step : Altion of prticle: 50µm 50µm Ojectives Altion of single prticle Optimiztion of signl cquisition Altion of 4 prticles Mesurement of signl Prticle numer #1 #2 # #4 Anlysis of environmentl smples which consists in dust collected with cotton clos wiped y inspectors on surfces inside declred nucler fcilities is key tool for sfegurds. Percentge of Prticle nlysis, i.e. mesurement of urnium isotopic composition in single micrometer-size prticles, is crried out of few lortories, which use two estlished techniques: Secondry Ions Mss re-deposition 1.1% 2.6% 0.4% Spectrometry nd comintion of fission trcks technique nd Thermo-Ioniztion Mss Spectrometry (TIMS). fter ltion ( ) The gol of this work is to explore potentil of Lser Altion HR-ICP-MS coupling s n lterntive technique for prticle nlysis. LA-HR-ICP-MS is promising techniques s its comines.5% following dvntges: rpidity, very high sensitivity, nd very high signl/noise rtio. Second step :Altion of crter + More precisely, study presented here is focused on : surrounding re to study of re-deposition chrcteriztion of performnce of technique: ccurcy, reproduciility, detection limits 00µm 00µm identifiction of limittions of this technique in terms of Regulr poster Prticle during ltion process tht might ffect mesure of surrounding prticles Interferences due to non-urnium prticles from surrounding environment (P prticles)? Performnce Altion of 5 prticles of NBS 950 stndrd Imging of re-deposition of urnium fter ltion No systemtic direction for fll-out loctions. Limited mounts of urnium re re-deposited (% rnge) Interferences Consistent with results of previous study (Huert et l (P) 2014) Altion of 4 prticles Mesurement of signl Comprison of isotopic rtios for: nd P prticles Sptil resolution 40 µm Estimtion of detection limits Imging of re-deposition of urnium round crter fter ltion

8 Are polytomic interferences, cross contmintion, mixing-effect, etc., ostcles for use of Lser ltion - ICP-MS coupling s n opertionl technique for urnium isotope rtio prticle nlysis? Arine DONARD,, Fien POINTRIER, Christophe PECHEYRAN : IPREM/LCABIE, MR VNRS niversité de Pu et des Pys de l Adour (PPA), F-6405 Pu Cedex 09 : CEA, DAM, DIF, F Arpjon, Cedex Smple preprtion / Instruments NBS 950 rnium prticles Polycronte disc V-Femtosecond lser ltion High Resolution Sector-Field ICP-MS (LAMDBA, Amplitude system/nexey) Plese touch following frmes Interferences to ccess detiled informtions Comprison of isotopic rtios for: NBS 950 urnium nd P prticles NBS 950 urnium Ojectives Optimiztion of signl cquisition Altion of single prticle P prticles Signl on urnium isotopes during ltion of P prticles (rtio with respect Anlysis of environmentl smples which consists in dust collected with cotton clos wiped y inspectors on surfces inside declred nucler fcilities is key to 208tool P)for sfegurds. Prticle nlysis, i.e. mesurement of urnium isotopic composition in single micrometer-size prticles, is crried out of few lortories, which use two estlished techniques: Secondry Ions Mss Spectrometry nd comintion of fission trcks technique nd Thermo-Ioniztion Mss Spectrometry (TIMS). Rtio / Regulr poster -5-7 The gol of this work is to explore potentil of Lser Altion HR-ICP-MS coupling s n lterntive technique for prticle nlysis. LA-HR-ICP-MS is promising techniques s its comines <LD <LD P following dvntges: rpidity, very high sensitivity, nd very high signl/noise rtio. More precisely, study presented here is focused on : chrcteriztion of performnce of technique: ccurcy, reproduciility, detection limits identifiction of limittions of this technique in terms of Prticle during ltion process tht might ffect mesure of surrounding prticles Interferences due to non-urnium prticles from surrounding environment (P prticles)? Interference t P14N2? 206 Performnce Altion of 5 prticles of NBS 950 stndrd Altion of 4 prticles Mesurement of signl Interferences (P) Comprison of isotopic rtios for: nd P prticles Imging of Very low signl recorded t mss of when P prticles re lted, possily due to re-deposition of urnium round interference of 206P14N2 crter fter ltion Estimtion of detection limits No significnt influence of polytomic interferences with P on isotopic rtio mesurement for urnium prticles surrounded y led prticles.

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SUPPLEMENTARY INFORMATION doi:.38/nture8499 doi:.38/nture8499 5 6 5 4.5 Firing rte (Hz) -67-65 -66-6 -58 V m (mv) -7-67 -68-66 -64 c Thet power (mv ) -73-69 -7-7 -7.5.8 3....9.9.4.6.6. 9 8 9 8 9 8 9 8 9 8 Supplementry Figure Firing