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1. $^{240}$Pu/$^{239}$Pu signatures allow refining the chronology of radionuclide fallout in South America

Author

Pierre-Alexis Chaboche, Fabien Pointurier, Pierre Sabatier, Anthony Foucher, Tales Tiecher, Jean P.G. Minella, Marcos Tassano, Amélie Hubert, Sergio Morera, Stéphane Guédron, Christophe Ardois, Béatrice Boulet, Catherine Cossonnet, Pablo Cabral, Mirel Cabrera, Guillermo Chalar, Olivier Evrard, Laboratoire des Sciences du Climat et de l'Environnement [Gif-sur-Yvette] (LSCE), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Géochimie Des Impacts (GEDI), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), CEA DAM ILE-DE-FRANCE - Bruyères-le-Châtel [Arpajon] (CEA DAM IDF), Environnements, Dynamiques et Territoires de Montagne (EDYTEM), Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS), Universidade Federal do Rio Grande do Sul [Porto Alegre] (UFRGS), Universidade Federal de Santa Maria = Federal University of Santa Maria [Santa Maria, RS, Brazil] (UFSM), Facultad de Ciencias (UDELAR), Instituto Geofísico del Perú (IGP), Institut des Sciences de la Terre (ISTerre), Institut national des sciences de l'Univers (INSU - CNRS)-Institut de recherche pour le développement [IRD] : UR219-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Gustave Eiffel-Université Grenoble Alpes (UGA), Laboratoire de métrologie de la radioactivité dans l'environnement (IRSN/PSE-ENV/SAME/LMRE), Service d'analyses et de métrologie de l'environnement (IRSN/PSE-ENV/SAME), and Institut de Radioprotection et de Sûreté Nucléaire (IRSN)-Institut de Radioprotection et de Sûreté Nucléaire (IRSN)

Subjects
Environmental Engineering, Nuclear weapon tests, Geochronology, Plutonium isotopes, [SDV.SA.SDS]Life Sciences [q-bio]/Agricultural sciences/Soil study, Pollution, Panoply, [SDU.STU.GC]Sciences of the Universe [physics]/Earth Sciences/Geochemistry, [SDE]Environmental Sciences, Soil erosion, Environmental Chemistry, [SDU.STU.GM]Sciences of the Universe [physics]/Earth Sciences/Geomorphology, [SDU.ENVI]Sciences of the Universe [physics]/Continental interfaces, environment, Waste Management and Disposal
Abstract

International audience; Atmospheric nuclear tests (1945-1980) have led to radioactive fallout across the globe. French tests in Polynesia (1966-1974) may influence the signature of fallout in South America in addition to those conducted by USA and former USSR until 1963 in the Northern hemisphere. Here, we compiled the $^{240}$Pu/$^{239}$Pu atom ratios reported for soils of South America and conducted additional measurements to examine their latitudinal distributions across this continent. Significantly lower ratio values were found in the 20-45° latitudinal band (0.04 to 0.13) compared to the rest of the continent (up to 0.20) and attributed to the contribution of the French atmospheric tests to the ultra-trace plutonium levels found in these soils. Based on sediment cores collected in lakes of Chile and Uruguay, we show the added value of measuring $^{240}$Pu/$^{239}$Pu atom ratios to refine the age models of environmental archives in this region of the world.

Published
2022
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2. New determination of the 229Th half-life

Author

Amy M. Gaffney, Ryan P. Fitzgerald, Ross W. Williams, Robert E. Steiner, M. E. Bennett, Jacqueline L. Mann, Alkiviadis Gourgiotis, Heather M. Dion, Richard M. Essex, Kenneth G. W. Inn, William S. Kinman, Ronald Colle, Lizbeth Laureano-Perez, Stephen P. LaMont, Amélie Hubert, National Institute of Standards and Technology [Gaithersburg] (NIST), Shine Medical Technologies, Los Alamos National Laboratory (LANL), Lawrence Livermore National Laboratory (LLNL), Laboratoire de recherche sur le devenir des pollutions de sites radioactifs (IRSN/PSE-ENV/SEDRE/LELI), Service des déchets radioactifs et des transferts dans la géosphère (IRSN/PSE-ENV/SEDRE), Institut de Radioprotection et de Sûreté Nucléaire (IRSN)-Institut de Radioprotection et de Sûreté Nucléaire (IRSN), CEA-DAM, K&E Innovations, PSE-ENV/SEDRE/LELI, and Institut de Radioprotection et de Sûreté Nucléaire (IRSN)

Subjects
Molality, Alpha spectrometry, 010308 nuclear & particles physics, Chemistry, Health, Toxicology and Mutagenesis, Liquid scintillation counting, Radiochemistry, Public Health, Environmental and Occupational Health, Half-life, Isotope dilution, 01 natural sciences, Pollution, Article, Analytical Chemistry, Nuclear Energy and Engineering, Standard addition, 0103 physical sciences, [CHIM]Chemical Sciences, Radiology, Nuclear Medicine and imaging, 010306 general physics, Spectroscopy
Abstract

A new determination of the (229)Th half-life was made based on measurements of the (229)Th massic activity of a high-purity solution for which the (229)Th molality had previously been measured. The (229)Th massic activity was measured by direct comparison with SRM 4328C using 4παβ liquid scintillation counting, NaI counting, and standard addition liquid scintillation counting. The massic activity was confirmed by isotope dilution alpha spectrometry measurements. The calculated (229)Th half-life is (7825 ± 87) years (k = 2), which is shorter than the three most recent half-life determinations but is consistent with these values within uncertainties.

Published
2019
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3. Method for detecting and characterising actinide-bearing micro-particles in soils and sediment of the Fukushima Prefecture, Japan

Author

Jaime F. Angulo, Anne-Laure Fauré, Nina M. Griffiths, Hugo Jaegler, Yuichi Onda, Olivier Evrard, Agnes Moureau, Fabien Pointurier, Olivier Marie, Amélie Hubert, Laboratoire des Sciences du Climat et de l'Environnement [Gif-sur-Yvette] (LSCE), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ), Géochimie Des Impacts (GEDI), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ), DAM Île-de-France (DAM/DIF), Direction des Applications Militaires (DAM), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Université de Tsukuba = University of Tsukuba, Laboratoire de Radiotoxicologie (LRT), Commissariat à l'énergie atomique et aux énergies alternatives (CEA), ANR-11-RSNR-0002,AMORAD,AMORAD1(2011), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), and Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)

Subjects
Soil test, actinide-bearing particles, Health, Toxicology and Mutagenesis, Mineralogy, 010501 environmental sciences, [SDV.SA.SDS]Life Sciences [q-bio]/Agricultural sciences/Soil study, 01 natural sciences, Analytical Chemistry, law.invention, law, [SDU.STU.GC]Sciences of the Universe [physics]/Earth Sciences/Geochemistry, Nuclear power plant, Radiology, Nuclear Medicine and imaging, [SDU.ENVI]Sciences of the Universe [physics]/Continental interfaces, environment, Spectroscopy, 0105 earth and related environmental sciences, mass spectrometry, Micro particles, 010401 analytical chemistry, Public Health, Environmental and Occupational Health, Sediment, Actinide, Pollution, 0104 chemical sciences, Plume, Fukushima Dai-ichi Nuclear Power Plant accident, Actinides in the environment, Nuclear Energy and Engineering, 13. Climate action, Soil water, [SDE]Environmental Sciences, Environmental science, Solid State Nuclear Track Detector, [CHIM.RADIO]Chemical Sciences/Radiochemistry, microscope characterisation
Abstract

International audience; The Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident released limited amounts of actinides on soils of Japan. Characterisation of these particles is essential to determine the fate of actinides in the environment. The method presented in this paper, based on α-tracks detections, microscope observations and mass-spectrometry measurements, was designed to identify and characterize actinide-bearing particles in soil samples. The method was tested on a road dust sample collected in the main radioactive plume of the Fukushima region. Accordingly, α-tracks detection was demonstrated to provide a powerful technique to localise these particles and prepare their morphological, elemental and isotopic characterization.

Published
2019
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4. Reconstruction of uranium and plutonium isotopic signatures in sediment accumulated in the Mano Dam reservoir, Japan, before and after the Fukushima nuclear accident

Author

Silvia Diez-Fernández, Hugo Jaegler, Amélie Hubert, Fabien Pointurier, Alkiviadis Gourgiotis, Yuichi Onda, Olivier Evrard, J. Patrick Laceby, Seiji Hayashi, Hideki Tsuji, Hélène Isnard, Laboratoire des Sciences du Climat et de l'Environnement [Gif-sur-Yvette] (LSCE), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ), CEA/DAM, CEA/DEN, PSE-ENV/SEDRE/LELI, Institut de Radioprotection et de Sûreté Nucléaire (IRSN), National Institute for Environmental Science [Fukushima], Center for Research in Isotopes and Environmental Dynamics, Université de Tsukuba = University of Tsukuba, Extrèmes : Statistiques, Impacts et Régionalisation (ESTIMR), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ), The collection and the analysis of the sediment samples were funded by the TOFU (ANR-11-JAPN-001) and the AMORAD (ANR-11-RSNR-0002) projects, funded by the French National Research Agency (ANR, Agence Nationale de la Recherche). Hugo Jaegler received a PhD fellowship from the French Atomic Energy Commission (CEA, Commissariat à l’Energie Atomique et aux Energies Alternatives). The authors are grateful to the Fukushima Agricultural Technology Centre for providing the soil samples collected before the FDNPP accident. This work is IRSN Paterson platform contribution number 2., ANR-11-JAPN-0001,TOFU,Traçage des conséquences environnementales du tsunami provoqué par le séisme de TOhoku et de l'accident de FUkushima(2011), ANR-11-RSNR-0002,AMORAD,AMORAD1(2011), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Laboratoire de recherche sur le devenir des pollutions de sites radioactifs (IRSN/PSE-ENV/SEDRE/LELI), Service des déchets radioactifs et des transferts dans la géosphère (IRSN/PSE-ENV/SEDRE), Institut de Radioprotection et de Sûreté Nucléaire (IRSN)-Institut de Radioprotection et de Sûreté Nucléaire (IRSN), and Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)

Subjects
Geologic Sediments, Water Pollutants, Radioactive, Environmental Engineering, Fukushima Nuclear Accident, Health, Toxicology and Mutagenesis, 0208 environmental biotechnology, chemistry.chemical_element, 02 engineering and technology, 010501 environmental sciences, 01 natural sciences, law.invention, Japan, law, Radiation Monitoring, Nuclear power plant, Environmental Chemistry, Soil Pollutants, Radioactive, 0105 earth and related environmental sciences, Hydrology, Radionuclide, Public Health, Environmental and Occupational Health, Sediment, General Medicine, General Chemistry, Uranium, Pollution, Plutonium, 020801 environmental engineering, Actinides in the environment, chemistry, 13. Climate action, Major actinide, Cesium Radioisotopes, Nuclear Power Plants, [SDE]Environmental Sciences, Environmental science
Abstract

The Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident in Japan resulted in a major release of radionuclides into the environment. Compared to other radionuclides, few studies have investigated the fate of actinides in the environment. Accordingly, this research investigates the Pu composition in soil samples collected in paddy fields before and after the accident. Furthermore, the vertical distributions of Pu and U isotopic signatures, along with 137Cs activities, were measured in a sediment core collected in the Mano Dam reservoir, in the Fukushima Prefecture. Changes in the relative contributions of the major actinide sources (global fallout or FDNPP derived fallout) were investigated in sediment deposited in the reservoir. The distinct peak observed for all Pu isotope ratios (240Pu/239Pu, 241Pu/239Pu and 242Pu/239Pu) and for 137Cs concentrations in the sediment core was attributed to the Fukushima fallout, and coincided with the maximum atomic contribution of only 4.8 ± 1.0% of Pu from the FDNPP. Furthermore, 236U/238U ratios measured in the sediment core remained close to the global fallout signature indicating there was likely no U from the FDNPP accident detected in the sediment core. More research is required on the environmental dynamics of trace actinides in landscapes closer to the FDNPP where there are likely to be greater abundances of FDNPP-derived Pu and U.

Published
2019
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5. More than Five Percent Ionization Efficiency by Cavity Source Thermal Ionization Mass Spectrometry for Uranium Subnanogram Amounts

Author

Anne Trinquier, Bernard Bourdon, Anne-Laure Fauré, Colin Maden, Fabien Pointurier, Amélie Hubert, Maria Schönbächler, Laboratoire de Géologie de Lyon - Terre, Planètes, Environnement (LGL-TPE), École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut national des sciences de l'Univers (INSU - CNRS)-Université Jean Monnet - Saint-Étienne (UJM)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Géologie de Lyon - Terre, Planètes, Environnement [Lyon] (LGL-TPE), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Claude Bernard Lyon 1 (UCBL), and Université de Lyon-Université de Lyon-École normale supérieure - Lyon (ENS Lyon)

Subjects
Isotope, Chemistry, Nuclear forensics, 010401 analytical chemistry, Radiochemistry, chemistry.chemical_element, Thermal ionization mass spectrometry, Uranium, 010402 general chemistry, 01 natural sciences, 7. Clean energy, 0104 chemical sciences, Analytical Chemistry, Nuclear safeguards, [SDU]Sciences of the Universe [physics], Ionization
Abstract

Numerous applications require the precise analysis of U isotope relative enrichment in sample amounts in the sub-nanogram to picogram range, among those are nuclear forensics, nuclear safeguards, environmental survey and geosciences. However, conven-tional thermal ionization mass spectrometry (TIMS) yields U combined ionization and transmission efficiencies (i.e ratio of ions detected to sample atoms loaded) less than 0.1 or 2% depending on the loading protocol, motivating the development of sources capable of enhancing ionization. The new prototype cavity source TIMS at ETH offers improvements from 4 to 15 times in com-bined ionization and transmission efficiency compared to conventional TIMS, yielding up to 5.6 % combined efficiency. Uranium isotope ratios have been determined on reference standards in the 100 pg range bound to ion-exchange or extraction resin beads. For natural U standards, n(235U)/n(238U) ratios are measured to relative external precisions of 0.5 to 1.0 % (2RSD, 2

Published
2019
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6. Capabilities of laser ablation – ICP-TOF-MS coupling for isotopic analysis of individual uranium micrometric particles

Author

Anne-Claire Humbert, Amélie Hubert, Jean Aupiais, Fabien Pointurier, Olga Borovinskaya, Nicolas Dacheux, Martin Tanner, Anne-Laure Ronzani, Martin Rittner, DAM Île-de-France (DAM/DIF), Direction des Applications Militaires (DAM), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Tofwerk AG, Interfaces de Matériaux en Evolution (LIME), Institut de Chimie Séparative de Marcoule (ICSM - UMR 5257), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Accuracy and precision, Materials science, Laser ablation, Isotope, 010401 analytical chemistry, Analytical chemistry, chemistry.chemical_element, 02 engineering and technology, Uranium, 021001 nanoscience & nanotechnology, 01 natural sciences, 0104 chemical sciences, Analytical Chemistry, Time of flight, Linear range, chemistry, [CHIM.ANAL]Chemical Sciences/Analytical chemistry, Nuclide, Time-of-flight mass spectrometry, 0210 nano-technology, [CHIM.RADIO]Chemical Sciences/Radiochemistry, Spectroscopy, ComputingMilieux_MISCELLANEOUS
Abstract

Capabilities of laser ablation coupled to a time of flight ICP-MS (‘icpTOF’, Tofwerk) for direct isotopic analysis of U micrometric reference particles deposited on carbon disks were demonstrated. Thanks to the very high temporal resolution which allows quasi simultaneous measurement of all nuclides, the icpTOF is well-suited for the acquisition of the very short transient signals produced by laser ablation of μm-sized particles. With appropriate corrections of the background due to high peak tailing of the 238U isotope and selection of signals within the detector's linear range, excellent internal and external precisions (0.2–0.4%) for measurement of the 235U/238U ratios were obtained in the most favorable cases (same abundances for the two isotopes). These precisions are better than the values reported until now in the literature, even with laser ablation coupled with multi-collector ICP-MS (MC-ICP-MS). For particles from other reference materials with low abundances of 235U, equal or close to the one of natural U, precisions for 235U/238U ratio measurements (4–5%) were not as good as the ones reported for MC-ICP-MS, but better than the ones obtained with single collector ICP-MS. Minor isotope ratios (234U/238U and 236U/238U) were also successfully measured, although with limited precision and accuracy when the abundances of the minor isotopes are very low, in the 10−5 range. This work shows that laser ablation coupled to ICP-TOF-MS has a great potential for ultra-precise isotope ratio measurements provided that the ablated area contains enough analyte and that abundances between isotopes are of the same order of magnitude.

Published
2018
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7. Plutonium isotopic signatures in soils and their variation (2011-2014) in sediment transiting a coastal river in the Fukushima Prefecture, Japan

Author

Hugo Jaegler, Maëva Cirella, Yuichi Onda, Fabien Pointurier, Amélie Hubert, Olivier Evrard, J. Patrick Laceby, Laboratoire des Sciences du Climat et de l'Environnement [Gif-sur-Yvette] (LSCE), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ), Géochimie Des Impacts (GEDI), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ), DAM Île-de-France (DAM/DIF), Direction des Applications Militaires (DAM), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Université de Tsukuba = University of Tsukuba, ANR-11-RSNR-0002,AMORAD,AMORAD1(2011), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), and Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)

Subjects
Geologic Sediments, Water Pollutants, Radioactive, 010504 meteorology & atmospheric sciences, Health, Toxicology and Mutagenesis, chemistry.chemical_element, 010501 environmental sciences, [SDV.SA.SDS]Life Sciences [q-bio]/Agricultural sciences/Soil study, Toxicology, 01 natural sciences, Mass Spectrometry, Panoply, Soil, Japan, Rivers, Radiation Monitoring, Fukushima Nuclear Accident, Soil Pollutants, Radioactive, [SDU.ENVI]Sciences of the Universe [physics]/Continental interfaces, environment, 0105 earth and related environmental sciences, Radioisotopes, Radionuclide, Sediment, General Medicine, Contamination, Pollution, Plutonium, Plume, Deposition (aerosol physics), chemistry, 13. Climate action, [SDU]Sciences of the Universe [physics], Nuclear Power Plants, Environmental chemistry, Soil water, [SDE]Environmental Sciences, Erosion, Environmental science, [CHIM.RADIO]Chemical Sciences/Radiochemistry
Abstract

International audience; The Fukushima Daiichi Nuclear Power Plant (FDNPP) accident resulted in a significant release of radionuclides that were deposited on soils in Northeastern Japan. Plutonium was detected at trace levels in soils and sediments collected around the FDNPP. However, little is known regarding the spatial-temporal variation of plutonium in sediment transiting rivers in the region. In this study, plutonium isotopic compositions were first measured in soils (n = 5) in order to investigate the initial plutonium deposition. Then, plutonium isotopic compositions were measured on flood sediment deposits (n = 12) collected after major typhoon events in 2011, 2013 and 2014. After a thorough radiochemical purification, isotopic ratios ($^{240}$Pu/$^{239}$Pu, $^{241}$Pu/$^{239}$Pu and $^{242}$Pu/$^{239}$Pu) were measured with a Multi-Collector Inductively Coupled Mass Spectrometer (MC ICP-MS), providing discrimination between plutonium derived from global fallout, from atmospheric nuclear weapon tests, and plutonium derived from the FDNPP accident. Results demonstrate that soils with the most Fukushima-derived plutonium were in the main radiocaesium plume and that there was a variable mixture of plutonium sources in the flood sediment samples. Plutonium concentrations and isotopic ratios generally decreased between 2011 and 2014, reflecting the progressive erosion and transport of contaminated sediment in this coastal river during flood events. Exceptions to this general trend were attributed to the occurrence of decontamination works or the remobilisation of contaminated material during typhoons. The different plutonium concentrations and isotopic ratios obtained on three aliquots of a single sample suggest that the Fukushima-derived plutonium was likely borne by discrete plutonium-containing particles. In the future, these particles should be isolated and further characterized in order to better understand the fate of this long-lived radionuclide in the environment.

Published
2018
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8. Design of a prototype thermal ionization cavity source intended for isotope ratio analysis

Author

Colin Maden, Anne Trinquier, Amélie Hubert, Jörg Rickli, Anne-Laure Fauré, Bernard Bourdon, Fabien Pointurier, Laboratoire de Géologie de Lyon - Terre, Planètes, Environnement (LGL-TPE), École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut national des sciences de l'Univers (INSU - CNRS)-Université Jean Monnet - Saint-Étienne (UJM)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Géologie de Lyon - Terre, Planètes, Environnement [Lyon] (LGL-TPE), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Claude Bernard Lyon 1 (UCBL), and Université de Lyon-Université de Lyon-École normale supérieure - Lyon (ENS Lyon)

Subjects
Thermal ionization cavity, Analytical chemistry, chemistry.chemical_element, Thermal ionization, 02 engineering and technology, Thermal ionization mass spectrometry, Mass spectrometry, 01 natural sciences, Ion, chemistry.chemical_compound, Uranium oxide, Physical and Theoretical Chemistry, Instrumentation, Spectroscopy, Isotopes of uranium, Chemistry, Electron impact heating, 010401 analytical chemistry, Uranium, Ion optics, 021001 nanoscience & nanotechnology, Condensed Matter Physics, Ion source, 0104 chemical sciences, [SDU]Sciences of the Universe [physics], Ion source design, Ionization efficiency, 0210 nano-technology
Abstract

The design of a prototype thermal ionization cavity (TIC) source attached to the mass analyser of a MAT262 thermal ionization mass spectrometer is presented. In addition to a detailed calculation and experimental verification of the ion optics, the new design includes several innovative features that set it apart from previously reported TIC sources. The goal is to employ this new ion source for high-efficiency isotope ratio analysis. For uranium adsorbed to a single resin bead, an overall efficiency gain of about a factor of 10 compared to the same sample type analysed by state-of-the-art conventional thermal ionization mass spectrometry (TIMS) on a Triton instrument is reported (ions detected per atom loaded). First attempts at isotope ratio analysis of micrometre sized uranium oxide particles, as is commonly done for nuclear safeguards, seem to confirm the enhancement in overall efficiency and could help with the analysis of the minor uranium isotopes on such samples. (C) 2018 Elsevier B.V. All rights reserved.

Published
2018
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9. A new thorium-229 reference material

Author

Alkiviadis Gourgiotis, Ross W. Williams, Jaqueline L. Mann, Richard M. Essex, M. E. Bennett, William S. Kinman, and Amélie Hubert

Subjects
Molality, Radiation, Nuclear forensics, 010401 analytical chemistry, Analytical chemistry, Thorium, chemistry.chemical_element, Isotope dilution, 010403 inorganic & nuclear chemistry, 01 natural sciences, Article, 0104 chemical sciences, chemistry, Isotopes of thorium
Abstract

A new reference material was characterized for (229)Th molality and thorium isotope amount ratios. This reference material is intended for use in nuclear forensic analyses as an isotope dilution mass spectrometry spike. The reference material value and expanded uncertainty (k = 2) for the (229)Th molality is (1.1498 ± 0.0016) × 10(−10) mol g(−1) solution. The value and expanded uncertainty (k = 2) for the n((230)Th)/n((229)Th) ratio is (5.18 ± 0.26) × 10(−5) and the n((232)Th)/n((229)Th) ratio is (3.815 ± 0.092) × 10(−4).

Published
2017

10. Determination of the isotopic composition of micrometric uranium particles by UV femtosecond laser ablation coupled with sector-field single-collector ICP-MS

Author

Amélie Hubert, Ariane Donard, Fabien Pointurier, Anne-Claire Pottin, Christophe Pécheyran, Institut des sciences analytiques et de physico-chimie pour l'environnement et les materiaux (IPREM), and Université de Pau et des Pays de l'Adour (UPPA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Accuracy and precision, isotopic compn detn micrometric uranium particle, Isotopes of uranium, Isotope, 010401 analytical chemistry, Analytical chemistry, chemistry.chemical_element, 02 engineering and technology, UV femtosecond laser ablation ICP mass spectrometry coupling, Uranium, 021001 nanoscience & nanotechnology, 01 natural sciences, 0104 chemical sciences, Analytical Chemistry, Deposition (aerosol physics), Certified reference materials, chemistry, 13. Climate action, [CHIM.ANAL]Chemical Sciences/Analytical chemistry, 0210 nano-technology, Inductively coupled plasma mass spectrometry, Spectroscopy, Isotope analysis
Abstract

In this article, the coupling of a UV-fs-LA system with a sector-field ICP-MS for isotopic analysis of individual sub micrometric and micrometric uranium particles, especially for the measurement of minor isotopes (234U and 236U), is discussed. Ablation of uranium particles results in short (a few seconds) and highly noisy signals with sudden and extremely brief (

Published
2017
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11. Improving Precision and Accuracy of Isotope Ratios from Short Transient Laser Ablation-Multicollector-Inductively Coupled Plasma Mass Spectrometry Signals: Application to Micrometer-Size Uranium Particles

Author

Christophe Pécheyran, Ariane Donard, Amélie Hubert, Fanny Claverie, Sylvain Bérail, Fabien Pointurier, Institut des sciences analytiques et de physico-chimie pour l'environnement et les materiaux (IPREM), and Université de Pau et des Pays de l'Adour (UPPA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Accuracy and precision, Laser ablation, Isotope, Chemistry, 010401 analytical chemistry, Detector, Analytical chemistry, chemistry.chemical_element, 02 engineering and technology, Uranium, 021001 nanoscience & nanotechnology, Laser, 7. Clean energy, 01 natural sciences, 0104 chemical sciences, Analytical Chemistry, law.invention, law, [CHIM]Chemical Sciences, 0210 nano-technology, Faraday cage, Inductively coupled plasma mass spectrometry
Abstract

International audience; The isotope drift encountered on short transient signals measured by multicollector inductively coupled plasma mass spectrometry (MC-ICPMS) is related to differences in detector time responses. Faraday to Faraday and Faraday to ion counter time lags were determined and corrected using VBA data processing based on the synchronization of the isotope signals. The coefficient of determination of the linear fit between the two isotopes was selected as the best criterion to obtain accurate detector time lag. The procedure was applied to the analysis by laser ablation-MC-ICPMS of micrometer sized uranium particles (1–3.5 μm). Linear regression slope (LRS) (one isotope plotted over the other), point-by-point, and integration methods were tested to calculate the 235U/238U and 234U/238U ratios. Relative internal precisions of 0.86 to 1.7% and 1.2 to 2.4% were obtained for 235U/238U and 234U/238U, respectively, using LRS calculation, time lag, and mass bias corrections. A relative external precision of 2.1% was obtained for 235U/238U ratios with good accuracy (relative difference with respect to the reference value below 1%).

Published
2016
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12. Determination of ionization efficiencies of thermal ionization cavity sources by numerical simulation of charged particle trajectories including space charge

Author

Anne-Laure Fauré, Amélie Hubert, Colin Maden, Fabien Pointurier, Bernard Bourdon, Heinrich Baur, Laboratoire de Géologie de Lyon - Terre, Planètes, Environnement (LGL-TPE), École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut national des sciences de l'Univers (INSU - CNRS)-Université Jean Monnet - Saint-Étienne (UJM)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Géologie de Lyon - Terre, Planètes, Environnement [Lyon] (LGL-TPE), École normale supérieure - Lyon (ENS Lyon)-Université Claude Bernard Lyon 1 (UCBL), and Université de Lyon-Université de Lyon-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Thermal ionization cavity, Thermal ionization, 02 engineering and technology, 01 natural sciences, Space charge, Ionization, Physical and Theoretical Chemistry, Instrumentation, Spectroscopy, Electron ionization, Charged particle optics, Chemistry, 010401 analytical chemistry, Cavity geometry, Plasma, 021001 nanoscience & nanotechnology, Condensed Matter Physics, Charged particle, Ion source, 0104 chemical sciences, [SDU]Sciences of the Universe [physics], Ionization efficiency, Atomic physics, 0210 nano-technology, Cavity wall
Abstract

An in-house developed code, Sofie, and the methods used for numerical determination of the ionization efficiency of thermal ionization cavity (TIC) sources up to intermediate temperatures (\textless2500 K for cavity dimensions of a few millimetres) are presented, thus, creating a tool to identify cavity geometries offering better ionization efficiencies and to aid in matching the ion beam produced by a TIC source to the ion optics of a beam line or a mass analyser as used in conventional thermal ionization mass spectrometry (TIMS). Essential is the code's ability to approximate the solution of Poisson's equation, in which the space charge predominantly originates from electrons thermally emitted from the inner cavity walls. The assumption of a quasi-neutral plasma forming in the volume of the cavity is no longer valid at lower temperatures and/or cavity dimensions, and charged particles can be regarded as moving freely throughout the cavity only interacting via the electrostatic potential shaped by the particles' space charge. Under such conditions the geometry of the cavity has got a large effect on the ionization efficiency of sample atoms loaded into the source. The code also allows the simulation of surface adsorption and re-emission of various particle species simultaneously, making the calculation of ionization efficiencies possible by determining the currents of sample ions and neutral atoms out of the cavity. The validity of the code is successfully demonstrated by simulating problem sets, for which analytical solutions exist, and also by reproducing experimental data from TIC sources found in the literature. The necessity of including space charge in such simulations is demonstrated. A non-exhaustive search for a best cavity geometry has been performed and a geometry has been identified that could enhance the ionization efficiency by up to a factor of 100 over the ionization efficiency of the Saha-Langmuir equation, which corresponds to the efficiency achievable with conventional flat filament TIMS sources. (C) 2016 Elsevier B.V. All rights reserved.

Published
2016
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13. Novel Insights into Fukushima Nuclear Accident from Isotopic Evidence of Plutonium Spread along Coastal Rivers

Author

Amélie Hubert, Sophie Ayrault, Yuichi Onda, Caroline Chartin, Fabien Pointurier, Anne-Claire Pottin, Hugo Lepage, Philippe Bonté, J. Patrick Laceby, Irène Lefèvre, Olivier Evrard, Laboratoire des Sciences du Climat et de l'Environnement [Gif-sur-Yvette] (LSCE), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ), Géochimie Des Impacts (GEDI), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ), DAM Île-de-France (DAM/DIF), Direction des Applications Militaires (DAM), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Université de Tsukuba = University of Tsukuba, Centre Georges Lemaître for Earth and Climate Research [Louvain] (TECLIM), Earth and Life Institute [Louvain-La-Neuve] (ELI), Université Catholique de Louvain = Catholic University of Louvain (UCL)-Université Catholique de Louvain = Catholic University of Louvain (UCL), CEA (Direction des Relations Internationales) and UVSQ (Bonus de Qualité Internationale) grants., ANR-11-JAPN-0001,TOFU,Traçage des conséquences environnementales du tsunami provoqué par le séisme de TOhoku et de l'accident de FUkushima(2011), ANR-11-RSNR-0002,AMORAD,AMORAD1(2011), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), and Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)

Subjects
Radioactive Fallout, Water Pollutants, Radioactive, Fukushima Nuclear Accident, chemistry.chemical_element, 010501 environmental sciences, 010403 inorganic & nuclear chemistry, 01 natural sciences, Pacific ocean, Japan, Rivers, Radiation Monitoring, [SDU.STU.GC]Sciences of the Universe [physics]/Earth Sciences/Geochemistry, Environmental Chemistry, [SDU.ENVI]Sciences of the Universe [physics]/Continental interfaces, environment, 0105 earth and related environmental sciences, Radioisotopes, Radionuclide, Pacific Ocean, Isotope, Radiochemistry, Sediment, General Chemistry, Plutonium, 0104 chemical sciences, Plume, chemistry, 13. Climate action, Global distribution, [SDU]Sciences of the Universe [physics], Nuclear Power Plants, Environmental chemistry, [SDE]Environmental Sciences, Environmental science, [CHIM.RADIO]Chemical Sciences/Radiochemistry
Abstract

International audience; The Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident led to important releases of radionuclides into the environment, and trace levels of plutonium (Pu) were detected in northeastern Japan. However, measurement of Pu isotopic atom and activity ratios is required to differentiate between the contributions of global nuclear test fallout and FDNPP emissions. In this study, we used a double-focusing sector field ICP-MS to measure Pu atom and activity ratios in recently deposited sediment along rivers draining the most contaminated part of the inland radioactive plume. Results showed that plutonium isotopes (i.e., 239 Pu, 240 Pu, 241 Pu, and 242 Pu) were detected in all samples, although in extremely low concentrations. The 241 Pu/ 239 Pu atom ratios measured in sediment deposits (0.0017-0.0884) were significantly higher than the corresponding values attributed to the global fallout (0.00113±0.00008 on average for the Northern Hemisphere between 31°-71°N, Kelley, J.M.; Bond, L.A.; Beasley, T.M., Global distribution of Pu isotopes and 237 Np, Sci. Total. Env., 1999, 237/238, 483-500). The results indicated the presence of Pu from FDNPP, in slight excess compared to the Pu background from global fallout that represented up to ca. 60% of Pu in the analyzed samples. These results demonstrate that this radionuclide has been transported relatively long distances (∼45 km) from FDNPP and been deposited in rivers representing a potential source of Pu to the ocean. In future, the high 241 Pu/ 239 Pu atom ratio of the Fukushima accident sourced-Pu should be measured to quantify the supply of continental-originating material from Fukushima Prefecture to the Pacific Ocean.

Published
2014
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14. Polyatomic interferences in plutonium determination in the femtogram range by double-focusing sector-field ICP-MS.

Author

Fabien Pointurier, Amélie Hubert, Anne-Laure Fauré, Philippe Hémet, and Anne-Claire Pottin

Subjects
*PLUTONIUM isotopes, *INDUCTIVELY coupled plasma mass spectrometry, *POLYATOMIC molecules, *HEAVY elements, *HAFNIUM, *BISMUTH, *TRACE analysis, *CHEMICAL reagents
Abstract

The determination of very low concentrations of plutonium, in the femtogram per millilitre range, in environmental samples using ICP-MS can be interfered by polyatomic species containing heavy elements, from hafnium to bismuth. Mass-to-charge ratios of these polyatomic species are very close to the ones of the plutonium isotopes and cannot be separated from them in the low resolution mode currently used for trace analysis. In this paper, we present an evaluation of the extent and impact of these interferences on the background at masses of plutonium isotopes 239Pu and 240Pu, based on measurement of environmental samples for three years using a double-focusing sector-field ICP-MS. We demonstrate that these molecular interferences, especially the ones involving lead, mercury, and iridium through species PbO2+, ArHg+, IrO3+, must be considered as the additional background induced by these interferences (on average for all interferences respectively ∼1.2 and ∼1.9 counts s−1at 239 and 240 atomic mass units) is often higher than the instrumental background measured with deionised water acidified at 2% by ultra-pure grade HNO3(∼0.4 counts s−1), and are generally of the same order as other usual sources of background for low-level plutonium analysis by ICP-MS, i.e.242Pu tracer isotopic impurities, 238U hydrides and peak tail. Thus, if not corrected, these polyatomic interferences may lead to false detection of femtogram amounts of plutonium or overestimation of results. The extents of formation of the main polyatomic species are highly variable from one analysis to the other, over one or two orders of magnitude, depending on instrumental settings. Chemical purification procedures are very efficient in eliminating the greater part of heavy elements present in the initial samples. However, these procedures also bring heavy elements into the final sample solutions through contamination by the atmosphere, glassware and reagents. [ABSTRACT FROM AUTHOR]

Published
2011
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15. Assessment of plutonium measurement in the femtogram range by ICP-MS; correction from interfering polyatomic species.

Author

Fabien Pointurier, Philippe Hémet, and Amélie Hubert

Subjects
METALS, HEAVY metals, SOIL composition, HEAVY metal content of sediments
Abstract

In the frame of the low level plutonium measurements performed by ICP-MS on environmental samples in support of the International Atomic Energy Agency’s safeguards program, we observe that background in the actinide mass range for the sample solutions is always higher than for blanks made of deionised water and ultra-pure grade nitric acid. This additional background is due to polyatomic species including heavy metals like Pb, Hg, Ir, etc., which remain in sample solutions despite the purification chemistry that is systematically carried out. As Pu content in the samples may be extremely low—in the femtogram (10–15 g) range—it is of uttermost importance to estimate detection limits as accurately as possible and to minimize risks of false detections. We propose an approach that consists of systematically correcting for contributions of polyatomic species to the background. To accomplish this, it is necessary to estimate all the formation rates of polyatomic species consisting of a “heavy metal” (from Hf to Bi) and one or more atoms, such as O, N, Ar, Cl, etc., that have total masses corresponding to those of Pu isotopes. Although the formation rates can vary largely with settings and analytical conditions, this study allows identification of the higher formation rates. The analytical procedure must also include, in addition to Pu and background masses, the measurement of one isotope for each “heavy metal”. Starting from examples of real sample measurements, we compare various calculation models for background and detection limits and prove that the one taking into account corrections from polyatomic interferences gives the most accurate results and minimises the risk of false detection for ultra low-level Pu measurements in the fg range. [ABSTRACT FROM AUTHOR]

Published
2007

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