Neutron capture signatures determined from gadolinium isotope compositions of uranium ore concentrates using MC-ICPMS

Shollenberger, Quinn R.; Herbst, Ashley K.; Johnson, Adelicia F.; Render, Jan; Brennecka, Gregory A.

doi:10.1007/s10967-025-10230-y

Neutron capture signatures determined from gadolinium isotope compositions of uranium ore concentrates using MC-ICPMS

Journal Article · Wed Jul 16 00:00:00 EDT 2025 · Journal of Radioanalytical and Nuclear Chemistry

DOI:https://doi.org/10.1007/s10967-025-10230-y· OSTI ID:2585324

^[1]; Herbst, Ashley K. ^[2]; Johnson, Adelicia F. ^[3]; Render, Jan ^[1]; Brennecka, Gregory A. ^[1]

Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
Arizona State Univ., Tempe, AZ (United States)
Univ. of California, Santa Cruz, CA (United States)

We present Gd isotope compositions on 25 well-characterized uranium ore concentrates (UOCs). About half the UOCs have isotope depletions in ¹⁵⁷Gd coupled with anticorrelated excesses in ¹⁵⁸Gd due to neutron capture effects. UOCs from older ore bodies and with higher U contents show larger neutron capture effects than UOCs from younger ore bodies with lower U contents. These Gd data are correlated with their previously measured Sm isotope compositions, and we use the Sm data to estimate the neutron fluence of these samples. In conclusion, this work demonstrates how Gd isotope signatures can be employed as a new tool for nuclear forensics.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 2585324

Report Number(s):: LLNL--JRNL-2003812

Journal Information:: Journal of Radioanalytical and Nuclear Chemistry, Journal Name: Journal of Radioanalytical and Nuclear Chemistry Journal Issue: 7 Vol. 334; ISSN 1588-2780; ISSN 0236-5731

Publisher:: Springer Science and Business Media LLCCopyright Statement

Country of Publication:: United States

Language:: English

References (34)

Investigation of the sample characteristics needed for the determination of the origin of uranium-bearing materials Švedkauskaitė-LeGore, J.; Rasmussen, G.; Abousahl, S. Journal of Radioanalytical and Nuclear Chemistry, Vol. 278, Issue 1 https://doi.org/10.1007/s10967-007-7215-y	journal	June 2008
Identification of uranium signatures relevant for nuclear safeguards and forensics Varga, Zsolt; Krajkó, Judit; Peńkin, Maxim Journal of Radioanalytical and Nuclear Chemistry, Vol. 312, Issue 3 https://doi.org/10.1007/s10967-017-5247-5	journal	April 2017
A search for fossil nuclear reactors in the Alligator River Uranium Field, Australia: Constraints from Sm, Gd and Nd isotopic studies Maas, R.; McCulloch, M. T. Chemical Geology, Vol. 88, Issue 3-4 https://doi.org/10.1016/0009-2541(90)90095-O	journal	November 1990
The Oklo natural reactor: Cumulative fission yields and retentivity of the symmetric mass region fission products De Laeter, J. R.; Rosman, K. J. R.; Smith, C. L. Earth and Planetary Science Letters, Vol. 50, Issue 1 https://doi.org/10.1016/0012-821X(80)90135-1	journal	October 1980
High fluences of neutrons determined from Sm and Gd isotopic compositions in aubrites Hidaka, Hiroshi; Ebihara, Mitsuru; Yoneda, Shigekazu Earth and Planetary Science Letters, Vol. 173, Issue 1-2 https://doi.org/10.1016/S0012-821X(99)00221-6	journal	November 1999
Neutron capture effects on Sm and Gd isotopes in uraninites Hidaka, Hiroshi; Gauthier-Lafaye, Francois Geochimica et Cosmochimica Acta, Vol. 65, Issue 6 https://doi.org/10.1016/S0016-7037(00)00567-6	journal	March 2001
Natural fission reactors in the Franceville basin, Gabon: A review of the conditions and results of a “critical event” in a geologic system Gauthier-Lafaye, F.; Holliger, P.; Blanc, P. -L. Geochimica et Cosmochimica Acta, Vol. 60, Issue 23 https://doi.org/10.1016/S0016-7037(96)00245-1	journal	December 1996
Geochemical and Neutronic Characteristics of the Natural Fossil Fission Reactors at Oklo and Bangombé, Gabon Hidaka, Hiroshi; Holliger, Philippe Geochimica et Cosmochimica Acta, Vol. 62, Issue 1 https://doi.org/10.1016/S0016-7037(97)00319-0	journal	January 1998
Attribution of uranium ore concentrates using elemental and anionic data Keegan, Elizabeth; Wallenius, Maria; Mayer, Klaus Applied Geochemistry, Vol. 27, Issue 8 https://doi.org/10.1016/j.apgeochem.2012.05.009	journal	August 2012
Trace element and U isotope analysis of uraninite and ore concentrate: Applications for nuclear forensic investigations Spano, Tyler L.; Simonetti, Antonio; Balboni, Enrica Applied Geochemistry, Vol. 84 https://doi.org/10.1016/j.apgeochem.2017.07.003	journal	September 2017
Molybdenum isotope compositions of uranium ore concentrates by double spike MC-ICP-MS Rolison, John M.; Druce, Matthew; Shollenberger, Quinn R. Applied Geochemistry, Vol. 103 https://doi.org/10.1016/j.apgeochem.2019.03.001	journal	April 2019
The nuclear field shift effect in chemical exchange reactions Fujii, Toshiyuki; Moynier, Frédéric; Albarède, Francis Chemical Geology, Vol. 267, Issue 3-4 https://doi.org/10.1016/j.chemgeo.2009.06.015	journal	September 2009
Nuclear field shift in natural environments Moynier, Frédéric; Fujii, Toshiyuki; Brennecka, Gregory A. Comptes Rendus Geoscience, Vol. 345, Issue 3 https://doi.org/10.1016/j.crte.2013.01.004	journal	March 2013
Natural variations in uranium isotope ratios of uranium ore concentrates: Understanding the 238U/235U fractionation mechanism Brennecka, Gregory A.; Borg, Lars E.; Hutcheon, Ian D. Earth and Planetary Science Letters, Vol. 291, Issue 1-4 https://doi.org/10.1016/j.epsl.2010.01.023	journal	March 2010
Rhenium Isotope Reconnaissance of Uranium Ore Concentrates Sullivan, Daniel L.; Brennecka, Gregory A.; Grant, Katherine E. Earth and Planetary Science Letters, Vol. 644 https://doi.org/10.1016/j.epsl.2024.118898	journal	October 2024
Sm and Gd isotopic shifts of Apollo 16 and 17 drill stem samples and their implications for regolith history Hidaka, Hiroshi; Yoneda, Shigekazu Geochimica et Cosmochimica Acta, Vol. 71, Issue 4 https://doi.org/10.1016/j.gca.2006.10.015	journal	February 2007
Uranium and Sm isotope studies of the supergiant Olympic Dam Cu–Au–U–Ag deposit, South Australia Kirchenbaur, Maria; Maas, Roland; Ehrig, Kathy Geochimica et Cosmochimica Acta, Vol. 180 https://doi.org/10.1016/j.gca.2016.01.035	journal	May 2016
Investigations for determination of Gd and Sm isotopic compositions in spent nuclear fuels samples by MC ICPMS Isnard, H.; Brennetot, R.; Caussignac, C. International Journal of Mass Spectrometry, Vol. 246, Issue 1-3 https://doi.org/10.1016/j.ijms.2005.08.008	journal	November 2005
The state of nuclear forensics Kristo, Michael J.; Tumey, Scott J. Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 294 https://doi.org/10.1016/j.nimb.2012.07.047	journal	January 2013
Application of neodymium isotope ratio measurements for the origin assessment of uranium ore concentrates Krajkó, Judit; Varga, Zsolt; Yalcintas, Ezgi Talanta, Vol. 129 https://doi.org/10.1016/j.talanta.2014.06.022	journal	November 2014
Samarium isotope compositions of uranium ore concentrates: A novel nuclear forensic signature Shollenberger, Quinn R.; Borg, Lars E.; Ramon, Erick C. Talanta, Vol. 221 https://doi.org/10.1016/j.talanta.2020.121431	journal	January 2021
Determining provenance of uranium ore concentrates using ¹⁴³Nd/¹⁴⁴Nd McLoughlin, Victoria E. Devlin; Schollenberger, Quinn R.; Brennecka, Gregory A. Talanta, Vol. 253 https://doi.org/10.1016/j.talanta.2022.124088	journal	November 2022
Trends and perspectives in Nuclear Forensic Science Varga, Z.; Wallenius, M.; Krachler, M. TrAC Trends in Analytical Chemistry, Vol. 146 https://doi.org/10.1016/j.trac.2021.116503	journal	January 2022
Determination of the Isotopic Compositions of Samarium and Gadolinium by Thermal Ionization Mass Spectrometry Hidaka, H.; Ebihara, M.; Shima, M. Analytical Chemistry, Vol. 67, Issue 8 https://doi.org/10.1021/ac00104a021	journal	April 1995
Application of Lead and Strontium Isotope Ratio Measurements for the Origin Assessment of Uranium Ore Concentrates Varga, Zsolt; Wallenius, Maria; Mayer, Klaus Analytical Chemistry, Vol. 81, Issue 20 https://doi.org/10.1021/ac901100e	journal	October 2009
Ultra-high-precision Nd-isotope measurements of geological materials by MC-ICPMS Saji, Nikitha Susan; Wielandt, Daniel; Paton, Chad Journal of Analytical Atomic Spectrometry, Vol. 31, Issue 7 https://doi.org/10.1039/C6JA00064A	journal	January 2016
High-precision Sm isotope analysis by thermal ionisation mass spectrometry for large meteorite samples (>1 g) Frossard, Paul; Ball, James M. J.; Schönbächler, Maria Journal of Analytical Atomic Spectrometry, Vol. 40, Issue 1 https://doi.org/10.1039/D4JA00301B	journal	January 2025
Heterogeneous Isotopic Anomalies of sm and gd in the Norton County Meteorite: Evidence for Irradiation from the Active Early sun Hidaka, Hiroshi; Kondo, Tomoyo; Yoneda, Shigekazu The Astrophysical Journal, Vol. 746, Issue 2 https://doi.org/10.1088/0004-637X/746/2/132	journal	February 2012
Separation of Heavy Lanthanoids by Flash Column Chromatography for Precise Determination of Er and Yb Isotope Compositions in Rock Samples Yokoyama, Tetsuya; Fukai, Ryota; Nakahara, Masaki Geostandards and Geoanalytical Research, Vol. 44, Issue 2 https://doi.org/10.1111/ggr.12317	journal	March 2020
Origin of uranium deposits revealed by their rare earth element signature: Origin of U deposits revealed by the rare earth elements Mercadier, Julien; Cuney, Michel; Lach, Philippe Terra Nova, Vol. 23, Issue 4 https://doi.org/10.1111/j.1365-3121.2011.01008.x	journal	May 2011
Nuclear Forensic Science: Analysis of Nuclear Material Out of Regulatory Control Kristo, Michael J.; Gaffney, Amy M.; Marks, Naomi Annual Review of Earth and Planetary Sciences, Vol. 44, Issue 1 https://doi.org/10.1146/annurev-earth-060115-012309	journal	June 2016
Origin assessment of uranium ore concentrates based on their rare-earth elemental impurity pattern Varga, Zsolt; Wallenius, Maria; Mayer, Klaus Radiochimica Acta, Vol. 98, Issue 12 https://doi.org/10.1524/ract.2010.1777	journal	January 2010
Chemical separation and determination of the isotopic compositions of dysprosium, erbium and ytterbium in geochemical materials by thermal ionization mass spectrometry Mizutani, Yuki; Hidaka, Hiroshi; Yoneda, Shigekazu GEOCHEMICAL JOURNAL, Vol. 54, Issue 6 https://doi.org/10.2343/geochemj.2.0609	journal	January 2020
Isotopic Evidence for Multi-stage Cosmic-ray Exposure Histories of Lunar Meteorites: Long Residence on the Moon and Short Transition to the Earth Hidaka, Hiroshi; Sakuma, Keisuke; Nishiizumi, Kunihiko The Astronomical Journal, Vol. 153, Issue 6 https://doi.org/10.3847/1538-3881/aa7139	journal	June 2017

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