Establishing discordance as a radiochronometric signature for nuclear forensic investigations: a multi-laboratory intercomparison exercise

Higginson, Matthew; Kayzar-Boggs, Theresa M.; Chen, Christine Y.; Cross, Samuel T. J.; Denton, Joanna S.; Dunne, James A.; Edwards, Mark A.; Eng, Charlotte; Gaffney, Amy M.; Gilligan, Chris; Morris, Maya N.; Rolison, John M.; Sanborn, M. E.; Wende, Allison M.

doi:10.1007/s10967-022-08428-5

Cited by 6 publications

(10 citation statements)

References 32 publications

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“…In this case, the divergent ages were thought to arise from the chemical separation of thorium and uranium that occurred during uranium metal casting. A more recent study by Higginson et al supports the finding that uranium metal casting fractionates Th from uranium more completely than Pa and suggests that such discordant chronometers can provide important insights into processing history …”

Section: Resultsmentioning

confidence: 86%

Trace Actinide Signatures of a Bulk Neptunium Sample

et al. 2023

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In nuclear forensic analyses, measurements of actinide elements in a sample can assist with identifying interdicted or unknown materials. While these radiochemical signatures have been extensively investigated in uranium materials, less is known about bulk neptunium samples. This paper describes the measurement of trace actinide concentrations and isotopic profiles in a 237Np oxide sample. Uranium, plutonium, americium, and curium concentrations and isotopic profiles in the sample were determined and deemed potentially useful for distinguishing different sources of 237Np. Several different potential radiochronometry systems were also investigated; discordant results indicate that the Np sample was never completely purified of other actinide elements, or that subsequent contamination of the sample occurred. Few prior studies of neptunium materials have been reported, and these data suggest that trace actinide constituents could provide unique signatures to identify material out of regulatory control.

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Section: Resultsmentioning

confidence: 86%

Trace Actinide Signatures of a Bulk Neptunium Sample

et al. 2023

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“…After AWE identified uranium materials satisfying the criteria for the interlaboratory investigation [ 18 ], subsamples (~ 0.5–1.0 g) of two unique depleted U–Nb alloys, Alloy-1 and Alloy-2, were prepared and distributed to each participating laboratory (Fig. 2 ).…”

Section: Methods Developmentmentioning

confidence: 99%

“…In addition, discordance may also provide more nuanced information about a sample’s history; the observation that discordance is more common in materials with impurities and complex production histories suggests that these aspects have an influence on progeny nuclide fractionation [ 14 , 15 ]. Thus, with further research, characteristic patterns of discordance could be harnessed as diagnostic signatures of specific uranium manufacturing processes involved in an unknown material’s production, such as bomb reduction, metal casting, remelting, recycling, or alloying with other elements [ 17 , 18 ].…”

Section: Introductionmentioning

confidence: 99%

“…To this end, here we present new analytical methods that were developed for an investigation of 231 Pa– 235 U and 230 Th– 234 U model age discordance in uranium-niobium metal alloys. This work represents the first published attempt to analyze U–Nb metal alloys for radiochronometry and was conducted as part of a multi-laboratory collaboration between the Atomic Weapons Establishment (AWE), Lawrence Livermore National Laboratory (LLNL), and Los Alamos National Laboratory (LANL), as described in Higginson et al [ 18 ]. For this collaboration, AWE distributed to each laboratory a set of depleted uranium metals which included two U–Nb metal alloys cast by vacuum induction melting and vacuum arc remelting, two common industrial-scale uranium casting processes [ 19 ].…”

Section: Introductionmentioning

confidence: 99%

“…U–Nb metal alloys possess properties that are more desirable for various applications compared to their pure uranium metal counterparts, such as oxidation and corrosion resistance and improved ductility for shaping into specific geometries [ 20 – 22 ]. These samples were selected because documentation of their casting history was available [ 18 ]. We refer the reader to the companion article by Higginson et al (2022) for a detailed description of the U–Nb metal alloy production histories and discussion of model age discordance in cast uranium metals.…”

Section: Introductionmentioning

confidence: 99%

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Separation of protactinium from uranium-niobium alloys for 231Pa–235U radiochronometry in nuclear forensic investigations

Chen

Higginson

Kayzar-Boggs

et al. 2023

J Radioanal Nucl Chem

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The isolation and purification of protactinium from uranium materials is essential for 231 Pa– 235 U radiochronometry, but separating Pa from uranium-niobium alloys, a common material in the nuclear fuel cycle, is challenging due to the chemical similarity of Pa and Nb. Here we present three resin chromatography separation techniques for isolating Pa from U and Nb which were independently developed by three different laboratories through ad hoc adaptations of standard operating procedures. Our results underscore the need for and value of purification methods suitable for a diversity of uranium-based materials to ensure the operational readiness of nuclear forensics laboratories. Supplementary Information The online version contains supplementary material available at 10.1007/s10967-023-08928-y.

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