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

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Abstract

The radiochronometric model age is an important signature in nuclear forensic analysis. Recent studies have illustrated the need for controlled experiments on the behavior of decay products during uranium metal casting to provide a foundation for interpretation of discordant model ages. A variety of uranium metal and alloy samples cast under known conditions were analysed by three laboratories. This work is the first multi-laboratory study of its kind to explore how these progeny isotopes are chemically fractionated from uranium metal during casting. The intercomparison allowed for capability demonstration and method development on samples and provided data to increase our understanding of the behavior of decay progeny in these complex systems.

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Acknowledgements

We thank AWE for funding this work at AWE. LANL and LLNL thank the NA-83 Office of Nuclear Forensics for funding the laboratory intercomparison. A portion of this work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344, LLNL document ID - LLNL-JRNL-834140. Work performed at Los Alamos National Laboratory (operated by Triad National Security, LLC) was performed under the auspices of the U.S. Department of Energy under contract 89233218CNA000001. LANL document ID - LA-UR-22-26640

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Authors and Affiliations

  1. AWE, AWE Aldermaston, RG7 4PR, Reading, UK

    Matthew A. Higginson, Samuel T. J. Cross, James A. Dunne & Chris R. D. Gilligan

  2. LANL, Nuclear and Radiochemistry Group, Chemistry Division, Los Alamos National Laboratory, 87545, Los Alamos, NM, USA

    Theresa M. Kayzar-Boggs, Joanna S. Denton, Mark A. Edwards, Matthew E. Sanborn & Allison M. Wende

  3. LLNL, Nuclear and Chemical Sciences Division, Lawrence Livermore National Laboratory, 7000 East Avenue, 94551, Livermore, CA, USA

    Christine Y. Chen, Charlotte Eng, Amy M. Gaffney, Maya N. Morris & John M. Rolison

Authors
  1. Matthew A. Higginson
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  2. Theresa M. Kayzar-Boggs
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  3. Christine Y. Chen
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Contributions

M.H., A.M.G., C.Y.C. and T.K.-B. were lead investigators for the intercomparison. J.D., S.C., C.G., J.D., M.A.E., M.S. and A.W. were involved in the formal analysis and investigation and review and editing of the manuscript. C.Y.C. performed radiochronometric analyses by LLNL and led the Pa-Nb separations method development work with assistance from M.N.M. and expertise by J.M.Rolison and A.G. C.Y.C. also performed microscopy on samples guided by expertise of C. Eng. Higginson: Funding Acquisition, Conceptualization, Data Curation, Formal Analysis, Investigation, Methodology, Project Administration, Software, Supervision, Validation, Visualization, Writing– Review and Editing. Kayzar-Boggs: Conceptualization, Funding Acquisition, Data Curation, Formal Analysis, Investigation, Methodology, Project Administration, Software, Supervision, Validation, Visualization, Writing – Review and Editing. Chen: Conceptualization, Data Curation, Formal Analysis, Investigation, Methodology, Project Administration, Supervision, Validation, Visualization, Writing – Review and Editing. Cross: Formal Analysis, Investigation, Writing – Review and Editing. Denton: Formal Analysis, Investigation, Methodology, Writing – Review and Editing. Dunne: Formal Analysis, Investigation, Writing – Review and Editing. Edwards: Formal Analysis, Investigation, Writing – Review and Editing. Eng: Investigation. Gaffney: Conceptualization, Funding Acquisition, Project Administration, Resources, Supervision, Writing – Review and Editing. Gilligan: Formal Analysis, Investigation, Writing – Review and Editing. Morris: Investigation, Methodology. Rolison: Conceptualization, Investigation, Methodology, Supervision. Sanborn: Formal Analysis, Investigation, Writing – Review and Editing. Wende: Formal Analysis, Investigation, Writing – Review and Editing.

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Correspondence to Matthew A. Higginson.

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Higginson, M.A., Kayzar-Boggs, T.M., Chen, C.Y. et al. Establishing discordance as a radiochronometric signature for nuclear forensic investigations: a multi-laboratory intercomparison exercise. J Radioanal Nucl Chem 331, 4799–4815 (2022). https://doi.org/10.1007/s10967-022-08428-5

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