Synthesis and characterization of isotopically barcoded nickel, molybdenum, and tungsten taggants for intentional nuclear forensics

Journal Article · Wed Dec 18 00:00:00 EST 2024 · Talanta

DOI:https://doi.org/10.1016/j.talanta.2024.127425· OSTI ID:2520061

Bergin, Rachel ^[1]; Samperton, Kyle ^[1]; Bronikowski, Michael ^[1]; Hoar, Eric ^[1]; Rolison, John ^[2]; Shollenberger, Quinn ^[2]; Marks, Naomi ^[2]; Wellons, Matthew ^[1]; Scott, Spencer ^[1]

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1. Savannah River National Laboratory (SRNL), Aiken, SC (United States)
2. Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Intentional nuclear forensics is a concept wherein the deliberate addition of benign and persistent material signatures to nuclear material can be used to reduce the time between the discovery of material outside of regulatory control and determination of its original provenance. One concept within intentional nuclear forensics involves the use of perturbed stable isotopes to generate unique isotope ratio “barcodes” to encode information (e.g., production batch, location, etc.) and track material throughout the nuclear fuel cycle. Synthesis of taggant species of nickel (Ni), molybdenum (Mo), and tungsten (W) was undertaken via a double-spike mechanism, wherein two highly enriched isotopes of interest per elemental taggant were mixed to form an enriched “double-spike” which was subsequently isotopically diluted with bulk material having a natural isotopic composition. Two taggant species perturbing isotopic ratios, alpha (α) and beta (β), for each of Ni, Mo, and W were synthesized. Independent measurements of double spikes and alpha and beta taggant species agreed within uncertainty and are clearly resolvable from natural compositions. High-precision analyses were independently performed by MC-ICP-MS at two U.S. National Laboratories, with consensus values and uncertainties calculated for all samples. Observed isotopic perturbations in the final taggant species measured on the order of hundreds to thousands of permille (‰) with respect to natural for isotope ratios of interest (e.g., ⁶⁰Ni/⁵⁸Ni, ¹⁰⁰Mo/⁹⁸Mo, ¹⁸⁶W/¹⁸³W). Discrepancies between modeled and measured isotopic compositions were observed and are largely attributed to imprecise vendor assay values for starting materials. Using measured starting material compositions as inputs for the mixing model improved the level of agreement between predicted and measured α and β taggant isotope ratios. Overall, characterization of all taggant species demonstrates that this “barcode” concept could have viability for use in nuclear forensics. Finally, it is expected that for any two-isotope mixing array dozens of isotopic barcodes could be encoded into a material system and subsequently resolved utilizing modern mass spectrometric methods.

• Research Organization: Savannah River National Laboratory (SRNL), Aiken, SC (United States)
• Sponsoring Organization: USDOE National Nuclear Security Administration (NNSA), Office of Defense Nuclear Nonproliferation; USDOE Office of Environmental Management (EM)
• Grant/Contract Number: 89303321CEM000080; AC52-07NA27344
• OSTI ID: 2520061
• Report Number(s): SRNL--STI-2024-00372
• Journal Information: Talanta, Journal Name: Talanta Vol. 285; ISSN 0039-9140
• Publisher: Elsevier
• Country of Publication: United States
• Language: English

Related Subjects

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL PROTECTION
Mass spectrometry
Molybdenum isotopes
Nickel isotopes
Nuclear forensics
Taggants
Tungsten isotopes