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The use of LA-SF-ICP-MS for nuclear forensics purposes: uranium isotope ratio analysis
Authors:Rafael C Marin  Jorge E S Sarkis  Marcos R L Nascimento
Institution:1. Instituto de Pesquisas Energéticas e Nucleares (IPEN/CNEN-SP), Av. Professor Lineu Prestes 2242, S?o Paulo, SP, 05508-000, Brazil
2. Laboratório de Po?os de Caldas (LAPOC/CNEN-MG), Rodovia Po?os de Caldas/Andradas, km 13, Po?os de Caldas, MG, 37701-970, Brasil
Abstract:This work describes the utilization of the laser ablation sector field inductively coupled plasma mass spectrometry (LA-SF-ICP-MS) technique for the determination of uranium isotopic composition in a highly enriched uranium sample. The measurements were performed on a continuous ablation with low energy density and defocusing, which demonstrated to be the optimum to reach the best signal stability. The measurements were improved by adjusting the following parameters: RF power, laser beam diameter, defocusing of laser beam, laser energy, laser energy density, auxiliary gas and sample gas. The 235U/238U isotope ratio with its respective uncertainty was 16.36 ± 0.15 and its precision was 1.12 % relative standard deviation. The uncertainties were estimated following the ISO GUM, with a confidence level of 95.45 % (k = 2.00). When compared the isotope abundances to the Round Robin Exercise Number 3’s average results a difference of 0.46 % has been found and when compared to supplier’s value, the difference was 0.41 %. The results presented by the measurements revealed that the LA-ICP-MS technique offers a rapid and accurate alternative to measure uranium isotope ratios without any sample preparation, since it allows carrying out the measurements straight on the sample. Moreover, it preserves the testimony—very important for safeguards and nuclear forensics purposes.
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