More than Five Percent Ionization Efficiency by Cavity Source Thermal Ionization Mass Spectrometry for Uranium Subnanogram Amounts

Numerous applications require the precise analysis of U isotope relative enrichment in sample amounts in the sub-nanogram to picogram range, among those are nuclear forensics, nuclear safeguards, environmental survey and geosciences. However, conven-tional thermal ionization mass spectrometry (TIMS) yields U combined ionization and transmission efficiencies (i.e ratio of ions detected to sample atoms loaded) less than 0.1 or 2% depending on the loading protocol, motivating the development of sources capable of enhancing ionization. The new prototype cavity source TIMS at ETH offers improvements from 4 to 15 times in com-bined ionization and transmission efficiency compared to conventional TIMS, yielding up to 5.6 % combined efficiency. Uranium isotope ratios have been determined on reference standards in the 100 pg range bound to ion-exchange or extraction resin beads. For natural U standards, n(235U)/n(238U) ratios are measured to relative external precisions of 0.5 to 1.0 % (2RSD, 2<n<11, conven-tional source) or 2.0 % (2RSD, n=6, cavity source) and accuracies of 0.2 to 0.7 % (conventional source) or 0.4-0.9 % (cavity source). Meanwhile, n(234U)/n(238U) ratios are determined to relative external precisions of 1.7 to 3.6 % (2RSD, 2<n<11, conven-tional source) or 5.6 % (2RSD, n=6, cavity source) and accuracies of 0.1 to 2.5% (conventional source) or 0.5 to 8.3% (cavity source), which would benefit further from in-run organic interference and peak tailing corrections.

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Trinquier Anne, Maden Colin, Faure Anne-Laure, Hubert Amélie, Pointurier Fabien, Bourdon Bernard, Schönbächler Maria (2019). More than Five Percent Ionization Efficiency by Cavity Source Thermal Ionization Mass Spectrometry for Uranium Subnanogram Amounts. Analytical Chemistry. 91 (9). 6190-6199. https://doi.org/10.1021/acs.analchem.9b00849, https://archimer.ifremer.fr/doc/00489/60037/

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