High Useful Yield and Isotopic Analysis of Uranium by Resonance Ionization Mass Spectrometry

Savina, Michael R.; Isselhardt, Brett H.; Kucher, Andrew; Trappitsch, Reto; King, Bruce V.; Ruddle, David; Gopal, Raja; Hutcheon, Ian

doi:10.1021/acs.analchem.7b01204

Title: High Useful Yield and Isotopic Analysis of Uranium by Resonance Ionization Mass Spectrometry

Journal Article · Tue May 09 00:00:00 EDT 2017 · Analytical Chemistry

DOI:https://doi.org/10.1021/acs.analchem.7b01204· OSTI ID:1368017

^[1]; Isselhardt, Brett H. ^[1]; Kucher, Andrew ^[1]; Trappitsch, Reto ^[1]; King, Bruce V. ^[2]; Ruddle, David ^[3]; Gopal, Raja ^[4]; Hutcheon, Ian ^[1]

Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Nuclear and Chemical Sciences Division
Univ. of Newcastle, NSW (Australia)
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). National Security Engineering Division
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Global Security Computing Division

Useful yields from resonance ionization mass spectrometry can be extremely high compared to other mass spectrometry techniques, but uranium analysis shows strong matrix effects arising from the tendency of uranium to form strongly bound oxide molecules that do not dissociate appreciably on energetic ion bombardment. Here, we demonstrate a useful yield of 24% for metallic uranium. Modeling the laser ionization and ion transmission processes shows that the high useful yield is attributable to a high ion fraction achieved by resonance ionization. We quantify the reduction of uranium oxide surface layers by Ar⁺ and Ga⁺ sputtering. The useful yield for uranium atoms from a uranium dioxide matrix is 0.4% and rises to 2% when the surface is in sputter equilibrium with the ion beam. The lower useful yield from the oxide is almost entirely due to uranium oxide molecules reducing the neutral atom content of the sputtered flux. We also demonstrate rapid isotopic analysis of solid uranium oxide at a precision of <0.5% relative standard deviation using relatively broadband lasers to mitigate spectroscopic fractionation.

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Research Organization:: Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC52-07NA27344; HSHQDN-16-X-0023; HDTRA 135636-M

OSTI ID:: 1368017

Report Number(s):: LLNL-JRNL-727677

Journal Information:: Analytical Chemistry, Vol. 89, Issue 11; ISSN 0003-2700

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 18 works

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Atomic spectrometry update: review of advances in atomic spectrometry and related techniques Evans, E. Hywel; Pisonero, Jorge; Smith, Clare M. M. Journal of Analytical Atomic Spectrometry, Vol. 34, Issue 5 https://doi.org/10.1039/c9ja90018g	journal	January 2019
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Title: High Useful Yield and Isotopic Analysis of Uranium by Resonance Ionization Mass Spectrometry

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