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Download Hi-Res ImageDownload to MS-PowerPointCite This:Anal. Chem. 2017, 89, 11, 6224-6231
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High Useful Yield and Isotopic Analysis of Uranium by Resonance Ionization Mass Spectrometry

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† Nuclear and Chemical Sciences Division, Lawrence Livermore National Laboratory, Livermore, California 94550, United States
‡ The University of Newcastle, Newcastle, New South Wales 2308, Australia
§ National Security Engineering Division, Lawrence Livermore National Laboratory, Livermore, California 94550, United States
∥ Global Security Computing Division, Lawrence Livermore National Laboratory, Livermore, California 94550, United States
*E-mail: [email protected]
Cite this: Anal. Chem. 2017, 89, 11, 6224–6231
Publication Date (Web):May 9, 2017
https://doi.org/10.1021/acs.analchem.7b01204
Copyright © 2017 American Chemical Society
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    Abstract

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    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. 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 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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