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

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.
Authors:
ORCiD logo [1] ;  [1] ;  [1] ;  [1] ;  [2] ;  [3] ;  [4] ;  [1]
  1. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Nuclear and Chemical Sciences Division
  2. Univ. of Newcastle, NSW (Australia)
  3. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). National Security Engineering Division
  4. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Global Security Computing Division
Publication Date:
Report Number(s):
LLNL-JRNL-727677
Journal ID: ISSN 0003-2700
Grant/Contract Number:
AC52-07NA27344; HSHQDN-16-X-0023; HDTRA 135636-M
Type:
Accepted Manuscript
Journal Name:
Analytical Chemistry
Additional Journal Information:
Journal Volume: 89; Journal Issue: 11; Journal ID: ISSN 0003-2700
Publisher:
American Chemical Society (ACS)
Research Org:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org:
USDOE National Nuclear Security Administration (NNSA)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; 11 NUCLEAR FUEL CYCLE AND RUEL MATERIALS; 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY
OSTI Identifier:
1368017

Savina, Michael R., Isselhardt, Brett H., Kucher, Andrew, Trappitsch, Reto, King, Bruce V., Ruddle, David, Gopal, Raja, and Hutcheon, Ian. High Useful Yield and Isotopic Analysis of Uranium by Resonance Ionization Mass Spectrometry. United States: N. p., Web. doi:10.1021/acs.analchem.7b01204.
Savina, Michael R., Isselhardt, Brett H., Kucher, Andrew, Trappitsch, Reto, King, Bruce V., Ruddle, David, Gopal, Raja, & Hutcheon, Ian. High Useful Yield and Isotopic Analysis of Uranium by Resonance Ionization Mass Spectrometry. United States. doi:10.1021/acs.analchem.7b01204.
Savina, Michael R., Isselhardt, Brett H., Kucher, Andrew, Trappitsch, Reto, King, Bruce V., Ruddle, David, Gopal, Raja, and Hutcheon, Ian. 2017. "High Useful Yield and Isotopic Analysis of Uranium by Resonance Ionization Mass Spectrometry". United States. doi:10.1021/acs.analchem.7b01204. https://www.osti.gov/servlets/purl/1368017.
@article{osti_1368017,
title = {High Useful Yield and Isotopic Analysis of Uranium by Resonance Ionization Mass Spectrometry},
author = {Savina, Michael R. and Isselhardt, Brett H. and Kucher, Andrew and Trappitsch, Reto and King, Bruce V. and Ruddle, David and Gopal, Raja and Hutcheon, Ian},
abstractNote = {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.},
doi = {10.1021/acs.analchem.7b01204},
journal = {Analytical Chemistry},
number = 11,
volume = 89,
place = {United States},
year = {2017},
month = {5}
}