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Title: New Resonance Ionization Mass Spectrometry Scheme for Improved Uranium Analysis

Abstract

Resonance ionization mass spectrometry (RIMS) combines tunable laser spectroscopy with mass spectrometry to provide here a high-efficiency means of analyzing solid materials. We previously showed a very high useful yield of 24% for analysis of uranium using three lasers to excite and ionize atoms sputtered from metallic uranium and uranium dioxide. A new resonance ionization scheme using only two lasers achieves a higher useful yield of 38% by accessing both the ground electronic state and a low-lying electronic state of atomic uranium that is significantly populated by sputtering. The major loss channel in analyzing uranium dioxide is the formation of UOx molecules during sputtering. Prebombardment of the surface with 3 keV noble gas ions prior to analysis reduces the surface and results in a sputtered flux with a greatly enhanced proportion of atomic U. This method of surface reduction results in uranium useful yields as high as 6.6% for uranium dioxide analysis, compared to 2% from previous work.

Authors:
ORCiD logo [1];  [1];  [1];  [1]
  1. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Nuclear and Chemical Sciences Division
Publication Date:
Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA), Office of Defense Nuclear Nonproliferation (NA-20); LLNL Laboratory Directed Research and Development (LDRD) Program; Dept. of Homeland Security (DHS) (United States); Defense Threat Reduction Agency (DTRA) (United States)
OSTI Identifier:
1497286
Report Number(s):
LLNL-JRNL-752818
Journal ID: ISSN 0003-2700; 938294
Grant/Contract Number:  
AC52-07NA27344
Resource Type:
Accepted Manuscript
Journal Name:
Analytical Chemistry
Additional Journal Information:
Journal Volume: 90; Journal Issue: 17; Journal ID: ISSN 0003-2700
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY

Citation Formats

Savina, Michael R., Trappitsch, Reto, Kucher, Andrew, and Isselhardt, Brett H. New Resonance Ionization Mass Spectrometry Scheme for Improved Uranium Analysis. United States: N. p., 2018. Web. doi:10.1021/acs.analchem.8b02656.
Savina, Michael R., Trappitsch, Reto, Kucher, Andrew, & Isselhardt, Brett H. New Resonance Ionization Mass Spectrometry Scheme for Improved Uranium Analysis. United States. doi:10.1021/acs.analchem.8b02656.
Savina, Michael R., Trappitsch, Reto, Kucher, Andrew, and Isselhardt, Brett H. Sat . "New Resonance Ionization Mass Spectrometry Scheme for Improved Uranium Analysis". United States. doi:10.1021/acs.analchem.8b02656. https://www.osti.gov/servlets/purl/1497286.
@article{osti_1497286,
title = {New Resonance Ionization Mass Spectrometry Scheme for Improved Uranium Analysis},
author = {Savina, Michael R. and Trappitsch, Reto and Kucher, Andrew and Isselhardt, Brett H.},
abstractNote = {Resonance ionization mass spectrometry (RIMS) combines tunable laser spectroscopy with mass spectrometry to provide here a high-efficiency means of analyzing solid materials. We previously showed a very high useful yield of 24% for analysis of uranium using three lasers to excite and ionize atoms sputtered from metallic uranium and uranium dioxide. A new resonance ionization scheme using only two lasers achieves a higher useful yield of 38% by accessing both the ground electronic state and a low-lying electronic state of atomic uranium that is significantly populated by sputtering. The major loss channel in analyzing uranium dioxide is the formation of UOx molecules during sputtering. Prebombardment of the surface with 3 keV noble gas ions prior to analysis reduces the surface and results in a sputtered flux with a greatly enhanced proportion of atomic U. This method of surface reduction results in uranium useful yields as high as 6.6% for uranium dioxide analysis, compared to 2% from previous work.},
doi = {10.1021/acs.analchem.8b02656},
journal = {Analytical Chemistry},
number = 17,
volume = 90,
place = {United States},
year = {2018},
month = {7}
}

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