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New Resonance Ionization Mass Spectrometry Scheme for Improved Uranium Analysis

  • Michael R. Savina*
    Michael R. Savina
    Nuclear and Chemical Sciences Division, Lawrence Livermore National Laboratory, 7000 East Avenue, Livermore, California 94550-5507, United States
  • Reto Trappitsch
    Reto Trappitsch
    Nuclear and Chemical Sciences Division, Lawrence Livermore National Laboratory, 7000 East Avenue, Livermore, California 94550-5507, United States
  • Andrew Kucher
    Andrew Kucher
    Nuclear and Chemical Sciences Division, Lawrence Livermore National Laboratory, 7000 East Avenue, Livermore, California 94550-5507, United States
  • , and 
  • Brett H. Isselhardt
    Brett H. Isselhardt
    Nuclear and Chemical Sciences Division, Lawrence Livermore National Laboratory, 7000 East Avenue, Livermore, California 94550-5507, United States
Cite this: Anal. Chem. 2018, 90, 17, 10551–10558
Publication Date (Web):July 21, 2018
https://doi.org/10.1021/acs.analchem.8b02656
Copyright © 2018 American Chemical Society

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    Abstract

    Abstract Image

    Resonance ionization mass spectrometry (RIMS) combines tunable laser spectroscopy with mass spectrometry to provide 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.

    Cited By

    This article is cited by 11 publications.

    1. Michael R. Savina, Brett H. Isselhardt, Reto Trappitsch. Simultaneous Isotopic Analysis of U, Pu, and Am in Spent Nuclear Fuel by Resonance Ionization Mass Spectrometry. Analytical Chemistry 2021, 93 (27) , 9505-9512. https://doi.org/10.1021/acs.analchem.1c01360
    2. Michael R. Savina, Brett H. Isselhardt, Danielle Z. Shulaker, Martin Robel, Andrew J. Conant, Brian J. Ade. Simultaneous isotopic analysis of fission product Sr, Mo, and Ru in spent nuclear fuel particles by resonance ionization mass spectrometry. Scientific Reports 2023, 13 (1) https://doi.org/10.1038/s41598-023-32203-5
    3. Michael R. Savina, Danielle Ziva Shulaker, Brett H. Isselhardt, Gregory A. Brennecka. Rapid isotopic analysis of uranium, plutonium, and americium in post-detonation debris simulants by RIMS. Journal of Analytical Atomic Spectrometry 2023, 38 (6) , 1205-1212. https://doi.org/10.1039/D3JA00096F
    4. R. Trappitsch, D. Z. Shulaker, W.-J. Ong, M. R. Savina, B. H. Isselhardt. Resonance ionization of zirconium. Journal of Radioanalytical and Nuclear Chemistry 2022, 331 (12) , 5199-5204. https://doi.org/10.1007/s10967-022-08581-x
    5. Akira Kuwahara, Kenta Murakami, Hideki Tomita, Kayo Sawada, Youichi Enokida. Doppler splitting and expansion dynamics of laser-produced plasma plume under a high vacuum ambience. Journal of Analytical Atomic Spectrometry 2022, 37 (10) , 2033-2041. https://doi.org/10.1039/D2JA00177B
    6. Manuel Raiwa, Sebastian Büchner, Nina Kneip, Martin Weiß, Paul Hanemann, Polina Fraatz, Maximilian Heller, Hauke Bosco, Felix Weber, Klaus Wendt, Clemens Walther. Actinide imaging in environmental hot particles from Chernobyl by rapid spatially resolved resonant laser secondary neutral mass spectrometry. Spectrochimica Acta Part B: Atomic Spectroscopy 2022, 190 , 106377. https://doi.org/10.1016/j.sab.2022.106377
    7. Alfredo Galindo-Uribarri, Yuan Liu, Elisa Romero Romero, Daniel W. Stracener. High efficiency laser resonance ionization of plutonium. Scientific Reports 2021, 11 (1) https://doi.org/10.1038/s41598-021-01886-z
    8. M Miyabe, Y Sato, I Wakaida, R Terabayashi, V Sonnenschein, H Tomita, Y Zhao, T Sakamoto. Odd-parity autoionizing levels of uranium observed by two-color two-step photoionization optogalvanic spectroscopy. Journal of Physics B: Atomic, Molecular and Optical Physics 2021, 54 (14) , 145003. https://doi.org/10.1088/1361-6455/abf89f
    9. Michael Savina, Reto Trappitsch. Resonance Ionization Mass Spectrometry ( RIMS ): Fundamentals and Applications Including Secondary Neutral Mass Spectrometry. 2021, 215-244. https://doi.org/10.1002/9783527682201.ch6
    10. E. J. Kautz, P. J. Skrodzki, M. Burger, B. E. Bernacki, I. Jovanovic, M. C. Phillips, S. S. Harilal. Time-resolved imaging of atoms and molecules in laser-produced uranium plasmas. Journal of Analytical Atomic Spectrometry 2019, 34 (11) , 2236-2243. https://doi.org/10.1039/C9JA00228F
    11. Reto Trappitsch, Michael R. Savina, Brett H. Isselhardt. Resonance ionization of titanium: high useful yield and new autoionizing states. Journal of Analytical Atomic Spectrometry 2018, 33 (11) , 1962-1969. https://doi.org/10.1039/C8JA00269J

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