Rapid isotopic analysis of uranium, plutonium, and americium in post-detonation debris simulants by RIMS

Savina, Michael R.; Shulaker, Danielle Ziva; Isselhardt, Brett H.; Brennecka, Gregory A.

doi:10.1039/D3JA00096F

Title: Rapid isotopic analysis of uranium, plutonium, and americium in post-detonation debris simulants by RIMS

Journal Article · Wed Jun 07 00:00:00 EDT 2023 · Journal of Analytical Atomic Spectrometry

DOI:https://doi.org/10.1039/D3JA00096F· OSTI ID:1972496

^[1];

^[1]

Lawrence Livermore National Laboratory, Nuclear and Chemical Sciences Division, USA

We demonstrate rapid isotopic analysis of trace U, Pu, and Am in solid basalt matrices using resonance ionization mass spectrometry (RIMS). The samples were intended to mimic post-detonation debris from a nuclear explosion, in which material from the device is intimately mixed with entrained material from the environment. Complete isotopic analysis of materials containing ppm to ppb levels of the actinides was done without separating them from the host matrix, and consumed <100 ng of sample. Measured isotopic compositions of U, Pu, and Am were accurate to ≤10% for most isotope ratios except ²³⁸Pu, which was compromised by low concentration and excesses of ²³⁸U up to 34 000: 1. A new method called “blinking” that takes advantage of the singular ability of RIMS to quantify backgrounds from all sources rapidly and accurately was developed for the analysis of ²³⁸Pu. Using the blinking method we accurately measured the ²³⁸Pu/²³⁹Pu ratio on a sample containing 1.4 × 10⁶ atoms of ²³⁸Pu at a concentration of 0.1 ppb in the host material.

View Journal Article

Cite

Export

Save

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

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

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 1972496

Alternate ID(s):: OSTI ID: 2007608

Report Number(s):: LLNL-JRNL-846363; JASPE2

Journal Information:: Journal of Analytical Atomic Spectrometry, Journal Name: Journal of Analytical Atomic Spectrometry Vol. 38 Journal Issue: 6; ISSN 0267-9477

Publisher:: Royal Society of Chemistry (RSC)Copyright Statement

Country of Publication:: United Kingdom

Language:: English

References (26)

Simultaneous uranium/plutonium separation and direct isotope ratio measurements by using CO2 as the gas in a collision/reaction cell based MC-ICPMS Gourgiotis, A.; Granet, M.; Isnard, H. Journal of Analytical Atomic Spectrometry, Vol. 25, Issue 12 https://doi.org/10.1039/c0ja00092b	journal	January 2010
CHILI – the Chicago Instrument for Laser Ionization – a new tool for isotope measurements in cosmochemistry Stephan, Thomas; Trappitsch, Reto; Davis, Andrew M. International Journal of Mass Spectrometry, Vol. 407 https://doi.org/10.1016/j.ijms.2016.06.001	journal	August 2016
Actinide imaging in environmental hot particles from Chernobyl by rapid spatially resolved resonant laser secondary neutral mass spectrometry Raiwa, Manuel; Büchner, Sebastian; Kneip, Nina Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 190 https://doi.org/10.1016/j.sab.2022.106377	journal	April 2022
Simultaneous determination of plutonium and uranium isotope ratios in individual plutonium–uranium mixed particles by thermal ionization mass spectrometry Lee, Chi-Gyu; Suzuki, Daisuke; Saito-Kokubu, Yoko International Journal of Mass Spectrometry, Vol. 314 https://doi.org/10.1016/j.ijms.2012.02.006	journal	March 2012
Natural fractionation of 238U/235U Weyer, S.; Anbar, A. D.; Gerdes, A. Geochimica et Cosmochimica Acta, Vol. 72, Issue 2 https://doi.org/10.1016/j.gca.2007.11.012	journal	January 2008
Detection of plutonium isotopes at lowest quantities using in-source resonance ionization mass spectrometry Raeder, S.; Hakimi, A.; Stöbener, N. Analytical and Bioanalytical Chemistry, Vol. 404, Issue 8 https://doi.org/10.1007/s00216-012-6238-6	journal	August 2012
In situ determination of 238Pu in the presence of uranium by triple quadrupole ICP-MS (ICP-QQQ-MS) Tiong, Ling Ying Diane; Tan, Shimin Journal of Radioanalytical and Nuclear Chemistry, Vol. 322, Issue 2 https://doi.org/10.1007/s10967-019-06695-3	journal	August 2019
Electronic excitation of uranium atoms sputtered from uranium metal and oxides Savina, Michael R.; Trappitsch, Reto; Isselhardt, Brett H. Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 149 https://doi.org/10.1016/j.sab.2018.08.003	journal	November 2018
Simultaneous Isotopic Analysis of U, Pu, and Am in Spent Nuclear Fuel by Resonance Ionization Mass Spectrometry Savina, Michael R.; Isselhardt, Brett H.; Trappitsch, Reto Analytical Chemistry, Vol. 93, Issue 27 https://doi.org/10.1021/acs.analchem.1c01360	journal	June 2021
Isotopic spectroscopy of uranium atomic beams produced by thermal reduction of uranium compounds Bartlett, Joshua H.; Castro, Alonso Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 155 https://doi.org/10.1016/j.sab.2019.03.011	journal	May 2019
Determination of plutonium isotopes (238Pu, 239Pu, 240Pu, 241Pu) in environmental samples using radiochemical separation combined with radiometric and mass spectrometric measurements Xu, Yihong; Qiao, Jixin; Hou, Xiaolin Talanta, Vol. 119 https://doi.org/10.1016/j.talanta.2013.11.061	journal	February 2014
New Resonance Ionization Mass Spectrometry Scheme for Improved Uranium Analysis Savina, Michael R.; Trappitsch, Reto; Kucher, Andrew Analytical Chemistry, Vol. 90, Issue 17 https://doi.org/10.1021/acs.analchem.8b02656	journal	July 2018
Analysis of plutonium isotope ratios including 238 Pu/ 239 Pu in individual U–Pu mixed oxide particles by means of a combination of alpha spectrometry and ICP-MS Esaka, Fumitaka; Yasuda, Kenichiro; Suzuki, Daisuke Talanta, Vol. 165 https://doi.org/10.1016/j.talanta.2016.12.041	journal	April 2017
New horizons in microparticle forensics: Actinide imaging and detection of ²³⁸ Pu and ^242m Am in hot particles Bosco, Hauke; Hamann, Linda; Kneip, Nina Science Advances, Vol. 7, Issue 44 https://doi.org/10.1126/sciadv.abj1175	journal	October 2021
Accurate determination of minor isotope ratios in individual plutonium–uranium mixed particles by thermal ionization mass spectrometry Lee, Chi-Gyu; Park, Jinkyu; Lim, Sang Ho Nuclear Engineering and Technology, Vol. 50, Issue 1 https://doi.org/10.1016/j.net.2017.10.010	journal	February 2018
Highly selective two-step laser ionization schemes for the analysis of actinide mixtures Kneip, Nina; Düllmann, Christoph E.; Gadelshin, Vadim Hyperfine Interactions, Vol. 241, Issue 1 https://doi.org/10.1007/s10751-020-01712-4	journal	March 2020
Development of a detection method for 244Pu by Resonance Ionization Mass Spectrometry Ofan, A.; Ahmad, I.; Greene, J. P. New Astronomy Reviews, Vol. 50, Issue 7-8 https://doi.org/10.1016/j.newar.2006.06.066	journal	October 2006
An Atomic Beam Source for Actinide Elements: Concept and Realization Eichler, B.; Hübener, S.; Erdmann, N. Radiochimica Acta, Vol. 79, Issue 4 https://doi.org/10.1524/ract.1997.79.4.221	journal	January 1997
Accuracy and precision of 238Pu determination at fg level by alpha spectrometry using 239Pu and 240Pu amount analyzed by ICP-MS Mácsik, Zsuzsanna; Shinonaga, Taeko Applied Radiation and Isotopes, Vol. 68, Issue 12 https://doi.org/10.1016/j.apradiso.2010.07.006	journal	December 2010
243Am certified reference material for mass spectrometry Jakopič, Rožle; Fankhauser, Adelheid; Aregbe, Yetunde Journal of Radioanalytical and Nuclear Chemistry, Vol. 327, Issue 1 https://doi.org/10.1007/s10967-020-07521-x	journal	January 2021
Uranium and Thorium Concentration and Isotopic Composition in Five Glass (BHVO-2G, BCR-2G, NKT-1G, T1-G, ATHO-G) and Two Powder (BHVO-2, BCR-2) Reference Materials Matthews, Kathryn A.; Murrell, Michael T.; Goldstein, Steven J. Geostandards and Geoanalytical Research, Vol. 35, Issue 2 https://doi.org/10.1111/j.1751-908X.2010.00080.x	journal	December 2010
A highly-enriched 244Pu reference material for nuclear safeguards and nuclear forensics measurements Essex, Richard M.; Williams, Ross W.; Treinen, Kerri C. Journal of Radioanalytical and Nuclear Chemistry, Vol. 324, Issue 1 https://doi.org/10.1007/s10967-020-07075-y	journal	March 2020
Rusty nails adsorb trace plutonium from the environment Oldham, W. J.; Matteson, B. S.; Miller, J. L. Journal of Radioanalytical and Nuclear Chemistry, Vol. 296, Issue 2 https://doi.org/10.1007/s10967-012-2066-6	journal	August 2012
High Useful Yield and Isotopic Analysis of Uranium by Resonance Ionization Mass Spectrometry Savina, Michael R.; Isselhardt, Brett H.; Kucher, Andrew Analytical Chemistry, Vol. 89, Issue 11 https://doi.org/10.1021/acs.analchem.7b01204	journal	May 2017
Resonance ionization of titanium: high useful yield and new autoionizing states Trappitsch, Reto; Savina, Michael R.; Isselhardt, Brett H. Journal of Analytical Atomic Spectrometry, Vol. 33, Issue 11 https://doi.org/10.1039/C8JA00269J	journal	January 2018
Resonance ionization mass spectrometry for ultratrace analysis of plutonium with a new solid state laser system Grüning, C.; Huber, G.; Klopp, P. International Journal of Mass Spectrometry, Vol. 235, Issue 2 https://doi.org/10.1016/j.ijms.2004.04.013	journal	July 2004

Similar Records

Isotopic analysis of uranium and plutonium mixtures by resonance ionization mass spectrometry

Journal Article · Thu Mar 01 00:00:00 EST 1984 · Anal. Chem.; (United States) · OSTI ID:1972496

Donohue, D L; Smith, D H; Young, J P; +2 more

Improved precision and accuracy in quantifying plutonium isotope ratios by RIMS

Journal Article · Tue Sep 01 00:00:00 EDT 2015 · Journal of Radioanalytical and Nuclear Chemistry · OSTI ID:1972496

Isselhardt, B. H.; Savina, M. R.; Kucher, A.; +3 more

Fission Gamma-Ray Spectra Relevant to Post-Detonation Debris Analysis

Technical Report · Thu Jan 03 00:00:00 EST 2019 · OSTI ID:1972496

Tonchev, Anton P.; Silano, Jack; Wilhelmy, Jerry; +1 more

Related Subjects

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY

Title: Rapid isotopic analysis of uranium, plutonium, and americium in post-detonation debris simulants by RIMS

Citation Formats

References (26)

Similar Records

Related Subjects