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Simultaneous Pu and U Isotope Nuclear Forensics on an Environmentally Recovered Hot Particle
Swedish Museum Nat Hist, Sweden.
Swedish Museum Nat Hist, Sweden.
IAEA, Austria.
Linköping University, Department of Medical and Health Sciences, Division of Radiological Sciences. Linköping University, Faculty of Medicine and Health Sciences. Swedish Radiat Safety Author, Sweden.
2019 (English)In: Analytical Chemistry, ISSN 0003-2700, E-ISSN 1520-6882, Vol. 91, no 9, p. 5599-5604Article in journal (Refereed) Published
Abstract [en]

An environmentally recovered, mixed Pu-U hot particle from the Thule accident, Greenland has been analyzed by Scanning Electron Microscopy and a large-geometry Secondary Ion Mass Spectrometry based Scanning Ion Imaging (SII) method for simultaneous U-235,U-236,U-238 and Pu-239,Pu-240 isotope compositions. This SII technique permits the visual assessment of the spatial distribution of the isotopes of U and Pu and can be used to obtain quantitative isotope ratios in any user-defined square region up to a few 100 itm in size. The particle measured here has two resolvable U isotopic compositions with a single composition of weapons grade Pu. The bulk of the particle has,, enriched U and weapons-grade Pu with U-235/U-238, U-236/U-238 and Pu-240/Pu-239 of 1.12 +/- 0.04, 0.006 +/- 0.002, 0.054 +/- 0.004, respectively (2 sigma). The Pu isotopic ratio was consistent across the Pu-239/U-238(raw) sample but decreased from 1.99 +/- 0.07 to 0.11 +/- 0.04 (2 sigma) corresponding to the area of the particle with a resolvably different U isotope composition. This portion of the particle has U-235/U-238 U-236/U-238 and Pu-240/Pu-239 ratios of 0.11 +/- 0.04, 0.001 +/- 0.002, and 0.05 +/- 0.04, respectively (2 sigma). The origin of the less enriched U could be environmental that mixed with the particle or heterogeneously enriched U from the weapons. The heterogeneity of hot particles on a micrometer scale highlights the need for spatially resolved techniques to avoid mixing during a bulk or whole particle analysis, as the mixing end members here would have been lost, and the measured ratios would have been inaccurate.

Place, publisher, year, edition, pages
AMER CHEMICAL SOC , 2019. Vol. 91, no 9, p. 5599-5604
National Category
Subatomic Physics
Identifiers
URN: urn:nbn:se:liu:diva-157527DOI: 10.1021/acs.analchern.8b04809ISI: 000467642100022OAI: oai:DiVA.org:liu-157527DiVA, id: diva2:1328783
Note

Funding Agencies|Swedish Radiation Safety Authority grant [SSM2017-1378-1]; Swedish Research Council [2017-00617]

Available from: 2019-06-23 Created: 2019-06-23 Last updated: 2019-06-23

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