Journal
ANALYTICAL CHEMISTRY
Volume 85, Issue 8, Pages 4195-4198Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ac400577p
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Funding
- DOE/NNSA [PDP11-40/DE-NA0001112]
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In the event of a rogue nuclear attack or interception of illicit nuclear materials, timely forensic investigations are critical for accurate source attribution. Uranium (U) and plutonium (Pu) isotopic ratios of intercepted materials or postdetonation samples are, perhaps, the most valuable evidence in modern nuclear forensics. These ratios simultaneously provide information regarding the material's age (i.e., time elapsed since last purification), actinide concentrations, and relevant isotopic ratios/enrichment values. Consequently, these isotope signatures are invaluable in determining the origin, processing history, and intended purpose of any nuclear material. Here we show, for the first time, that it is feasible to determine the U and Pu isotopic compositions of historic nuclear devices from their postdetonation materials utilizing in situ U isotopic measurements. The U isotopic compositions of trinitite glass, produced subsequent to the world's first atomic explosion, indicate two sources: the device's tamper, composed of natural U that underwent fission during detonation, and natural U from the geological background. Enrichments in U-234,U-235,U-236 reflect the in situ decay of Pu-238,Pu-239,Pu-240, the fuel used in the device. Time-integrated U isotopic modeling yields supergrade compositions, where Pu-240/Pu-239 approximate to 0.01-0.03 and Pu-238/Pu-239 approximate to 0.00011-0.00017, which are consistent with the Pu originating from the Hanford reactor.(1) Spatially resolved U isotopic data of postdetonation debris reveal important details of the device in a relatively short time frame (hours). This capacity serves as an important deterrent to future nuclear threats and/or terrorist activities and is critical for source attribution and international security.
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