Improved precision and accuracy in quantifying plutonium isotope ratios by RIMS
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Resonance ionization mass spectrometry (RIMS) holds the promise of rapid, isobar-free quantification of actinide isotope ratios in as-received materials (i.e. not chemically purified). Recent progress in achieving this potential using two Pu test materials is presented. RIMS measurements were conducted multiple times over a period of two months on two different Pu solutions deposited on metal surfaces. Measurements were bracketed with a Pu isotopic standard, and yielded absolute accuracies of the measured 240Pu/239Pu ratios of 0.7 and 0.58 %, with precisions (95 % confidence intervals) of 1.49 and 0.91 %. The minor isotope 238Pu was also quantified despite the presence of a significant quantity of 238U in the samples.
KeywordsResonance ionization mass spectrometry Nuclear forensics Plutonium Isotope ratios Laser post-ionization
The authors dedicate this work to the memory and inspiration of our mentor Dr. Ian D. Hutcheon, without whom this work would not have been possible. The authors would also like to thank Dr. Roger Henderson, Dr. Ross Williams, Dr. Amy Gaffney for their help in sample preparation and sample characterization. This work was funded by the U.S. Department of Homeland Security National Technical Nuclear Forensics Center and Laboratory Directed Research and Development Program at LLNL under project 14-ER-082. This work performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344. The CHARISMA instrument at Argonne is supported by the U.S. Department of Energy, Basic Energy Sciences, Division of Material Sciences and Engineering under Award No. DE-AC02-06CH11357. LLNL-JRNL-674877.
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