Intercomparison of the Radio-Chronometric Ages of Plutonium-Certified Reference Materials with Distinct Isotopic Compositions

Journal Article · Fri Aug 16 00:00:00 EDT 2019 · Analytical Chemistry

DOI:https://doi.org/10.1021/acs.analchem.9b02156· OSTI ID:1570646

Mathew, Kattathu Joseph  ^[1]; Kayzar-Boggs, Theresa Marie  ^[1]; Varga, Zsolt  ^[2]; Gaffney, Amy M. ^[3]; Denton, Joanna S.  ^[1]; Fulwyler, James Brent ^[1]; Garduno, Katherine ^[1]; Gaunt, Andrew James  ^[1]; Inglis, Jeremy David  ^[1]; Keller, Russell C. ^[1]; Kinman, William Scott  ^[1]; Labotka, Dana Miller  ^[1]; Lujan, Elmer J. W ^[1]; Maassen, Joel Ryan  ^[1]; Mastren, Tara  ^[1]; May, Iain  ^[1]; Mayer, Klaus ^[2]; Nicholl, Adrian ^[2]; Ottenfeld, Chelsea Faith ^[1]; Parsons-Davis, Tashi ^[3] ; Porterfield, Donivan R. ^[1]; Rim, Jung Ho  ^[1]; Rolison, John M. ^[3]; Stanley, Floyd E.  ^[1]; Steiner, Robert Ernest  ^[1]; Tandon, Lav  ^[1]; Thomas, Mariam R. ^[1]; Torres, Richard A. ^[3]; Treinen, Kerri C. ^[3]; Wallenius, Maria ^[2]; Wende, Allison Marie ^[1]; Williams, Ross W. ^[3]; Wimpenny, Josh B.N ^[3]

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1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
2. Joint Research Centre (JRC), Karlsruhe (Germany)
3. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

In this article, an intercomparison of the radio-chronometric ages of four distinct plutonium-certified reference materials varying in chemical form, isotopic composition, and period of production are presented. The cross-comparison of the different ²³⁴U/²³⁸Pu, ²³⁵U/²³⁹Pu, ²³⁶U/²⁴⁰Pu, and ²⁴¹Am/²⁴¹Pu model purification ages obtained at four independent analytical facilities covering a range of laboratory environments from bulk sample processing to clean facilities dedicated to nuclear forensic investigation of environmental samples enables a true assessment of the state-of-practice in “age dating capabilities” for nuclear materials. The analytical techniques evaluated used modern mass spectrometer instrumentation including thermal ionization mass spectrometers and inductively coupled plasma mass spectrometers for isotopic abundance measurements. Both multicollector and single collector instruments were utilized to generate the data presented here. Consensus values established in this study make it possible to use these isotopic standards as quality control standards for radio-chronometry applications. Results highlight the need for plutonium isotopic standards that are certified for ²³⁴U/²³⁸Pu, ²³⁵U/²³⁹Pu, ²³⁶U/²⁴⁰Pu, and ²⁴¹Am/²⁴¹Pu model purification ages as well as other multigenerational radio-chronometers such as ²³⁷Np/²⁴¹Pu. Due to the capabilities of modern analytical instrumentation, analytical laboratories that focus on trace level analyses can obtain model ages with marginally larger uncertainties than laboratories that handle bulk samples. Lastly, when isotope ratio measurement techniques like thermal ionization mass spectrometry and inductively coupled plasma mass spectrometry with comparable precision are utilized, model purification ages with similar uncertainties are obtained.

• Research Organization: Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
• Sponsoring Organization: USDOE National Nuclear Security Administration (NNSA)
• Grant/Contract Number: 89233218CNA000001; AC52-07NA27344
• OSTI ID: 1570646
• Alternate ID(s): OSTI ID: 1601561
• Report Number(s): LA-UR-19-23330; LLNL-JRNL-765551; LLNLJRNL-765551-DRAFT; TRN: US2001085
• Journal Information: Analytical Chemistry, Vol. 91, Issue 18; ISSN 0003-2700
• Publisher: American Chemical Society (ACS)
• Country of Publication: United States
• Language: English

Related Subjects

36 MATERIALS SCIENCE
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY
Purification
Organic polymers
Assays
Isotopes
Materials