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

被引：34

作者：

Mathew, Kattathu ^{[1
]}

Kayzar-Boggs, Theresa ^{[2
]}

Varga, Zsolt ^{[3
]}

Gaffney, Amy ^{[5
]}

Denton, Joanna ^{[2
]}

Fulwyler, James ^{[1
,2
]}

Garduno, Katherine ^{[1
]}

Gaunt, Andrew ^{[2
]}

Inglis, Jeremy ^{[2
]}

Keller, Russ ^{[1
]}

Kinman, William ^{[2
]}

Labotka, Dana ^{[1
]}

Lujan, Elmer ^{[1
]}

Maassen, Joel ^{[2
]}

Mastren, Tara ^{[2
]}

May, Iain ^{[2
]}

Mayer, Klaus ^{[3
]}

Nichol, Adrian ^{[3
]}

Ottenfeld, Chelsea ^{[1
]}

Parsons-Davis, Tashi ^{[4
]}

Porterfield, Donivan ^{[1
]}

Rim, Jung ^{[1
]}

Rolison, John ^{[4
]}

Stanley, Floyd ^{[1
,6
]}

Steiner, Rob ^{[2
]}

Tandon, Lav ^{[1
,7
]}

Thomas, Mariam ^{[1
]}

Torres, Richard ^{[5
]}

Treinen, Kerri ^{[4
]}

Wallenius, Maria ^{[3
]}

Wende, Allison ^{[2
]}

Williams, Ross ^{[4
]}

Wimpenny, Josh ^{[4
]}

机构：

[1] Los Alamos Natl Lab, Actinide Analyt Chem, MS G740, Los Alamos, NM 87545 USA

[2] Los Alamos Natl Lab, Nucl & Radiochem, MS J514, Los Alamos, NM 87545 USA

[3] European Commiss, JRC, Directorate Nucl Safety & Secur, POB 2340, D-76125 Karlsruhe, Germany

[4] Lawrence Livermore Natl Lab, Nucl & Chem Sci Div, 7000 East Ave,L-231, Livermore, CA 94550 USA

[5] Lawrence Livermore Natl Lab, Mat Sci Div, 7000 East Ave,L-231, Livermore, CA 94550 USA

[6] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA

[7] Lawrence Livermore Natl Lab, Strateg Dev Off, Livermore, CA 94550 USA

来源：

ANALYTICAL CHEMISTRY | 2019年 / 91卷 / 18期

关键词：

NUCLEAR FORENSICS; RATIO; SAFEGUARDS; TIMS;

D O I：

10.1021/acs.analchem.9b02156

中图分类号：

O65 [分析化学];

学科分类号：

070302 ; 081704 ;

摘要：

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 U-234/(238)pu, U-235/Pu-239, U-236/Pu-240, and Am-241/Pu-241 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 U-234/(238)pu, U-235/(239)pu, (236)u/(240)pu, Am-241 /(241)pu standards that are certified for F and Pu model purification ages as well as other multigenerational radio-chronometers such as Np-237/Pu-241. 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. 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.

引用

页码：11643 / 11652

页数：10

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