Round-robin 230Th–234U age dating of bulk uranium for nuclear forensics

Gaffney, Amy M.; Hubert, Amélie; Kinman, William S.; Magara, Masaaki; Okubo, Ayako; Pointurier, Fabien; Schorzman, Kerri C.; Steiner, R. E.; Williams, Ross W.

doi:10.1007/s10967-015-4334-8

Cited by 25 publications

(19 citation statements)

References 5 publications

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“…These methods are capable of the highest-precision analyses for most uranium and plutonium radiochronometry systems. Because of their higher sensitivity relative to counting methods for most radionuclides, mass spectrometry methods can be used to analyze samples that are comparatively much smaller or younger and therefore have very low total amounts of decay products (e.g., Wallenius & Mayer 2000, Wallenius et al 2002, Eppich et al 2013, Gaffney et al 2015, Kayzar & Williams 2016, Varga et al 2015. Isotope dilution methods are used for quantification of parent and progeny isotope abundances by TIMS or ICP-MS. For ICP-MS and TIMS, the analyte must be purified from sample matrix, whereas SIMS analysis utilizes bulk sample.…”

Section: Methodsmentioning

confidence: 99%

Nuclear Forensic Science: Analysis of Nuclear Material Out of Regulatory Control

Kristo

Gaffney

Marks

et al. 2016

Annu. Rev. Earth Planet. Sci.

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Nuclear forensic science seeks to identify the origin of nuclear materials found outside regulatory control. It is increasingly recognized as an integral part of a robust nuclear security program. This review highlights areas of active, evolving research in nuclear forensics, with a focus on analytical techniques commonly employed in Earth and planetary sciences. Applications of nuclear forensics to uranium ore concentrates (UOCs) are discussed first. UOCs have become an attractive target for nuclear forensic researchers because of the richness in impurities compared to materials produced later in the fuel cycle. The development of chronometric methods for age dating nuclear materials is then discussed, with an emphasis on improvements in accuracy that have been gained from measurements of multiple radioisotopic systems. Finally, papers that report on casework are reviewed, to provide a window into current scientific practice. Ian Hutcheon, our friend, colleague, and mentor, passed away on March 26, 2015, during the writing of this review paper. Ian (PhD, Physics, University of California, Berkeley, 1974)

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Section: Methodsmentioning

confidence: 99%

Nuclear Forensic Science: Analysis of Nuclear Material Out of Regulatory Control

Kristo

Gaffney

Marks

et al. 2016

Annu. Rev. Earth Planet. Sci.

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“…The degree to which these assumptions are met in diverse materials produced during different stages in the nuclear fuel cycle is an area of active research; different materials that are both consistent and inconsistent with model age assumptions have been recognized [1][2][3][4]. Furthermore, simply because a material is discovered to have discordant model ages does not preclude gaining useful information from the radiochronometric investigation.…”

Section: Introductionmentioning

confidence: 99%

230Th-234U and 231Pa-235U radiochronometry of hydrolyzed uranium hexafluoride gas

Harrison

Gaffney

2021

J Radioanal Nucl Chem

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Radiochronometry analyses of three hydrolyzed UF 6 gas samples were performed using the 230 Th-234 U and 231 Pa-235 U chronometers. All 230 Th-234 U model ages are younger than, and two of the three 231 Pa-235 U model ages overlap with, the known UF 6 gas transfer dates. The 230 Th-234 U discordance is caused by 8-10% 230 Th loss relative to the measurement reference date, likely during alkali hydrolysis. These results confirm that UF 6 gas transfers effectively purify uranium from daughter progeny. Daughter progeny fractionation can occur if solutions are not kept within optimal conditions post-UF 6 gas transfer and hydrolysis, and discordance between the 230 Th-234 U and 231 Pa-235 U chronometers may result from the laboratory procedures used to prepare samples.

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“…Age dating of bulk uranium, in the tens-of-micrograms range, was successfully carried out in the context of a round-robin exercise. 4 Nevertheless, the principal limitation of such techniques is the impossibility to determine the individual ages of a sample which consists of a mixture of nuclear materials of different ages. The measured age would be a mean of the ages of the different populations of nuclear materials, leading to a false value that would not match the real composition of the sample.…”

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confidence: 99%

“…All of these techniques require ponderable amounts of sample. Age dating of bulk uranium, in the tens-of-micrograms range, was successfully carried out in the context of a round-robin exercise . Nevertheless, the principal limitation of such techniques is the impossibility to determine the individual ages of a sample which consists of a mixture of nuclear materials of different ages.…”

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confidence: 99%

Age Dating of Individual Micrometer-Sized Uranium Particles by Secondary Ion Mass Spectrometry: An Additional Fingerprint for Nuclear Safeguards Purposes

Fauré

Dalger

2017

Anal. Chem.

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A direct and simultaneous analysis of the age and isotopic composition of nuclear material at the particle scale is described in this study. By comparison with other conventional techniques such as inductively-coupled plasma mass spectrometry or thermal-ionization mass spectrometry, secondary ion mass spectrometry enables one to determine the ages of individual particles in a mixture of nuclear materials. Having access to the purification date can give precious information on the history of a nuclear facility or nuclear material for safeguarding purposes. The high sensitivity of this technique combined with its imaging capabilities enables one to detect and to sort out all particles according to their isotopic composition in one analysis. The succession of two microbeam analyses on an individual particle allows the determination of the precise U abundance and the model age. The methodology was successfully applied to a mixture of uranium particles coming from certified reference material with aU abundance ranging from 10% to 97%: the accuracy on the U abundance is greater than 0.5% and the accuracies on theU abundance and the model age are better than 0.5% and 3%, respectively.

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Round-robin 230Th–234U age dating of bulk uranium for nuclear forensics

Cited by 25 publications

References 5 publications

Nuclear Forensic Science: Analysis of Nuclear Material Out of Regulatory Control

Nuclear Forensic Science: Analysis of Nuclear Material Out of Regulatory Control

230Th-234U and 231Pa-235U radiochronometry of hydrolyzed uranium hexafluoride gas

Age Dating of Individual Micrometer-Sized Uranium Particles by Secondary Ion Mass Spectrometry: An Additional Fingerprint for Nuclear Safeguards Purposes

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