4.8 Article

In View of On-Site Nuclear Forensics and Assay of Fissile Materials in Sealed Packages by High-Resolution γ-Ray Spectrometry

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ANALYTICAL CHEMISTRY
卷 95, 期 6, 页码 3247-3254

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AMER CHEMICAL SOC
DOI: 10.1021/acs.analchem.2c04110

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Several incidences of nuclear smuggling have highlighted the need for a strong on-site nuclear forensic infrastructure. High-resolution gamma-ray spectrometry plays a crucial role, but existing methodologies have limitations for absolute assay of special nuclear materials in nonstandard samples. This study proposes a methodology using HRGRS that can accurately quantify fissile and other radioisotopes in sealed packages without knowledge of sample geometry and matrices. The methodology demonstrates potential for on-site nuclear forensic analysis with a short assay time, and it can be extended for wider applications beyond nuclear forensics.
Several incidences of nuclear smuggling during the past few decades have raised the demand for the development of a strong on-site nuclear forensic infrastructure. High-resolution gamma- ray spectrometry (HRGRS) plays an important role in nuclear forensics. However, the existing methodologies, developed primarily for nuclear fuel cycle applications, are relative and rely on the availability of a standard, limiting their use for the absolute assay of special nuclear materials in nonstandard geometry samples with an unknown matrix, which is vital to make a quick on-site decision on the severity, potential radiological threat, and intended use of an interdicted package. In this work, a methodology has been developed using HRGRS for quantifying fissile (235U, 239Pu) and other radioisotopes, which is applicable to sealed packages without requiring the knowledge of the sample geometry and the matrices. By combining experiments and Monte Carlo simulations, an iterative methodology has been proposed for point to extended source absolute efficiency transformation and demonstrated further for the absolute isotopic assay of uranium and plutonium standards, mock-up nuclear forensic samples, and an unknown nuclear material mixture with a nonstandard geometry, compound matrices, and a wide variation in the elemental and isotopic compositions with a view to imitate an on-site experience. The present methodology requires an assay time of only a few minutes to an hour and thus promises on-site nuclear forensic analysis of suspected flagged packages at borders and ports using high-resolution gamma-ray spectrometry. Furthermore, the present methodology is versatile and can also be adopted for wider applications, beyond nuclear forensics.

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