Interrogating a Mixed Actinide Basket Using High-Resolution γ-Ray Spectrometry: A Nuclear Forensic Perspective on Possible Smuggling Scenarios.

The total fissile content in seized nuclear materials is of immense importance and needs to be estimated with reasonable accuracy as a part of nuclear forensics for early decision-making in legal proceedings. High-resolution γ-ray spectrometry (HRGRS), because of its nondestructive nature, is a powerful tool for the assay of such samples to reach a quick "on-site" decision on the severity, intended use, and associated radiological threat. If the seized package contains fissile isotopes of more than one actinide in a multicompartmental heterogeneous mixture, analogous to the most likely scenario of a "smuggled mixed actinide basket", its "on-site" quantification can be extremely challenging. This makes up an increasing share of the absolute HRGRS in nuclear forensics and demands for fundamentally new approaches. In the present work, the challenges associated with varying attenuation experienced by γ-rays of different actinides at different subcontainments of the heterogeneous sample matrix have been addressed by an iterative efficiency transfer approach from "point" to "extended" source for individual actinides and demonstrated for the assay of four mock-up samples and a legacy packet, mimicking seized packages containing nuclear materials. An absolute isotopic inventory of the fissile and other radioisotopes has been obtained within <10% along with the assay of total U and Pu within <3% of the expected values with measurement uncertainty <10% for the majority. The present approach has a good potential for "on-site" nuclear forensics in nuclear smuggling scenarios and also can be adapted easily for a wide variety of other applications.