PNNL

Abstract

Nuclear power is enjoying rapid growth as government energy policies and public demand shift toward low carbon energy production. Pivotal to the global nuclear power renaissance is the development and deployment of robust safeguards instrumentation that allows the limited resources of the IAEA to keep pace with the expansion of the nuclear fuel cycle. Undeclared production of highly enriched uranium (HEU) remains a primary proliferation concern for modern gaseous centrifuge enrichment plants (GCEPs), due to their massive separative work unit (SWU) processing power and comparably short cascade equilibrium timescale. The Pacific Northwest National Laboratory is developing an unattended safeguards instrument, combining continuous aerosol particulate collection with uranium isotope assay, to provide timely detection of HEU production within a GCEP. This approach is based on laser vaporization of aerosol particulates, followed by laser spectroscopy to characterize the uranium enrichment level. Our prior investigation demonstrated single-shot detection sensitivity approaching the femtogram range and relative isotope ratio uncertainty better than 10% using gadolinium as a surrogate for uranium. In this paper we present measurement results on standard samples containing traces of depleted, natural, and low enriched uranium, as well as measurements on aerodynamic size uranium particles mixed in background materials (e.g., dust, minerals, soils). Improvements and optimizations in the detection electronics, signal timing, calibration, and laser alignment have lead to significant improvements in detection sensitivity and enrichment accuracy, contributing to an overall reduction in the false alarm probability. The sample substrate media was also found to play a significant role in facilitating laser-induced vaporization and the production of energetic plasma conditions, resulting in ablation optimization and further improvements in the isotope abundance sensitivity.