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Safeguards Technology Program FY2026 Mid-Year Report for Project WBS# 24.1.3.3: Development of Procedures for Th-U Radiochronometry of Uranium Particles by LG-SIMS

Implementing 230 Th- 234 U radiochronometry of environmental uranium particles by large geometry secondary ion mass spectrometry (LG-SIMS) requires assessment, validation, and technical support before safeguards conclusions can be drawn from the information. This project investigates the most challenging aspects of LG-SIMS particle radiochronometry 230 Th- 234 U measurements through a collaboration between LANL and NIST, to provide best practices and procedures for determining high quality ages with optimized uncertainties. This includes exploration of reducing detector backgrounds, investigating the best ways to report uncertainties, and establishing recommended instrument setups.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Report to NCSP on 2008 DANCE measurements of 233 U($\eta$,$\gamma$)

Uranium-233 plays an important role in the Th-U fuel cycle, with substantial production in the cycle. This cycle has been proposed as an alternative to the U-Pu fuel cycle due to its reduced production of transuranic elements. An accurate measurement of the 233 U($\eta$,$\gamma$) cross section is required by the National Criticality Safety Program (NCSP) to complete the neutron-induced cross section data, where experimental capture cross section data are scarce and were measured decades ago. The most recent capture cross section data available in the literature were measured in 2007 at the n_TOF facility (CERN); in the 60s measurements were performed at Rensselaer Polytechnic Institute (RPI) and at LANL. Finally, as reported by ORNL, a new evaluation with a revised (renormalized) fission cross section is needed on 233 U. The challenge for this measurement lies in the difficulty of measuring the capture cross section data in the competing fission background, as the fission cross section is around one order of magnitude larger than the capture cross section for 233 U. The accuracy of a capture cross section measurement depends on discrimination between $\gamma$’s produced in capture and fission reactions, for which an experimental setup combining capture and fission detectors is needed. For the ($\eta$,$\gamma$) cross section measurement at LANSCE, this discrimination is achieved by combining the Detector for Advanced Neutron Capture Experiments (DANCE), to measure $\gamma$’s from capture reactions, with a Parallel Plate Avalanche Counter (PPAC) to tag the $\gamma$’s produced by fission. This method was successfully used to measure 235 U and 239 Pu capture cross sections. In these measurements, the neutron capture cross section was determined in a large fission background well above 100 keV. As part of the NCSP nuclear data effort, we have looked at past DANCE measurements on 233 U($\eta$,$\gamma$) and evaluated whether existing data is adequate to apply this technique.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DANCE and NEUANCE measurements of 233 U(n, γ) (Q4 Report to NCSP on FY2022)

Uranium-233 plays an important role in the Th-U fuel cycle, which has been proposed as an alternative to the U-Pu fuel cycle due to its reduced amount of transuranium elements. The available experimental 233 U(n,γ) cross section data in the literature are scarce [1, 2, 3], from which the capture to fission ratio is shown in figure 1. In 2008, the 233 U(n,γ) cross section was investigated at LANL using the DANCE detector combined with a PPAC, however the statistics in the keV regime were inadequate for a reliable extraction of the cross section at 100 keV. Large discrepancies are found between the evaluations, especially in the Unresolved Resonance Region (URR), see figure 1. An accurate measurement of the 233 U(n,γ) cross section is required by the NCSP to complete the neutron-induced cross section data; a new evaluation reported the need of 233 U capture data.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Materials Data on Th3U by Materials Project

UTh3 is Uranium Silicide structured and crystallizes in the cubic Pm-3m space group. The structure is three-dimensional. U is bonded to twelve equivalent Th atoms to form UTh12 cuboctahedra that share corners with twelve equivalent UTh12 cuboctahedra, edges with twenty-four equivalent ThTh8U4 cuboctahedra, faces with six equivalent UTh12 cuboctahedra, and faces with twelve equivalent ThTh8U4 cuboctahedra. All U–Th bond lengths are 3.48 Å. Th is bonded to four equivalent U and eight equivalent Th atoms to form ThTh8U4 cuboctahedra that share corners with twelve equivalent ThTh8U4 cuboctahedra, edges with eight equivalent UTh12 cuboctahedra, edges with sixteen equivalent ThTh8U4 cuboctahedra, faces with four equivalent UTh12 cuboctahedra, and faces with fourteen equivalent ThTh8U4 cuboctahedra. All Th–Th bond lengths are 3.48 Å.

36 MATERIALS SCIENCE↗