Accurate determination of uranium isotope abundances by wavelength modulation spectroscopy in atomic beams

Wei, Wei; Castro, Alonso

doi:10.1016/j.sab.2025.107202

Accurate determination of uranium isotope abundances by wavelength modulation spectroscopy in atomic beams

Journal Article · Tue Apr 01 00:00:00 EDT 2025 · Spectrochimica Acta. Part B, Atomic Spectroscopy

DOI:https://doi.org/10.1016/j.sab.2025.107202· OSTI ID:2561295

Wei, Wei ^[1]; ^[1]

Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

The design and demonstration of an optical analysis system based on wavelength modulation spectroscopy in an atomic beam for uranium isotope abundance determinations is presented. This system probes the uranium 5f³6d7s² (⁵L₆) → 5f²6d²7s² (⁵K₅) transition at 861.031 nm, which is considered to be the most suitable transition for uranium isotopic analysis. A new laser characterization strategy was developed for the conditions where optimum laser wavelength modulation depth was small compared to the free spectral range (FSR) of etalons. Two capabilities enabled the higher-precision determination of isotope abundances of atomic beams: (1) reduction of low-frequency additive noise, especially the noise caused by black-body radiation and (2) suppression of non-absorption transmission losses. The performance of this system was validated with uranium samples of various isotopic compositions. Further, by comparing the measurements using natural uranium samples between the direct absorption and the wavelength modulation approaches, a 21-fold decrease in uncertainty of the integrated absorbance and a 6.8-fold improvement in the 1-σ precision of the number density were achieved. In addition, by comparing the results using uranium oxide samples, a 6.1-fold decrease in the uncertainty of inferred isotope abundance was obtained. These results demonstrate that the 1f-normalized 2f wavelength modulation spectroscopy (WMS-2f/1f) technique enables higher-precision analysis of atomic beams.

View Accepted Manuscript (DOE)

Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA), Office of Defense Nuclear Nonproliferation

Grant/Contract Number:: 89233218CNA000001

OSTI ID:: 2561295

Alternate ID(s):: OSTI ID: 2549456

Report Number(s):: LA-UR--24-33228

Journal Information:: Spectrochimica Acta. Part B, Atomic Spectroscopy, Journal Name: Spectrochimica Acta. Part B, Atomic Spectroscopy Vol. 229; ISSN 0584-8547

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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