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

References (29)

Isotope selective element analysis by diode laser atomic absorption spectrometry Wizemann, H. D.; Niemax, K. Mikrochimica Acta, Vol. 129, Issue 3-4 https://doi.org/10.1007/BF01244743	journal	September 1998
Wavelength-modulation spectroscopy near 2.5 μm for H2O and temperature in high-pressure and -temperature gases Goldenstein, C. S.; Spearrin, R. M.; Jeffries, J. B. Applied Physics B, Vol. 116, Issue 3 https://doi.org/10.1007/s00340-013-5754-1	journal	January 2014
Wavelength modulation spectroscopy with signal–reference beam method for highly sensitive gas detection Wei, Wei; Chang, Jun; Huang, Qingjie Applied Physics B, Vol. 118, Issue 1 https://doi.org/10.1007/s00340-014-5956-1	journal	November 2014
Demonstration of non-absorbing interference rejection using wavelength modulation spectroscopy in high-pressure shock tubes Wei, Wei; Peng, Wen Yu; Wang, Yu Applied Physics B, Vol. 125, Issue 1 https://doi.org/10.1007/s00340-018-7118-3	journal	December 2018
Two-color frequency-multiplexed IMS technique for gas thermometry at elevated pressures Wei, Wei; Peng, Wen Yu; Wang, Yu Applied Physics B, Vol. 126, Issue 3 https://doi.org/10.1007/s00340-020-7396-4	journal	March 2020
Use of data from environmental sampling for IAEA safeguards. Case study: uranium with near-natural 235U abundance Axelsson, A.; Fischer, D. M.; Peńkin, M. V. Journal of Radioanalytical and Nuclear Chemistry, Vol. 282, Issue 3 https://doi.org/10.1007/s10967-009-0149-9	journal	July 2009
Applications of gamma-ray spectrometry in the quantitative nondestructive assay of special nuclear materials Sampson, Thomas E.; Parker, Jack L. Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 299, Issue 1-3 https://doi.org/10.1016/0168-9002(90)90801-C	journal	December 1990
Wavelength modulation absorption spectrometry — an extensive scrutiny of the generation of signals Kluczynski, Pawel; Gustafsson, Jörgen; Lindberg, Åsa M. Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 56, Issue 8 https://doi.org/10.1016/S0584-8547(01)00248-8	journal	August 2001
Characterization of 2f-, 4f-, and 6f-background signals in wavelength modulation diode laser absorption spectrometry in graphite furnaces Gustafsson, Jörgen; Chekalin, Nikolai; Axner, Ove Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 58, Issue 1 https://doi.org/10.1016/S0584-8547(02)00217-3	journal	January 2003
Diode-laser atomic-absorption spectrometry by the double-beam—double-modulation technique Liger, Vladimir; Zybin, Alexander; Kuritsyn, Yurii Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 52, Issue 8 https://doi.org/10.1016/S0584-8547(97)00029-3	journal	July 1997
The influence of hyperfine structure and isotope shift on the detection of Rb by 2f-wavelength modulation diode laser absorption spectrometry—experimental verification of simulations Gustafsson, Jörgen; Axner, Ove Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 53, Issue 14 https://doi.org/10.1016/S0584-8547(98)00200-6	journal	December 1998
Nuclear forensic science—From cradle to maturity Mayer, K.; Wallenius, M.; Fanghänel, T. Journal of Alloys and Compounds, Vol. 444-445 https://doi.org/10.1016/j.jallcom.2007.01.164	journal	October 2007
Isotopic spectroscopy of uranium atomic beams produced by thermal reduction of uranium compounds Bartlett, Joshua H.; Castro, Alonso Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 155 https://doi.org/10.1016/j.sab.2019.03.011	journal	May 2019
High sensitivity measurement of atomic emission spectra with an applied voltage modulation technique Wagatsuma, Kazuaki.; Hirokawa, Kichinosuke. Analytical Chemistry, Vol. 56, Issue 14 https://doi.org/10.1021/ac00278a024	journal	December 1984
Use of Secondary Ion Mass Spectrometry in Nuclear Forensic Analysis for the Characterization of Plutonium and Highly Enriched Uranium Particles Betti, Maria; Tamborini, Gabriele; Koch, Lothar Analytical Chemistry, Vol. 71, Issue 14 https://doi.org/10.1021/ac981184r	journal	July 1999
Determination of Uranium Isotopes in Soil Core Samples Collected on the JCO Grounds after the Criticality Accident Yoshida, Satoshi; Muramatsu, Yasuyuki; Tagami, Keiko Environmental Science & Technology, Vol. 35, Issue 21 https://doi.org/10.1021/es0106265	journal	September 2001
Mass spectrometric analysis for nuclear safeguards Boulyga, Sergei; Konegger-Kappel, Stefanie; Richter, Stephan Journal of Analytical Atomic Spectrometry, Vol. 30, Issue 7 https://doi.org/10.1039/C4JA00491D	journal	January 2015
Isotope-resolved atomic beam laser spectroscopy of natural uranium Lebedev, Vyacheslav; Bartlett, Joshua H.; Castro, Alonso Journal of Analytical Atomic Spectrometry, Vol. 33, Issue 11 https://doi.org/10.1039/C8JA00242H	journal	January 2018
Application of saturation absorption spectroscopy to study the hyperfine structure of ²³⁵U and accurate ²³⁵U/²³⁸U isotope ratio determinations at 861.031 nm Wei, Wei; Savukov, Igor; Castro, Alonso Journal of Analytical Atomic Spectrometry, Vol. 36, Issue 9 https://doi.org/10.1039/D1JA00140J	journal	January 2021
Improvement in detection limits in graphite furnace diode laser atomic absorption spectrometry by wavelength modulation technique. Plenary lecture Schnürer-Patschan, Christoph; Zybin, Aleksandr; Groll, Henning J. Anal. At. Spectrom., Vol. 8, Issue 8 https://doi.org/10.1039/JA9930801103	journal	January 1993
Determination of isotope ratios using Laser-Induced Breakdown Spectroscopy in ambient air at atmospheric pressure for nuclear forensics Doucet, François R.; Lithgow, Gregg; Kosierb, Rick Journal of Analytical Atomic Spectrometry, Vol. 26, Issue 3 https://doi.org/10.1039/c0ja00199f	journal	January 2011
Handbook of Basic Atomic Spectroscopic Data Sansonetti, J. E.; Martin, W. C. Journal of Physical and Chemical Reference Data, Vol. 34, Issue 4 https://doi.org/10.1063/1.1800011	journal	December 2005
Note: Micro-channel array crucible for isotope-resolved laser spectroscopy of high-temperature atomic beams Lebedev, Vyacheslav; Bartlett, Joshua H.; Malyzhenkov, Alexander Review of Scientific Instruments, Vol. 88, Issue 12 https://doi.org/10.1063/1.5006457	journal	December 2017
High-resolution laser spectroscopy for the study of nuclear sizes and shapes Billowes, J.; Campbell, P. Journal of Physics G: Nuclear and Particle Physics, Vol. 21, Issue 6 https://doi.org/10.1088/0954-3899/21/6/003	journal	June 1995
Absorption sensor for CO in combustion gases using 2.3 µm tunable diode lasers Chao, X.; Jeffries, J. B.; Hanson, R. K. Measurement Science and Technology, Vol. 20, Issue 11 https://doi.org/10.1088/0957-0233/20/11/115201	journal	September 2009
Analysis of calibration-free wavelength-scanned wavelength modulation spectroscopy for practical gas sensing using tunable diode lasers Sun, K.; Chao, X.; Sur, R. Measurement Science and Technology, Vol. 24, Issue 12 https://doi.org/10.1088/0957-0233/24/12/125203	journal	October 2013
Stable isotope analysis using tunable diode laser spectroscopy Becker, Joseph F.; Sauke, Todd B.; Loewenstein, Max Applied Optics, Vol. 31, Issue 12 https://doi.org/10.1364/AO.31.001921	journal	January 1992
Extension of wavelength-modulation spectroscopy to large modulation depth for diode laser absorption measurements in high-pressure gases Li, Hejie; Rieker, Gregory B.; Liu, Xiang Applied Optics, Vol. 45, Issue 5 https://doi.org/10.1364/AO.45.001052	journal	January 2006
Fitting of calibration-free scanned-wavelength-modulation spectroscopy spectra for determination of gas properties and absorption lineshapes Goldenstein, Christopher S.; Strand, Christopher L.; Schultz, Ian A. Applied Optics, Vol. 53, Issue 3 https://doi.org/10.1364/AO.53.000356	journal	January 2014

Similar Records

Application of saturation absorption spectroscopy to study the hyperfine structure of 235U and accurate 235U/238U isotope ratio determinations at 861.031 nm

Journal Article · Mon Jul 19 20:00:00 EDT 2021 · Journal of Analytical Atomic Spectrometry · OSTI ID:1812675

Term analysis of the spectrum of neutral neptunium (Np I)

Journal Article · Fri Dec 31 23:00:00 EST 1976 · J. Opt. Soc. Am.; (United States) · OSTI ID:7316827

SECOND SYSTEM OF THE ARC SPECTRUM OF PLUTONIUM. NEW EVEN LEVELS OF THE I AND II SPECTRA AND THE IONIZATION POTENTIAL OF PuI.

Journal Article · Mon Oct 14 00:00:00 EDT 1963 · Compt. Rend. · OSTI ID:4130620

Related Subjects

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY
Isotopic analysis
Wavelength modulation spectroscopy

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

Citation Formats

References (29)

Similar Records

Related Subjects