Analytical characterization of laser induced plasmas towards uranium isotopic analysis in gaseous uranium hexafluoride

Chan, George C.-Y.; Martin, Leigh R.; Trowbridge, Lee D.; Zhu, Zhenli; Mao, Xianglei; Russo, Richard E.

doi:10.1016/j.sab.2020.106036

Title: Analytical characterization of laser induced plasmas towards uranium isotopic analysis in gaseous uranium hexafluoride

Journal Article · Thu Feb 04 00:00:00 EST 2021 · Spectrochimica Acta. Part B, Atomic Spectroscopy

DOI:https://doi.org/10.1016/j.sab.2020.106036· OSTI ID:1775215

Chan, George C.-Y. ^[1];

^[2];

^[2]; Zhu, Zhenli ^[3]; Mao, Xianglei ^[1]; Russo, Richard E. ^[4]

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); China University of Geosciences, Wuhan (China)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Applied Spectra, West Sacramento, CA (United States)

To perform direct enrichment assay on gaseous uranium hexafluoride (UF₆) with laser induced breakdown spectroscopy (LIBS), the dominant spectral-line features, evolution of the signal and background of the U II 424.437 nm line, and its Stark width and shift, were studied as a function of UF₆ gas pressure and pulse energy of a nanosecond Nd:YAG laser. In this work, vapor pressure of UF₆ was found to be the most important parameter for LIBS analysis of gaseous UF₆. Spectral congestion with numerous U lines of high excitation potential was observed and signal-to-background ratio (SBR) was low for measurements with 80 Torr UF₆. Only when both UF₆ vapor pressure and laser pulse energy were low, for example, less than 20 Torr pressure and 30 mJ pulse energy, the resultant LIBS spectra from gaseous UF₆ resembled those obtained from solid U samples. The experimental data also suggest that U and F atoms recombine back to UF₆ after the laser pulse. The U emission was found to decay fast with a persistent background signal, degrading SBR with delay time. Systematic positive biases were found for UF₆ enrichment assays performed with the ²³⁵U–²³⁸U line pair at 424.412–424.437 nm, which was confirmed to be caused by self-absorption. Even with optimization of experimental parameters and incorporation of a self-absorption term into the spectral-fitting algorithm, to reduce and compensate for self-absorption, self-absorption is still a main factor limiting accurate UF₆ enrichment assay. The use of another spectral window which contains no resonance lines is a prospective solution for the self-absorption issue.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA), Office of Defense Nuclear Nonproliferation; China Scholarship Council (CSC)

Grant/Contract Number:: AC05-00OR22725; AC02-05CH11231

OSTI ID:: 1775215

Alternate ID(s):: OSTI ID: 1841165; OSTI ID: 2325385

Journal Information:: Spectrochimica Acta. Part B, Atomic Spectroscopy, Vol. 176; ISSN 0584-8547

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (42)

The Absorption Spectrum of UF ₆ , from 2000 to 4200 Å Depoorter, G. L.; Rofer-depoorter, C. K. Spectroscopy Letters, Vol. 8, Issue 8 https://doi.org/10.1080/00387017508067354	journal	January 1975
Detection of BO2 isotopes using laser-induced breakdown spectroscopy Amiri, Seyyed Hossein; Darbani, Seyyed Mohammad Reza; Saghafifar, Hossein Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 150 https://doi.org/10.1016/j.sab.2018.10.012	journal	December 2018
Spectroscopy and Structure of the Simplest Actinide Bonds Heaven, Michael C.; Barker, Beau J.; Antonov, Ivan O. The Journal of Physical Chemistry A, Vol. 118, Issue 46 https://doi.org/10.1021/jp507283n	journal	October 2014
Study of UF ₆ photodissociation through light scattering of UF ₅ particles Borsella, E.; Catoni, F.; Freddi, G. The Journal of Chemical Physics, Vol. 73, Issue 1 https://doi.org/10.1063/1.439877	journal	July 1980
Detection of Uranium Using Laser-Induced Breakdown Spectroscopy Chinni, Rosemarie C.; Cremers, David A.; Radziemski, Leon J. Applied Spectroscopy, Vol. 63, Issue 11 https://doi.org/10.1366/000370209789806867	journal	November 2009
Portable Spectroscopy Crocombe, Richard A. Applied Spectroscopy, Vol. 72, Issue 12 https://doi.org/10.1177/0003702818809719	journal	September 2018
On the usefulness of a duplicating mirror to evaluate self-absorption effects in laser induced breakdown spectroscopy Moon, Heh-Young; Herrera, Kathleen K.; Omenetto, Nicoló Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 64, Issue 7 https://doi.org/10.1016/j.sab.2009.06.011	journal	July 2009
Laser-induced breakdown self-reversal isotopic spectrometry for isotopic analysis of lithium Touchet, Kévin; Chartier, Frédéric; Hermann, Jörg Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 168 https://doi.org/10.1016/j.sab.2020.105868	journal	June 2020
Study of low-temperature uranium plasmas not within local thermodynamical equilibrium Fontaine, A. Compant La Journal of Physics B: Atomic and Molecular Physics, Vol. 20, Issue 24 https://doi.org/10.1088/0022-3700/20/24/016	journal	December 1987
Isotopic analysis of uranium by laser induced breakdown spectroscopy Rinaldi, Carlos; Pozzi, Marcelo; Boggio, Norberto Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 167 https://doi.org/10.1016/j.sab.2020.105841	journal	May 2020
Mass-independent analysis of the stable isotopologues of gas-phase titanium monoxide – TiO Breier, Alexander A.; Waßmuth, Björn; Fuchs, Guido W. Journal of Molecular Spectroscopy, Vol. 355 https://doi.org/10.1016/j.jms.2018.11.006	journal	January 2019
Mechanisms and efficient elimination approaches of self-absorption in LIBS Hou, Jiajia; Zhang, Lei; Zhao, Yang Plasma Science and Technology, Vol. 21, Issue 3 https://doi.org/10.1088/2058-6272/aaf875	journal	January 2019
Laser photolysis of UF ₆ molecules Baranov, V. Yu; Kolesnikov, Yu A.; Kotov, A. A. Quantum Electronics, Vol. 29, Issue 8 https://doi.org/10.1070/QE1999v029n08ABEH001549	journal	August 1999
Mapping of Uranium in Surrogate Nuclear Debris Using Laser-Induced Breakdown Spectroscopy (LIBS) Shattan, Michael B.; Gragston, Mark; Zhang, Zhili Applied Spectroscopy, Vol. 73, Issue 6 https://doi.org/10.1177/0003702819842871	journal	March 2019
Moving your laboratories to the field – Advantages and limitations of the use of field portable instruments in environmental sample analysis Gałuszka, Agnieszka; Migaszewski, Zdzisław M.; Namieśnik, Jacek Environmental Research, Vol. 140 https://doi.org/10.1016/j.envres.2015.05.017	journal	July 2015
Matrix IR spectra of the products from fluorine molecule, chlorine molecule, and chlorine fluoride (ClF) reactions with pulsed-laser evaporated uranium atoms Hunt, R. D.; Thompson, C.; Hassanzadeh, P. Inorganic Chemistry, Vol. 33, Issue 2 https://doi.org/10.1021/ic00080a031	journal	January 1994
A procedure for correcting self-absorption in calibration free-laser induced breakdown spectroscopy Bulajic, D.; Corsi, M.; Cristoforetti, G. Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 57, Issue 2 https://doi.org/10.1016/S0584-8547(01)00398-6	journal	February 2002
Einstein coefficients, cross sections, f values, dipole moments, and all that Hilborn, Robert C. American Journal of Physics, Vol. 50, Issue 11 https://doi.org/10.1119/1.12937	journal	November 1982
Polyhalide photofragment spectra. II. Ultraviolet photodissociation dynamics of UF ₆ Kroger, Peter M.; Riley, Stephen J.; Kwei, George H. The Journal of Chemical Physics, Vol. 68, Issue 9 https://doi.org/10.1063/1.436283	journal	May 1978
Photolysis of uranium hexafluoride and some reaction variables affecting the apparent quantum yield Lewis, W. B.; Wampler, F. B.; Huber, E. J. Journal of Photochemistry, Vol. 11, Issue 5 https://doi.org/10.1016/0047-2670(79)85028-5	journal	January 1979
Measurement and analysis of the pure rotational spectra of tin monochloride, SnCl, using laser ablation equipped chirped pulse and cavity Fourier transform microwave spectroscopy Grubbs, G. S.; Frohman, Daniel J.; Novick, Stewart E. Journal of Molecular Spectroscopy, Vol. 280 https://doi.org/10.1016/j.jms.2012.07.013	journal	October 2012
Role of elemental fluorine in nuclear field Groult, H.; Lantelme, F.; Salanne, M. Journal of Fluorine Chemistry, Vol. 128, Issue 4 https://doi.org/10.1016/j.jfluchem.2006.11.012	journal	April 2007
Theoretical spectroscopy study of the low-lying electronic states of UX and UX+, X = F and Cl Bross, David H.; Peterson, Kirk A. The Journal of Chemical Physics, Vol. 143, Issue 18 https://doi.org/10.1063/1.4935492	journal	November 2015
A review of the current analytical approaches for evaluating, compensating and exploiting self-absorption in Laser Induced Breakdown Spectroscopy Rezaei, Fatemeh; Cristoforetti, Gabriele; Tognoni, Elisabetta Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 169 https://doi.org/10.1016/j.sab.2020.105878	journal	July 2020
Spectroscopic diagnostics of laser-induced plasmas Konjević, N.; Ivković, M.; Jovićević, S. Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 65, Issue 8 https://doi.org/10.1016/j.sab.2010.03.009	journal	August 2010
Multivariate determination of 10B isotopic ratio by laser-induced breakdown spectroscopy using multiple BO molecular emissions Akpovo, Codjo A.; Helms, Luke; Profeta, Luisa T. M. Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 162 https://doi.org/10.1016/j.sab.2019.105710	journal	December 2019
Multivariate nonlinear spectral fitting for uranium isotopic analysis with laser-induced breakdown spectroscopy Song, Jiaojian; Chan, George C. -Y.; Mao, Xianglei Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 150 https://doi.org/10.1016/j.sab.2018.10.008	journal	December 2018
Hydrogen isotopic analysis using molecular emission from laser-induced plasma on liquid and frozen water Choi, Sung-Uk; Han, Sol-Chan; Yun, Jong-Il Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 162 https://doi.org/10.1016/j.sab.2019.105716	journal	December 2019
Laser-induced breakdown spectroscopy of uranium in the vacuum ultraviolet range Rollin, E.; Musset, O.; Cardona, D. Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 166 https://doi.org/10.1016/j.sab.2020.105796	journal	April 2020
A high-resolution laser ablation study of the transition of SrCCH Dick, M. J.; Sheridan, P. M.; Wang, J. -G. Journal of Molecular Spectroscopy, Vol. 233, Issue 2 https://doi.org/10.1016/j.jms.2005.06.016	journal	October 2005
Field instrumentation in atomic spectroscopy Hou, Xiandeng; Jones, Bradley T. Microchemical Journal, Vol. 66, Issue 1-3 https://doi.org/10.1016/S0026-265X(00)00058-8	journal	November 2000
Emission spectroscopy of expanding laser-induced gaseous hydrogen–nitrogen plasma Gautam, Ghaneshwar; Parigger, Christian G.; Helstern, Christopher M. Applied Optics, Vol. 56, Issue 33 https://doi.org/10.1364/AO.56.009277	journal	January 2017
Oscillator strengths for lines of ionized uranium (UII) Corliss, Charles H. Journal of Research of the National Bureau of Standards Section A: Physics and Chemistry, Vol. 80A, Issue 3 https://doi.org/10.6028/jres.080A.045	journal	May 1976
Measurements of Gaseous Hydrogen–Nitrogen Laser-Plasma Parigger, Christian G. Atoms, Vol. 7, Issue 3 https://doi.org/10.3390/atoms7030061	journal	June 2019
Fluorination of uranium dioxide particles: a review of physical and chemical properties of the compounds involved Sazhin, S. S.; Jeapes, A. P. Journal of Nuclear Materials, Vol. 275, Issue 3 https://doi.org/10.1016/S0022-3115(99)00131-2	journal	November 1999
The Spectrographic Determination of Uranium 235. Part IV. Using a Direct Reading, Littrow, Grating Spectrograph and a Hollow Cathode Lee, Ted; Killeen, Owen P.; MacIntyre, S. A. Applied Spectroscopy, Vol. 15, Issue 4 https://doi.org/10.1366/000370261774426984	journal	July 1961
Spectroscopic and Theoretical Investigations of UF and UF ⁺ Antonov, Ivan O.; Heaven, Michael C. The Journal of Physical Chemistry A, Vol. 117, Issue 39 https://doi.org/10.1021/jp312362e	journal	February 2013
Evaluation of self-absorption coefficients of aluminum emission lines in laser-induced breakdown spectroscopy measurements El Sherbini, A. M.; El Sherbini, Th. M.; Hegazy, H. Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 60, Issue 12 https://doi.org/10.1016/j.sab.2005.10.011	journal	December 2005
Reactions of Laser-Ablated U Atoms with HF: Infrared Spectra and Quantum Chemical Calculations of HUF, UH, and UF in Noble Gas Solids Vent-Schmidt, Thomas; Andrews, Lester; Riedel, Sebastian The Journal of Physical Chemistry A, Vol. 119, Issue 11 https://doi.org/10.1021/jp5055827	journal	August 2014
A review of the development of portable laser induced breakdown spectroscopy and its applications Rakovský, J.; Čermák, P.; Musset, O. Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 101 https://doi.org/10.1016/j.sab.2014.09.015	journal	November 2014
Optical spectroscopy of laser-produced plasmas for standoff isotopic analysis Harilal, S. S.; Brumfield, B. E.; LaHaye, N. L. Applied Physics Reviews, Vol. 5, Issue 2 https://doi.org/10.1063/1.5016053	journal	June 2018
The development of fieldable laser-induced breakdown spectrometer: No limits on the horizon Fortes, F. J.; Laserna, J. J. Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 65, Issue 12 https://doi.org/10.1016/j.sab.2010.11.009	journal	December 2010

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