Search Menu
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information
Search Scholarly Publications

Title: Spectroscopic signatures and oxidation characteristics of nanosecond laser-induced cerium plasmas

Abstract

Improving technologies related to the wide area environmental sampling of nuclear materials supports the nuclear nonproliferation mission of preventing the proliferation of nuclear weapons by monitoring nuclear weapons tests and detecting undeclared nuclear fuel cycle activities. Standoff, laser-based detection techniques such as laser-induced breakdown spectroscopy have the potential to offer robust, field-deployable methods that provide rapid element-specific and phase identifiable measurements over a wide range of materials. This work aims to elucidate the effects of atmospheric conditions and oxidation reactions on the highly complex and transient spectroscopic signatures of laser-induced plutonium surrogate plasmas. Time-resolved spectra of nanosecond laser ablation cerium plasmas were measured using laser-induced breakdown spectroscopy in a range of atmospheres containing low to high concentrations of oxygen. Here, the growth of strong CeO molecular emission bands was observed in the visible spectrum, where it was shown that the persistence of CeO is reduced from around 60 μs to 50 μs in oxygen rich atmospheric environments. To further investigate the growth and depletion of CeO in the laser-produced plasma, ratios of CeO-to-Ce emission were generated using integrated intensities corresponding to the Q-branch of the CeO D1-X1 transitions and numerous strong atomic Ce peaks. It was determined that the fastestmore » rate of formation of CeO in argon occurred for moderate oxygen mass fractions between 0.10 and 0.15 while the ratios were reduced at higher oxygen mass fractions (i.e., YO2 = 0.20) due to competing oxidation reactions and lower plasma temperatures.« less

Authors:
 [1];  [2];  [1]
+ Show Author Affiliations
  1. Univ. of Florida, Gainesville, FL (United States)
  2. Savannah River National Lab., Aiken, SC (United States)
Publication Date:
Research Org.:
Univ. of Michigan, Ann Arbor, MI (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1916462
Grant/Contract Number:  
NA0003920
Resource Type:
Accepted Manuscript
Journal Name:
Spectrochimica Acta. Part B, Atomic Spectroscopy
Additional Journal Information:
Journal Volume: 200; Journal ID: ISSN 0584-8547
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
70 PLASMA PHYSICS AND FUSION TECHNOLOGY; Cerium; Laser ablation; Laser-induced breakdown spectroscopy; Plasma chemistry; Oxidation

Citation Formats

Kwapis, Emily H., Villa-Aleman, Eliel, and Hartig, Kyle C. Spectroscopic signatures and oxidation characteristics of nanosecond laser-induced cerium plasmas. United States: N. p., 2022. Web. doi:10.1016/j.sab.2022.106610.
Copy to clipboard
Kwapis, Emily H., Villa-Aleman, Eliel, & Hartig, Kyle C. Spectroscopic signatures and oxidation characteristics of nanosecond laser-induced cerium plasmas. United States. https://doi.org/10.1016/j.sab.2022.106610
Copy to clipboard
Kwapis, Emily H., Villa-Aleman, Eliel, and Hartig, Kyle C. Wed . "Spectroscopic signatures and oxidation characteristics of nanosecond laser-induced cerium plasmas". United States. https://doi.org/10.1016/j.sab.2022.106610. https://www.osti.gov/servlets/purl/1916462.
Copy to clipboard
@article{osti_1916462,
title = {Spectroscopic signatures and oxidation characteristics of nanosecond laser-induced cerium plasmas},
author = {Kwapis, Emily H. and Villa-Aleman, Eliel and Hartig, Kyle C.},
abstractNote = {Improving technologies related to the wide area environmental sampling of nuclear materials supports the nuclear nonproliferation mission of preventing the proliferation of nuclear weapons by monitoring nuclear weapons tests and detecting undeclared nuclear fuel cycle activities. Standoff, laser-based detection techniques such as laser-induced breakdown spectroscopy have the potential to offer robust, field-deployable methods that provide rapid element-specific and phase identifiable measurements over a wide range of materials. This work aims to elucidate the effects of atmospheric conditions and oxidation reactions on the highly complex and transient spectroscopic signatures of laser-induced plutonium surrogate plasmas. Time-resolved spectra of nanosecond laser ablation cerium plasmas were measured using laser-induced breakdown spectroscopy in a range of atmospheres containing low to high concentrations of oxygen. Here, the growth of strong CeO molecular emission bands was observed in the visible spectrum, where it was shown that the persistence of CeO is reduced from around 60 μs to 50 μs in oxygen rich atmospheric environments. To further investigate the growth and depletion of CeO in the laser-produced plasma, ratios of CeO-to-Ce emission were generated using integrated intensities corresponding to the Q-branch of the CeO D1-X1 transitions and numerous strong atomic Ce peaks. It was determined that the fastest rate of formation of CeO in argon occurred for moderate oxygen mass fractions between 0.10 and 0.15 while the ratios were reduced at higher oxygen mass fractions (i.e., YO2 = 0.20) due to competing oxidation reactions and lower plasma temperatures.},
doi = {10.1016/j.sab.2022.106610},
journal = {Spectrochimica Acta. Part B, Atomic Spectroscopy},
number = ,
volume = 200,
place = {United States},
year = {Wed Dec 21 00:00:00 EST 2022},
month = {Wed Dec 21 00:00:00 EST 2022}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1016/j.sab.2022.106610
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Save / Share:
Export Metadata
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.

Works referenced in this record:

Laboratory-Scale Method for Estimating Explosive Performance from Laser-Induced Shock Waves
journal, May 2015

Physical conditions for UO formation in laser-produced uranium plumes
journal, January 2019

  • Harilal, S. S.; Kautz, E. J.; Bernacki, B. E.
  • Physical Chemistry Chemical Physics, Vol. 21, Issue 29
  • DOI: 10.1039/C9CP02250C

Analysis of Rare Earth Elements in Uranium Using Handheld Laser-Induced Breakdown Spectroscopy (HH LIBS)
journal, May 2018

  • Manard, Benjamin T.; Wylie, E. Miller; Willson, Stephen P.
  • Applied Spectroscopy, Vol. 72, Issue 11
  • DOI: 10.1177/0003702818775431

Term analysis of the spectrum of neutral plutonium, Pu i
journal, January 1986

  • Blaise, Jean; Fred, Mark; Gutmacher, Ralph G.
  • Journal of the Optical Society of America B, Vol. 3, Issue 3
  • DOI: 10.1364/JOSAB.3.000403

Laser-induced plasma chemistry of the explosive RDX with various metallic nanoparticles
journal, January 2012

Determination of Impurities in Uranium and Plutonium Dioxides by Laser-Induced Breakdown Spectroscopy
journal, September 1999

Laser-induced breakdown spectroscopy of light water reactor simulated used nuclear fuel: Main oxide phase
journal, July 2017

  • Campbell, Keri R.; Judge, Elizabeth J.; Barefield, James E.
  • Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 133
  • DOI: 10.1016/j.sab.2017.04.006

Plasma plume behavior of laser ablated cerium oxide: Effect of oxygen partial pressure
journal, June 2014

  • Panda, Arun Kumar; Singh, Akash; Mishra, Maneesha
  • Laser and Particle Beams, Vol. 32, Issue 3
  • DOI: 10.1017/S0263034614000330

Exploring laser-induced breakdown spectroscopy for nuclear materials analysis and in-situ applications
journal, August 2012

  • Martin, Madhavi Z.; Allman, Steve; Brice, Deanne J.
  • Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 74-75
  • DOI: 10.1016/j.sab.2012.06.049

Pu-239/Pu-240 isotope ratios determined using high resolution emission spectroscopy in a laser-induced plasma
journal, May 2002

  • Smith, Coleman A.; Martinez, Max A.; Veirs, D. Kirk
  • Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 57, Issue 5, p. 929-937
  • DOI: 10.1016/S0584-8547(02)00023-X

Formation of 238 U 16 O and 238 U 18 O observed by time-resolved emission spectroscopy subsequent to laser ablation
journal, July 2017

  • Weisz, David G.; Crowhurst, Jonathan C.; Siekhaus, Wigbert J.
  • Applied Physics Letters, Vol. 111, Issue 3
  • DOI: 10.1063/1.4991824

Spectroscopy of laser-produced cerium plasma for remote isotope analysis of nuclear fuel
journal, June 2010

Improved photodarkening resistivity in ytterbium-doped fiber lasers by cerium codoping
journal, April 2009

Time-resolved imaging of atoms and molecules in laser-produced uranium plasmas
journal, January 2019

  • Kautz, E. J.; Skrodzki, P. J.; Burger, M.
  • Journal of Analytical Atomic Spectrometry, Vol. 34, Issue 11
  • DOI: 10.1039/C9JA00228F

Expansion dynamics and chemistry evolution in ultrafast laser filament produced plasmas
journal, January 2020

  • Kautz, Elizabeth J.; Yeak, Jeremy; Bernacki, Bruce E.
  • Physical Chemistry Chemical Physics, Vol. 22, Issue 16
  • DOI: 10.1039/D0CP00078G

Time-resolved formation of uranium and silicon oxides subsequent to the laser ablation of U3Si2
journal, August 2020

  • Weerakkody, Emily N.; Weisz, David G.; Crowhurst, Jonathan
  • Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 170
  • DOI: 10.1016/j.sab.2020.105925

Kinetics and mechanism of the oxidation of cerium in air at ambient temperature
journal, October 2016

Characterization of laser-induced plasmas as a complement to high-explosive large-scale detonations
journal, September 2017

  • Kimblin, Clare; Trainham, Rusty; Capelle, Gene A.
  • AIP Advances, Vol. 7, Issue 9
  • DOI: 10.1063/1.4999793

Electron density and temperature measurements in a laser produced carbon plasma
journal, September 1997

  • Harilal, S. S.; Bindhu, C. V.; Issac, Riju C.
  • Journal of Applied Physics, Vol. 82, Issue 5
  • DOI: 10.1063/1.366276

Integration of bulk-quality thin film magneto-optical cerium-doped yttrium iron garnet on silicon nitride photonic substrates
journal, January 2014

  • Onbasli, Mehmet C.; Goto, Taichi; Sun, Xueyin
  • Optics Express, Vol. 22, Issue 21
  • DOI: 10.1364/OE.22.025183

Electronic Spectroscopy of UO
journal, September 1997

  • Kaledin, Leonid A.; Heaven, Michael C.
  • Journal of Molecular Spectroscopy, Vol. 185, Issue 1
  • DOI: 10.1006/jmsp.1997.7383

Quantitative absorption spectroscopy of laser-produced plasmas
journal, January 2021

  • Weerakkody, Emily N.; Glumac, Nick G.
  • Journal of Physics D: Applied Physics, Vol. 54, Issue 12
  • DOI: 10.1088/1361-6463/abd210

Photoemission of surface oxides and hydrides of delta plutonium
journal, November 2004

Influence of the laser parameters on the space and time characteristics of an aluminum laser-induced plasma
journal, August 2005

  • Barthélemy, O.; Margot, J.; Chaker, M.
  • Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 60, Issue 7-8
  • DOI: 10.1016/j.sab.2005.07.001

Dynamics of femto- and nanosecond laser ablation plumes investigated using optical emission spectroscopy
journal, November 2012

  • Verhoff, B.; Harilal, S. S.; Freeman, J. R.
  • Journal of Applied Physics, Vol. 112, Issue 9
  • DOI: 10.1063/1.4764060

Laser Spectroscopy of UO: Characterization and Assignment of States in the 0- to 3-eV Range, with a Comparison to the Electronic Structure of ThO
journal, March 1994

  • Kaledin, L. A.; Mccord, J. E.; Heaven, M. C.
  • Journal of Molecular Spectroscopy, Vol. 164, Issue 1
  • DOI: 10.1006/jmsp.1994.1055

Time-resolved evaluation of uranium plasma in different atmospheres by laser-induced breakdown spectroscopy
journal, September 2018

Transition probabilities of Ce I obtained from Boltzmann analysis of visible and near-infrared emission spectra
journal, January 2018

  • Nitz, D. E.; Curry, J. J.; Buuck, M.
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 51, Issue 4
  • DOI: 10.1088/1361-6455/aaa658

Experimental Investigation of Uranium Volatility during Vapor Condensation
journal, April 2020

The electronic spectrum of gaseous CeO
journal, April 1979

  • Barrow, R. F.; Clements, R. M.; Harris, S. M.
  • The Astrophysical Journal, Vol. 229
  • DOI: 10.1086/156972

Rotationally resolved electronic spectra for uranium monoxide
journal, August 1985

  • Heaven, Michael C.; Nicolai, Jean-Philippe; Riley, Stephen J.
  • Chemical Physics Letters, Vol. 119, Issue 2-3
  • DOI: 10.1016/0009-2614(85)80065-8

Permanent Electric Dipole Moment of Cerium Monoxide †
journal, November 2009

  • Linton, Colan; Chen, Jinhai; Steimle, Timothy C.
  • The Journal of Physical Chemistry A, Vol. 113, Issue 47
  • DOI: 10.1021/jp9010873

Elucidating uranium monoxide spectral features from a laser-produced plasma
journal, January 2018

  • Harilal, Sivanandan S.; Brumfield, Brian E.; Glumac, Nick
  • Optics Express, Vol. 26, Issue 16
  • DOI: 10.1364/OE.26.020319

Elemental Detection of Cerium and Gadolinium in Aqueous Aerosol Using Laser-Induced Breakdown Spectroscopy
journal, July 2016

The effect of oxygen concentration on the speciation of laser ablated uranium
journal, March 2022

The surface chemistry of cerium oxide
journal, March 2015

Analysis and Spectral Assignments of Mixed Actinide Oxide Samples Using Laser-Induced Breakdown Spectroscopy (LIBS)
journal, April 2013

  • Barefield, James E.; Judge, Elizabeth J.; Berg, John M.
  • Applied Spectroscopy, Vol. 67, Issue 4
  • DOI: 10.1366/12-06830

Persistence of uranium emission in laser-produced plasmas
journal, April 2014

  • LaHaye, N. L.; Harilal, S. S.; Diwakar, P. K.
  • Journal of Applied Physics, Vol. 115, Issue 16
  • DOI: 10.1063/1.4873120

Measurement of Cerium and Gadolinium in Solid Lithium Chloride–Potassium Chloride Salt Using Laser-Induced Breakdown Spectroscopy (LIBS)
journal, July 2017

  • Williams, Ammon; Bryce, Keith; Phongikaroon, Supathorn
  • Applied Spectroscopy, Vol. 71, Issue 10
  • DOI: 10.1177/0003702817709298

Spectroscopic ellipsometry extraction of optical constants for materials from oxide covered samples: Application to the plutonium/oxides system
journal, May 2019

  • Dinh, L. N.; Stanford, J. A.; Saw, C. K.
  • Journal of Applied Physics, Vol. 125, Issue 18
  • DOI: 10.1063/1.5092129

Emission characteristics and dynamics of neutral, ionic and molecular species in a laser produced CaF2 plasma
journal, December 2021

  • Oujja, M.; Camacho, J. J.; Paradela, D.
  • Journal of Quantitative Spectroscopy and Radiative Transfer, Vol. 276
  • DOI: 10.1016/j.jqsrt.2021.107924

Laser Spectroscopy of CeO: Characterization and Assignment of States in the 0-3 eV Range
journal, March 1993

  • Kaledin, L. A.; Mccord, J. E.; Heaven, M. C.
  • Journal of Molecular Spectroscopy, Vol. 158, Issue 1
  • DOI: 10.1006/jmsp.1993.1053

Remote detection of cerium using laser-induced breakdown spectroscopy
conference, June 2013

Spectral dynamics and gas-phase oxidation of laser-produced plutonium plasmas
journal, January 2021

  • Harilal, S. S.; Murzyn, C. M.; Kautz, E. J.
  • Journal of Analytical Atomic Spectrometry, Vol. 36, Issue 1
  • DOI: 10.1039/D0JA00416B

Standoff Detection of Uranium and its Isotopes by Femtosecond Filament Laser Ablation Molecular Isotopic Spectrometry
journal, March 2017

  • Hartig, Kyle C.; Ghebregziabher, Isaac; Jovanovic, Igor
  • Scientific Reports, Vol. 7, Issue 1
  • DOI: 10.1038/srep43852

Unraveling Spatio-Temporal Chemistry Evolution in Laser Ablation Plumes and Its Relation to Initial Plasma Conditions
journal, September 2020

Evolution of uranium monoxide in femtosecond laser-induced uranium plasmas
journal, January 2017

  • Hartig, Kyle C.; Harilal, Sivanandan S.; Phillips, Mark C.
  • Optics Express, Vol. 25, Issue 10
  • DOI: 10.1364/OE.25.011477

Laser Thomson scattering for low-temperature plasmas
journal, January 2011

Analysis of plutonium oxide surrogate residue using laser-induced breakdown spectroscopy
journal, September 2008

  • Zheng, Hongbo; Yueh, Fang Yu; Miller, Tracy
  • Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 63, Issue 9
  • DOI: 10.1016/j.sab.2008.06.005

Plume dynamics and gas-phase molecular formation in transient laser-produced uranium plasmas
journal, August 2019

  • Skrodzki, P. J.; Burger, M.; Jovanovic, I.
  • Physics of Plasmas, Vol. 26, Issue 8
  • DOI: 10.1063/1.5087704

Tracking of oxide formation in laser-produced uranium plasmas
journal, January 2018

  • Skrodzki, P. J.; Burger, M.; Jovanovic, I.
  • Optics Letters, Vol. 43, Issue 20
  • DOI: 10.1364/OL.43.005118

Significance of ambient conditions in uranium absorption and emission features of laser ablation plasmas
journal, November 2016

  • Skrodzki, P. J.; Shah, N. P.; Taylor, N.
  • Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 125
  • DOI: 10.1016/j.sab.2016.09.012

Electronic states of the CeO molecule: Absorption, emission, and laser spectroscopy
journal, December 1983

Comparison of optical emission from nanosecond and femtosecond laser produced plasma in atmosphere and vacuum conditions
journal, September 2013

  • Freeman, J. R.; Harilal, S. S.; Diwakar, P. K.
  • Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 87
  • DOI: 10.1016/j.sab.2013.05.011

Laser spectroscopy of CeO
journal, December 1979

Low Energy Levels of Neutral Cerium (Ce i)
journal, September 1963

Wavelengths and energy levels of the second spectrum of cerium (Ce II)
journal, July 1973

  • Corliss, Charles H.
  • Journal of Research of the National Bureau of Standards Section A: Physics and Chemistry, Vol. 77A, Issue 4
  • DOI: 10.6028/jres.077A.032
    Sort by:
    [ × clear filter / sort ]

    Similar Records in DOE PAGES and OSTI.GOV collections: