skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Time-resolved imaging of atoms and molecules in laser-produced uranium plasmas

Abstract

Gas-phase oxidation of uranium (U), plume chemistry, and its impact on optical emission features of the uranium plasma are investigated. Plasmas were produced via nanosecond laser ablation of a natural uranium target in a chamber where uranium oxidation was controlled by varying the oxygen partial pressure within argon cover gas. Monochromatic imaging of uranium atoms and monoxide molecules was performed using narrowband optical filters, which clearly reveals the spatio-temporal evolution of these species in the plasma. Uranium oxides are found to be formed at the plasma edges, where lower temperatures favor molecular recombination. Segregation between the distribution of uranium atoms and monoxide species is observed at later times of plasma evolution, and is more apparent at lower oxygen partial pressures. At higher oxygen partial pressures, significant variation in plume morphology is noticed for UO species, which is attributed to higher rate of oxide (UxOy) formation at the plume edges. The monochromatic images of U atoms and molecules and corresponding spectral features at various oxygen partial pressures presented here provide a unique insight into gas-phase, high-temperature uranium oxidation, and its chemistry and have implications for a wide range of nuclear applications, from stand-off detection of radioisotopes to forensics and safeguards.

Authors:
 [1];  [2];  [2];  [1];  [3];  [4]; ORCiD logo [1]
  1. BATTELLE (PACIFIC NW LAB)
  2. UNIVERSITY OF MICHIGAN
  3. University of Michigan
  4. UNIVERSITY PROGRAMS
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1574887
Report Number(s):
PNNL-SA-144962
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Journal of Analytical Atomic Spectrometry
Additional Journal Information:
Journal Volume: 34; Journal Issue: 11
Country of Publication:
United States
Language:
English
Subject:
(140.3440) Laser-induced breakdown, (280.4788) Optical Sensing, (280.5395) Plasma Diagnostics, (300.2140) Emission Spectroscopy, 2D fast imaging, plasma chemistry

Citation Formats

Kautz, Elizabeth J., Skrodzki, Patrick J., Burger, Milos, Bernacki, Bruce E., Jovanovic, Igor, Phillips, Mark C., and Harilal, Sivanandan S. Time-resolved imaging of atoms and molecules in laser-produced uranium plasmas. United States: N. p., 2019. Web. doi:10.1039/C9JA00228F.
Kautz, Elizabeth J., Skrodzki, Patrick J., Burger, Milos, Bernacki, Bruce E., Jovanovic, Igor, Phillips, Mark C., & Harilal, Sivanandan S. Time-resolved imaging of atoms and molecules in laser-produced uranium plasmas. United States. doi:10.1039/C9JA00228F.
Kautz, Elizabeth J., Skrodzki, Patrick J., Burger, Milos, Bernacki, Bruce E., Jovanovic, Igor, Phillips, Mark C., and Harilal, Sivanandan S. Fri . "Time-resolved imaging of atoms and molecules in laser-produced uranium plasmas". United States. doi:10.1039/C9JA00228F.
@article{osti_1574887,
title = {Time-resolved imaging of atoms and molecules in laser-produced uranium plasmas},
author = {Kautz, Elizabeth J. and Skrodzki, Patrick J. and Burger, Milos and Bernacki, Bruce E. and Jovanovic, Igor and Phillips, Mark C. and Harilal, Sivanandan S.},
abstractNote = {Gas-phase oxidation of uranium (U), plume chemistry, and its impact on optical emission features of the uranium plasma are investigated. Plasmas were produced via nanosecond laser ablation of a natural uranium target in a chamber where uranium oxidation was controlled by varying the oxygen partial pressure within argon cover gas. Monochromatic imaging of uranium atoms and monoxide molecules was performed using narrowband optical filters, which clearly reveals the spatio-temporal evolution of these species in the plasma. Uranium oxides are found to be formed at the plasma edges, where lower temperatures favor molecular recombination. Segregation between the distribution of uranium atoms and monoxide species is observed at later times of plasma evolution, and is more apparent at lower oxygen partial pressures. At higher oxygen partial pressures, significant variation in plume morphology is noticed for UO species, which is attributed to higher rate of oxide (UxOy) formation at the plume edges. The monochromatic images of U atoms and molecules and corresponding spectral features at various oxygen partial pressures presented here provide a unique insight into gas-phase, high-temperature uranium oxidation, and its chemistry and have implications for a wide range of nuclear applications, from stand-off detection of radioisotopes to forensics and safeguards.},
doi = {10.1039/C9JA00228F},
journal = {Journal of Analytical Atomic Spectrometry},
number = 11,
volume = 34,
place = {United States},
year = {2019},
month = {11}
}

Works referenced in this record:

Rapid extraction and assay of uranium from environmental surface samples
journal, October 2017


Phase transformation of metastable discontinuous precipitation products to equilibrium phases in U10Mo alloys
journal, November 2018


The Attractiveness of Materials in Advanced Nuclear Fuel Cycles for Various Proliferation and Theft Scenarios
journal, July 2012

  • Bathke, Charles G.; Ebbinghaus, Bartley B.; Collins, Brian A.
  • Nuclear Technology, Vol. 179, Issue 1
  • DOI: 10.13182/NT10-203

Nanoscale Spatially Resolved Mapping of Uranium Enrichment
journal, August 2019


New Resonance Ionization Mass Spectrometry Scheme for Improved Uranium Analysis
journal, July 2018


Phase discrimination of uranium oxides using laser-induced breakdown spectroscopy
journal, August 2017

  • Campbell, Keri R.; Wozniak, Nicholas R.; Colgan, James P.
  • Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 134
  • DOI: 10.1016/j.sab.2017.05.007

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

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

Optical spectroscopy of laser-produced plasmas for standoff isotopic analysis
journal, June 2018

  • Harilal, S. S.; Brumfield, B. E.; LaHaye, N. L.
  • Applied Physics Reviews, Vol. 5, Issue 2
  • DOI: 10.1063/1.5016053

Single-shot, multi-signature remote detection of uranium by filament-induced breakdown spectroscopy
journal, January 2019

  • Finney, L. A.; Skrodzki, P. J.; Burger, M.
  • Optics Letters, Vol. 44, Issue 11
  • DOI: 10.1364/OL.44.002783

Two-dimensional fluorescence spectroscopy of uranium isotopes in femtosecond laser ablation plumes
journal, June 2017


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

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

Simulation of uranium plasma plume dynamics in atmospheric oxygen produced via femtosecond laser ablation
journal, August 2018

  • Finko, Mikhail S.; Curreli, Davide
  • Physics of Plasmas, Vol. 25, Issue 8
  • DOI: 10.1063/1.5034470

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

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

Combination of atomic lines and molecular bands for uranium optical isotopic analysis in laser induced plasma spectrometry
journal, February 2017

  • Mao, Xianglei; Chan, George C. -Y.; Choi, Inhee
  • Journal of Radioanalytical and Nuclear Chemistry, Vol. 312, Issue 1
  • DOI: 10.1007/s10967-017-5197-y

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

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

Effects of Plume Hydrodynamics and Oxidation on the Composition of a Condensing Laser-Induced Plasma
journal, February 2018

  • Weisz, David G.; Crowhurst, Jonathan C.; Finko, Mikhail S.
  • The Journal of Physical Chemistry A, Vol. 122, Issue 6
  • DOI: 10.1021/acs.jpca.7b11994

Influence of Ambient Gas on Laser-Induced Breakdown Spectroscopy of Uranium Metal
journal, November 2015


A model of early formation of uranium molecular oxides in laser-ablated plasmas
journal, November 2017

  • Finko, Mikhail S.; Curreli, Davide; Weisz, David G.
  • Journal of Physics D: Applied Physics, Vol. 50, Issue 48
  • DOI: 10.1088/1361-6463/aa92f5

Diagnostics and simulations of molecular formation in laser-induced plasmas
journal, October 2018

  • Dietz, Thomas; Kohns, Peter; Ankerhold, Georg
  • Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 148
  • DOI: 10.1016/j.sab.2018.06.007

Radiative models of laser-induced plasma and pump-probe diagnostics relevant to laser-induced breakdown spectroscopy
journal, May 2010

  • Gornushkin, Igor B.; Panne, Ulrich
  • Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 65, Issue 5
  • DOI: 10.1016/j.sab.2010.03.021

Nonisothermal asymmetric expansion of laser induced plasmas into vacuum
journal, October 2006

  • Gornushkin, I. B.; Shabanov, S. V.; Omenetto, N.
  • Journal of Applied Physics, Vol. 100, Issue 7
  • DOI: 10.1063/1.2345460

Laser-generated plasma plume expansion: Combined continuous-microscopic modeling
journal, December 2002


Investigation of nanoparticle generation during femtosecond laser ablation of metals
journal, May 2007


Measurement Technique of Boron Isotopic Ratio by Laser-induced Breakdown Spectroscopy
journal, January 1998


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

Shock Wave Mediated Plume Chemistry for Molecular Formation in Laser Ablation Plasmas
journal, January 2016


Molecule formation induced by non-uniform plume–air interactions in laser induced plasma
journal, January 2017

  • Ran, Pengxu; Hou, Huaming; Luo, Sheng-Nian
  • Journal of Analytical Atomic Spectrometry, Vol. 32, Issue 11
  • DOI: 10.1039/C7JA00287D

Insight into the Formation of Molecular Species in Laser-Induced Plasma of Isotopically Labeled Organic Samples
journal, September 2015


Molecular formation in the stagnation region of colliding laser-produced plasmas
journal, October 2016


Multidiagnostic analysis of ion dynamics in ultrafast laser ablation of metals over a large fluence range
journal, February 2015

  • Anoop, K. K.; Polek, M. P.; Bruzzese, R.
  • Journal of Applied Physics, Vol. 117, Issue 8
  • DOI: 10.1063/1.4913505

Experimental and theoretical investigations of a laser-produced aluminum plasma
journal, August 2008


Morphological changes in ultrafast laser ablation plumes with varying spot size
journal, January 2015

  • Harilal, S. S.; Diwakar, P. K.; Polek, M. P.
  • Optics Express, Vol. 23, Issue 12
  • DOI: 10.1364/OE.23.015608

Temporally and spectrally resolved imaging of laser-induced plasmas
journal, January 2004


Emission features and expansion dynamics of nanosecond laser ablation plumes at different ambient pressures
journal, January 2014

  • Farid, N.; Harilal, S. S.; Ding, H.
  • Journal of Applied Physics, Vol. 115, Issue 3
  • DOI: 10.1063/1.4862167

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

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

Internal structure and expansion dynamics of laser ablation plumes into ambient gases
journal, March 2003

  • Harilal, S. S.; Bindhu, C. V.; Tillack, M. S.
  • Journal of Applied Physics, Vol. 93, Issue 5
  • DOI: 10.1063/1.1544070

Laser-induced plasma expansion: theoretical and experimental aspects
journal, March 2004

  • Capitelli, M.; Casavola, A.; Colonna, G.
  • Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 59, Issue 3
  • DOI: 10.1016/j.sab.2003.12.017

Modeling chemical reactions in laser-induced plasmas
journal, September 2015


Theoretical investigation of the Rayleigh-Taylor instability in laser-produced plasmas driving into background gases
journal, August 2007

  • Rifai, K.; Vidal, F.; Johnston, T. W.
  • Physics of Plasmas, Vol. 14, Issue 8
  • DOI: 10.1063/1.2766497