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Physical conditions for UO formation in laser-produced uranium plumes

Journal Article · · Physical Chemistry Chemical Physics. PCCP
DOI:https://doi.org/10.1039/C9CP02250C· OSTI ID:1601803

Laser-induced plasma spectroscopy is a powerful method for elemental detection and analysis, however the broadening and merging of densely packed spectral lines can make it especially challenging for studying high-Z elements such as uranium and other actinides. In order to understand the processes occurring in laser-induced plasma, it is necessary to evaluate the variation of its thermodynamic parameters. We performed spatiotemporal diagnostics of uranium species in plasma plumes produced by nanosecond near-infrared laser pulses in low- pressure environment. Spatially- and temporally-resolved emission spectroscopy experiments are supported by modeling of uranium emission and its persistence in the plume. Saha-Eggert equation as well as Boltzmann diagrams generated from numerous U I transitions are used to infer temperature. We report the rst measurements of uranium Stark broadening parameters for U I 499.01 nm and U II 500.82 nm transitions. The Stark widths of selected U transitions were measured by comparing their linewidths with the broadening of O I 777.19 nm line. Electron density was found to be on the order of 1016 cm??3, while the temperature was found to be in the range of 3000{8000 K. In addition to enhancing the fundamental understanding of high-Z plasmas under reduced-pressure environments, the knowledge of Stark broadening parameters could improve modeling capabilities and analytical performance of techniques that rely on emission plasma spectroscopy.

Research Organization:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE National Nuclear Security Administration (NNSA), Office of Defense Nuclear Nonproliferation
DOE Contract Number:
AC05-76RL01830
OSTI ID:
1601803
Report Number(s):
PNNL-SA-142809
Journal Information:
Physical Chemistry Chemical Physics. PCCP, Vol. 21, Issue 29
Country of Publication:
United States
Language:
English

References (42)

Internal structure and expansion dynamics of laser ablation plumes into ambient gases journal March 2003
Atomic-scale Studies of Uranium Oxidation and Corrosion by Water Vapour journal July 2016
Gas Phase Chemical Evolution of Uranium, Aluminum, and Iron Oxides journal July 2018
A comparison of single and double pulse laser-induced breakdown spectroscopy of aluminum samples journal July 2002
A model of early formation of uranium molecular oxides in laser-ablated plasmas journal November 2017
Molecular formation dynamics of 5-nitro-2,4-dihydro-3H-1,2,4-triazol-3-one, 1,3,5-trinitroperhydro-1,3,5-triazine, and 2,4,6-trinitrotoluene in air, nitrogen, and argon atmospheres studied using femtosecond laser induced breakdown spectroscopy journal September 2013
Elucidating uranium monoxide spectral features from a laser-produced plasma journal January 2018
Two-dimensional fluorescence spectroscopy of uranium isotopes in femtosecond laser ablation plumes journal June 2017
Atlas of uranium emission intensities in a hollow cathode discharge report July 1980
Formation of 238 U 16 O and 238 U 18 O observed by time-resolved emission spectroscopy subsequent to laser ablation journal July 2017
Laser-Induced Breakdown Spectroscopy (LIBS), Part II: Review of Instrumental and Methodological Approaches to Material Analysis and Applications to Different Fields journal April 2012
Energy levels of neutral atomic uranium (Ui) journal January 1976
Combination of atomic lines and molecular bands for uranium optical isotopic analysis in laser induced plasma spectrometry journal February 2017
Temperature and density of an expanding laser produced plasma journal March 1974
Analysis of geological materials containing uranium using laser-induced breakdown spectroscopy journal June 2016
Introduction to Plasma Spectroscopy book January 2009
Shock Wave Mediated Plume Chemistry for Molecular Formation in Laser Ablation Plasmas journal January 2016
Temporally resolved laser induced plasma diagnostics of single crystal silicon — Effects of ambient pressure journal October 2008
Simulation of uranium plasma plume dynamics in atmospheric oxygen produced via femtosecond laser ablation journal August 2018
Multiple emission line analysis for improved isotopic determination of uranium — a computer simulation study journal November 2013
Electronic Spectroscopy of UO journal September 1997
Emission features and expansion dynamics of nanosecond laser ablation plumes at different ambient pressures journal January 2014
Quantitative Analysis of Additives in Solid Zinc Alloys by Laser-induced Plasma Spectrometry journal January 1997
Evolution of uranium monoxide in femtosecond laser-induced uranium plasmas journal January 2017
Propagation dynamics of a LaMnO3 laser ablation plume in an oxygen atmosphere journal July 2006
Dual-comb spectroscopy of laser-induced plasmas journal March 2018
Laser-induced breakdown spectroscopy for determination of uranium in thorium–uranium mixed oxide fuel materials journal May 2009
Plasma plume induced during ArF laser ablation of hydroxyapatite journal December 2008
Insight into the Formation of Molecular Species in Laser-Induced Plasma of Isotopically Labeled Organic Samples journal September 2015
Energy levels and isotope shifts for singly ionized uranium (U II) journal January 1994
Molecular signatures in femtosecond laser-induced organic plasmas: comparison with nanosecond laser ablation journal January 2016
Tracking of oxide formation in laser-produced uranium plasmas journal January 2018
Influence of Ambient Gas on Laser-Induced Breakdown Spectroscopy of Uranium Metal journal November 2015
Standoff analysis of laser-produced plasmas using laser-induced fluorescence journal January 2018
Experimental and theoretical investigations of a laser-produced aluminum plasma journal August 2008
Enhanced shock wave detection sensitivity for laser-produced plasmas in low pressure ambient gases using interferometry journal November 2012
Persistence of atomic spectral line on laser-induced Cu plasma with spatial confinement journal November 2016
Laser-induced breakdown spectroscopy measurements of uranium and thorium powders and uranium ore journal May 2013
Impact of oxygen chemistry on the emission and fluorescence spectroscopy of laser ablation plumes journal September 2017
Significance of ambient conditions in uranium absorption and emission features of laser ablation plasmas journal November 2016
Optical spectroscopy of laser-produced plasmas for standoff isotopic analysis journal June 2018
Dual-Comb Spectroscopy of Laser-Induced Plasmas conference January 2017

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