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Title: Physical conditions for UO formation in laser-produced uranium plumes

Abstract

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 Starkmore » broadening parameters could improve modeling capabilities and analytical performance of techniques that rely on emission plasma spectroscopy.« less

Authors:
ORCiD logo [1];  [1];  [1];  [2];  [3];  [3];  [4]
  1. BATTELLE (PACIFIC NW LAB)
  2. UNIVERSITY PROGRAMS
  3. UNIVERSITY OF MICHIGAN
  4. University of Michigan
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1601803
Report Number(s):
PNNL-SA-142809
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Physical Chemistry Chemical Physics. PCCP
Additional Journal Information:
Journal Volume: 21; Journal Issue: 29
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, Uranim

Citation Formats

Harilal, Sivanandan S., Kautz, Elizabeth J., Bernacki, Bruce E., Phillips, Mark C., Skrodzki, Patrick J., Burger, Milos, and Jovanovic, I. Physical conditions for UO formation in laser-produced uranium plumes. United States: N. p., 2019. Web. doi:10.1039/C9CP02250C.
Harilal, Sivanandan S., Kautz, Elizabeth J., Bernacki, Bruce E., Phillips, Mark C., Skrodzki, Patrick J., Burger, Milos, & Jovanovic, I. Physical conditions for UO formation in laser-produced uranium plumes. United States. doi:10.1039/C9CP02250C.
Harilal, Sivanandan S., Kautz, Elizabeth J., Bernacki, Bruce E., Phillips, Mark C., Skrodzki, Patrick J., Burger, Milos, and Jovanovic, I. Wed . "Physical conditions for UO formation in laser-produced uranium plumes". United States. doi:10.1039/C9CP02250C.
@article{osti_1601803,
title = {Physical conditions for UO formation in laser-produced uranium plumes},
author = {Harilal, Sivanandan S. and Kautz, Elizabeth J. and Bernacki, Bruce E. and Phillips, Mark C. and Skrodzki, Patrick J. and Burger, Milos and Jovanovic, I},
abstractNote = {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.},
doi = {10.1039/C9CP02250C},
journal = {Physical Chemistry Chemical Physics. PCCP},
number = 29,
volume = 21,
place = {United States},
year = {2019},
month = {8}
}

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