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Title: Significance of ambient conditions in uranium absorption and emission features of laser ablation plasmas

This study employs laser ablation (LA) to investigate mechanisms for U optical signal variation under various environmental conditions during laser absorption spectroscopy (LAS) and optical emission spectroscopy (OES). Potential mechanisms explored for signal quenching related to ambient conditions include plasma chemistry (e.g., uranium oxide formation), ambient gas confinement effects, and other collisional interactions between plas-ma constituents and the ambient gas. LA-LAS studies show that the persistence of the U ground state population is significantly reduced in the presence of air ambient compared to nitrogen. LA-OES yields congested spectra from which the U I 356.18 nm transition is prominent and serves as the basis for signal tracking. LA-OES signal and per-sistence vary negligibly between the test gases (air and N 2), unlike the LA-LAS results. The plume hydrodynamic features and plume fundamental properties showed similar results in both air and nitrogen ambient. In conclusion, investigation of U oxide formation in the laser-produced plasma suggests that low U concentration in a sample hinders consistent detection of UO molecular spectra.
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [3] ;  [3] ;  [5] ;  [3] ;  [3]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Nuclear and Radiological Sciences; Purdue Univ., West Lafayette, IN (United States). School of Nuclear Engineering
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Nuclear and Radiological Sciences
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  4. Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Pennsylvania State Univ., University Park, PA (United States). Dept. of Mechanical and Nuclear Engineering
  5. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Nuclear and Radiological Sciences
Publication Date:
Grant/Contract Number:
NA0002534; AC05-76RL01830; 2012.05 DN-130-NF0001; AC05-76RLO1830
Type:
Accepted Manuscript
Journal Name:
Spectrochimica Acta. Part B, Atomic Spectroscopy
Additional Journal Information:
Journal Volume: 125; Journal Issue: C; Journal ID: ISSN 0584-8547
Publisher:
Elsevier
Research Org:
Univ. of Michigan, Ann Arbor, MI (United States)
Sponsoring Org:
USDOE National Nuclear Security Administration (NNSA); US Department of Homeland Security (DHS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Laser ablation; Optical emission spectroscopy (OES); Laser absorption spectroscopy (LAS); Laser-induced breakdown spectroscopy (LIBS) Plasma chemistry; Plasma diagnostics
OSTI Identifier:
1367669
Alternate Identifier(s):
OSTI ID: 1397006

Skrodzki, P. J., Shah, N. P., Taylor, N., Hartig, K. C., LaHaye, N. L., Brumfield, B. E., Jovanovic, I., Phillips, M. C., and Harilal, S. S.. Significance of ambient conditions in uranium absorption and emission features of laser ablation plasmas. United States: N. p., Web. doi:10.1016/j.sab.2016.09.012.
Skrodzki, P. J., Shah, N. P., Taylor, N., Hartig, K. C., LaHaye, N. L., Brumfield, B. E., Jovanovic, I., Phillips, M. C., & Harilal, S. S.. Significance of ambient conditions in uranium absorption and emission features of laser ablation plasmas. United States. doi:10.1016/j.sab.2016.09.012.
Skrodzki, P. J., Shah, N. P., Taylor, N., Hartig, K. C., LaHaye, N. L., Brumfield, B. E., Jovanovic, I., Phillips, M. C., and Harilal, S. S.. 2016. "Significance of ambient conditions in uranium absorption and emission features of laser ablation plasmas". United States. doi:10.1016/j.sab.2016.09.012. https://www.osti.gov/servlets/purl/1367669.
@article{osti_1367669,
title = {Significance of ambient conditions in uranium absorption and emission features of laser ablation plasmas},
author = {Skrodzki, P. J. and Shah, N. P. and Taylor, N. and Hartig, K. C. and LaHaye, N. L. and Brumfield, B. E. and Jovanovic, I. and Phillips, M. C. and Harilal, S. S.},
abstractNote = {This study employs laser ablation (LA) to investigate mechanisms for U optical signal variation under various environmental conditions during laser absorption spectroscopy (LAS) and optical emission spectroscopy (OES). Potential mechanisms explored for signal quenching related to ambient conditions include plasma chemistry (e.g., uranium oxide formation), ambient gas confinement effects, and other collisional interactions between plas-ma constituents and the ambient gas. LA-LAS studies show that the persistence of the U ground state population is significantly reduced in the presence of air ambient compared to nitrogen. LA-OES yields congested spectra from which the U I 356.18 nm transition is prominent and serves as the basis for signal tracking. LA-OES signal and per-sistence vary negligibly between the test gases (air and N2), unlike the LA-LAS results. The plume hydrodynamic features and plume fundamental properties showed similar results in both air and nitrogen ambient. In conclusion, investigation of U oxide formation in the laser-produced plasma suggests that low U concentration in a sample hinders consistent detection of UO molecular spectra.},
doi = {10.1016/j.sab.2016.09.012},
journal = {Spectrochimica Acta. Part B, Atomic Spectroscopy},
number = C,
volume = 125,
place = {United States},
year = {2016},
month = {10}
}