Physical conditions for UO formation in laser-produced uranium plumes
Abstract
In this paper, we investigate the oxidation of uranium (U) species, the physical conditions leading to uranium monoxide (UO) formation and the interplay between plume hydrodynamics and plasma chemistry in a laser-produced U plasma. Plasmas are produced by ablation of metallic U using nanosecond laser pulses. An ambient gas environment with varying oxygen partial pressures in 100 Torr inert Ar gas is used for controlling the plasma oxidation chemistry. Optical emission spectroscopic analysis of U atomic and monoxide species shows a reduction in the emission intensity and persistence with increasing oxygen partial pressure. Spectral modelling is used for identifying the physical conditions in the plasma that favor UO formation. The optimal temperature for UO formation is found to be in the temperature range of ~1500–5000 K. The spectrally integrated and spectrally filtered (monochromatic) imaging of U atomic and molecular species reveals the evolutionary paths of various species in the plasma. Our results also highlight that oxidation in U plasmas predominantly occurs at the cooler periphery and is delayed with respect to plasma formation, and the dissipation of molecular species strongly depends on oxygen partial pressure.
- Authors:
-
[1];
[1];
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Univ. of Arizona, Tucson, AZ (United States); Opticslah, LLC, Albuquerque, NM (United States)
- Univ. of Michigan, Ann Arbor, MI (United States)
- Publication Date:
- Research Org.:
- Univ. of Michigan, Ann Arbor, MI (United States)
- Sponsoring Org.:
- USDOE National Nuclear Security Administration (NNSA), Office of Defense Nuclear Nonproliferation; National Science Foundation (NSF)
- OSTI Identifier:
- 1798654
- Alternate Identifier(s):
- OSTI ID: 1544589
- Grant/Contract Number:
- NA0002534; AC05-76RLO1830; DGE 1256260
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Chemistry Chemical Physics. PCCP
- Additional Journal Information:
- Journal Volume: 21; Journal Issue: 29; Journal ID: ISSN 1463-9076
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY
Citation Formats
Harilal, S. S., Kautz, E. J., Bernacki, B. E., Phillips, M. C., Skrodzki, P. J., Burger, M., and Jovanovic, I. Physical conditions for UO formation in laser-produced uranium plumes. United States: N. p., 2019.
Web. doi:10.1039/c9cp02250c.
Harilal, S. S., Kautz, E. J., Bernacki, B. E., Phillips, M. C., Skrodzki, P. J., Burger, M., & Jovanovic, I. Physical conditions for UO formation in laser-produced uranium plumes. United States. https://doi.org/10.1039/c9cp02250c
Harilal, S. S., Kautz, E. J., Bernacki, B. E., Phillips, M. C., Skrodzki, P. J., Burger, M., and Jovanovic, I. Wed .
"Physical conditions for UO formation in laser-produced uranium plumes". United States. https://doi.org/10.1039/c9cp02250c. https://www.osti.gov/servlets/purl/1798654.
@article{osti_1798654,
title = {Physical conditions for UO formation in laser-produced uranium plumes},
author = {Harilal, S. S. and Kautz, E. J. and Bernacki, B. E. and Phillips, M. C. and Skrodzki, P. J. and Burger, M. and Jovanovic, I.},
abstractNote = {In this paper, we investigate the oxidation of uranium (U) species, the physical conditions leading to uranium monoxide (UO) formation and the interplay between plume hydrodynamics and plasma chemistry in a laser-produced U plasma. Plasmas are produced by ablation of metallic U using nanosecond laser pulses. An ambient gas environment with varying oxygen partial pressures in 100 Torr inert Ar gas is used for controlling the plasma oxidation chemistry. Optical emission spectroscopic analysis of U atomic and monoxide species shows a reduction in the emission intensity and persistence with increasing oxygen partial pressure. Spectral modelling is used for identifying the physical conditions in the plasma that favor UO formation. The optimal temperature for UO formation is found to be in the temperature range of ~1500–5000 K. The spectrally integrated and spectrally filtered (monochromatic) imaging of U atomic and molecular species reveals the evolutionary paths of various species in the plasma. Our results also highlight that oxidation in U plasmas predominantly occurs at the cooler periphery and is delayed with respect to plasma formation, and the dissipation of molecular species strongly depends on oxygen partial pressure.},
doi = {10.1039/c9cp02250c},
journal = {Physical Chemistry Chemical Physics. PCCP},
number = 29,
volume = 21,
place = {United States},
year = {Wed Jul 03 00:00:00 EDT 2019},
month = {Wed Jul 03 00:00:00 EDT 2019}
}
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Works referencing / citing this record:
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