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Title: 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:1798654
ORCiD logo [1]; ORCiD logo [1];  [1];  [2];  [3];  [3];  [3]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Univ. of Arizona, Tucson, AZ (United States); Opticslah, LLC, Albuquerque, NM (United States)
  3. Univ. of Michigan, Ann Arbor, MI (United States)

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.

Research Organization:
Univ. of Michigan, Ann Arbor, MI (United States)
Sponsoring Organization:
USDOE National Nuclear Security Administration (NNSA), Office of Defense Nuclear Nonproliferation; National Science Foundation (NSF)
Grant/Contract Number:
NA0002534; AC05-76RLO1830; DGE 1256260
OSTI ID:
1798654
Alternate ID(s):
OSTI ID: 1544589
Journal Information:
Physical Chemistry Chemical Physics. PCCP, Vol. 21, Issue 29; ISSN 1463-9076
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 27 works
Citation information provided by
Web of Science

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

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