Time-resolved imaging of atoms and molecules in laser-produced uranium plasmas

Kautz, E. J.; Skrodzki, P. J.; Burger, M.; Bernacki, B. E.; Jovanovic, I.; Phillips, M. C.; Harilal, S. S.

doi:10.1039/c9ja00228f

Time-resolved imaging of atoms and molecules in laser-produced uranium plasmas

Journal Article · Fri Sep 27 00:00:00 EDT 2019 · Journal of Analytical Atomic Spectrometry

DOI:https://doi.org/10.1039/c9ja00228f· OSTI ID:1798667

^[1]; Skrodzki, P. J. ^[2]; Burger, M. ^[2]; Bernacki, B. E. ^[3]; Jovanovic, I. ^[2]; Phillips, M. C. ^[4]; ^[3]

Pacific Northwest National Lab. (PNNL), Richland, WA (United States); University of Michigan
Univ. of Michigan, Ann Arbor, MI (United States)
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)

Gas-phase oxidation of uranium (U), plume chemistry, and the corresponding impact on optical emission features of the U plasma are investigated. Plasmas were produced via nanosecond laser ablation of a natural U target in a chamber where U oxidation was controlled by varying the oxygen partial pressure in an argon cover gas. Monochromatic imaging of U atoms and monoxide (UO) molecules was performed using narrow bandpass optical filters. Results reveal the spatio-temporal evolution of atomic and molecular species in the plasma. U oxides are found to be formed further from the target (in comparison to U atoms), where lower temperatures favor molecular recombination. Segregation between the distribution of U atoms and UO species is observed at later times of plasma evolution, and is more apparent at lower oxygen partial pressures. At higher oxygen partial pressures, significant variation in plume morphology is noticed for UO species, which can be attributed to the higher oxide (U_xO_y) formation further from the target. Here, the monochromatic images of U atoms and UO molecules and corresponding spectral features at various oxygen partial pressures presented here provide unique insight into gas-phase, high-temperature U oxidation and chemistry, with implications for a wide range of nuclear applications, from stand-off detection of radioisotopes to forensics and safeguards.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Michigan, Ann Arbor, MI (United States)

Sponsoring Organization:: USDOE; USDOE National Nuclear Security Administration (NNSA), Office of Nonproliferation and Verification Research and Development

Grant/Contract Number:: AC05-76RL01830; NA0002534

OSTI ID:: 1798667

Alternate ID(s):: OSTI ID: 1566926
OSTI ID: 1574887

Journal Information:: Journal of Analytical Atomic Spectrometry, Journal Name: Journal of Analytical Atomic Spectrometry Journal Issue: 11 Vol. 34; ISSN 0267-9477

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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