TY - JOUR
T1 - Optical spectroscopy and modeling of uranium gas-phase oxidation
T2 - Progress and perspectives
AU - Kautz, Elizabeth J.
AU - Weerakkody, Emily N.
AU - Finko, Mikhail S.
AU - Curreli, Davide
AU - Koroglu, Batikan
AU - Rose, Timothy P.
AU - Weisz, David G.
AU - Crowhurst, Jonathan C.
AU - Radousky, Harry B.
AU - DeMagistris, Michael
AU - Sinha, Neeraj
AU - Levin, Deborah A.
AU - Dreizin, Ed L.
AU - Phillips, Mark C.
AU - Glumac, Nick G.
AU - Harilal, Sivanandan S.
N1 - Publisher Copyright:
© 2021 Elsevier B.V.
PY - 2021/11
Y1 - 2021/11
N2 - Studies related to U gas-phase oxidation through plasma- and thermo-chemistry are important for many fields, including environmental monitoring, forensic analysis, debris analysis in a weapon detonation event, and nucleation physics. Recently, significant efforts have been made to understand the chemical pathways involved in the progression from U atoms to diatoms (UO) and polyatomic molecules (UxOy), employing optical spectroscopy tools and computational modeling. In many studies, laser ablation of U or a U-containing flow reactor are used as a highly resource-efficient, repeatable, tunable, and lab-scale testbed for studying gas-phase oxidation in U plasmas. The spectroscopic analysis of high-temperature gas-phase oxidation of U is challenging due to the congested U spectra, resolution limitations of instrumentation, and the numerous chemical reaction pathways possible. This article focuses on the current understanding and challenges related to studying U plasma chemistry, specifically U gas-phase oxidation and molecular formation, via optical spectroscopy of plasmas and associated computational and spectral modeling. The physical and chemical processes involved in the evolution from U atoms to U oxide molecules to nanoparticles and agglomerates (i.e., debris) are discussed in the context of optical spectroscopic studies. The article concludes by highlighting opportunities for future research efforts based on existing knowledge published in the literature.
AB - Studies related to U gas-phase oxidation through plasma- and thermo-chemistry are important for many fields, including environmental monitoring, forensic analysis, debris analysis in a weapon detonation event, and nucleation physics. Recently, significant efforts have been made to understand the chemical pathways involved in the progression from U atoms to diatoms (UO) and polyatomic molecules (UxOy), employing optical spectroscopy tools and computational modeling. In many studies, laser ablation of U or a U-containing flow reactor are used as a highly resource-efficient, repeatable, tunable, and lab-scale testbed for studying gas-phase oxidation in U plasmas. The spectroscopic analysis of high-temperature gas-phase oxidation of U is challenging due to the congested U spectra, resolution limitations of instrumentation, and the numerous chemical reaction pathways possible. This article focuses on the current understanding and challenges related to studying U plasma chemistry, specifically U gas-phase oxidation and molecular formation, via optical spectroscopy of plasmas and associated computational and spectral modeling. The physical and chemical processes involved in the evolution from U atoms to U oxide molecules to nanoparticles and agglomerates (i.e., debris) are discussed in the context of optical spectroscopic studies. The article concludes by highlighting opportunities for future research efforts based on existing knowledge published in the literature.
KW - Computational fluid dynamics
KW - Plasma chemistry
KW - Plasma diagnostics
KW - Spectral modeling
KW - Uranium
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U2 - 10.1016/j.sab.2021.106283
DO - 10.1016/j.sab.2021.106283
M3 - Review article
AN - SCOPUS:85117365707
SN - 0584-8547
VL - 185
JO - Spectrochimica Acta - Part B Atomic Spectroscopy
JF - Spectrochimica Acta - Part B Atomic Spectroscopy
M1 - 106283
ER -