Effects of Plume Hydrodynamics and Oxidation on the Composition of a Condensing Laser-Induced Plasma

Weisz, David G.; Crowhurst, Jonathan C.; Finko, Mikhail S.; Rose, Timothy P.; Koroglu, Batikan; Trappitsch, Reto; Radousky, Harry B.; Siekhaus, Wigbert J.; Armstrong, Michael R.; Isselhardt, Brett H.; Azer, Magdi; Curreli, Davide

doi:10.1021/acs.jpca.7b11994

Title: Effects of Plume Hydrodynamics and Oxidation on the Composition of a Condensing Laser-Induced Plasma

Journal Article · Thu Feb 01 00:00:00 EST 2018 · Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory

DOI:https://doi.org/10.1021/acs.jpca.7b11994· OSTI ID:1426133

^[1]; Crowhurst, Jonathan C. ^[1]; Finko, Mikhail S. ^[2]; Rose, Timothy P. ^[1]; Koroglu, Batikan ^[1]; Trappitsch, Reto ^[1]; Radousky, Harry B. ^[1]; Siekhaus, Wigbert J. ^[1]; Armstrong, Michael R. ^[1]; Isselhardt, Brett H. ^[1]; Azer, Magdi ^[3]; Curreli, Davide ^[2]

Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Univ. of Illinois, Urbana-Champaign, IL (United States). Department of Nuclear, Plasma, and Radiological Engineering
University of Illinois at Urbana-Champaign, IL (United States). Illinois Applied Research Institute

High-temperature chemistry in laser ablation plumes leads to vapor-phase speciation, which can induce chemical fractionation during condensation. In this work, using emission spectroscopy acquired after ablation of a SrZrO₃ target, we have experimentally observed the formation of multiple molecular species (ZrO and SrO) as a function of time as the laser ablation plume evolves. Although the stable oxides SrO and ZrO₂ are both refractory, we observed emission from the ZrO intermediate at earlier times than SrO. We deduced the time-scale of oxygen entrainment into the laser ablation plume using an ¹⁸O₂ environment by observing the in-growth of Zr¹⁸O in the emission spectra relative to Zr¹⁶O, which was formed by reaction of Zr with ¹⁶O from the target itself. Using temporally resolved plume-imaging, we determined that ZrO formed more readily at early times, volumetrically in the plume, while SrO formed later in time, around the periphery. Lastly, using a simple temperature-dependent reaction model, we have illustrated that the formation sequence of these oxides subsequent to ablation is predictable to first order.

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Research Organization:: Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 1426133

Report Number(s):: LLNL-JRNL-741043; TRN: US1802225

Journal Information:: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory, Vol. 122, Issue 6; ISSN 1089-5639

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 19 works

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