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

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 SrZrO 3 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 ZrO 2 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 18O 2 environment by observing the in-growth of Zr 18O in the emission spectra relative to Zr 16O, 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.
Authors:
ORCiD logo [1] ;  [1] ;  [2] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [3] ;  [2]
  1. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
  2. Univ. of Illinois, Urbana-Champaign, IL (United States). Department of Nuclear, Plasma, and Radiological Engineering
  3. University of Illinois at Urbana-Champaign, IL (United States). Illinois Applied Research Institute
Publication Date:
Report Number(s):
LLNL-JRNL-741043
Journal ID: ISSN 1089-5639; TRN: US1802225
Grant/Contract Number:
AC52-07NA27344
Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory
Additional Journal Information:
Journal Volume: 122; Journal Issue: 6; Journal ID: ISSN 1089-5639
Publisher:
American Chemical Society
Research Org:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
42 ENGINEERING; 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 70 PLASMA PHYSICS AND FUSION
OSTI Identifier:
1426133

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, and Curreli, Davide. Effects of Plume Hydrodynamics and Oxidation on the Composition of a Condensing Laser-Induced Plasma. United States: N. p., Web. doi:10.1021/acs.jpca.7b11994.
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. Effects of Plume Hydrodynamics and Oxidation on the Composition of a Condensing Laser-Induced Plasma. United States. doi:10.1021/acs.jpca.7b11994.
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, and Curreli, Davide. 2018. "Effects of Plume Hydrodynamics and Oxidation on the Composition of a Condensing Laser-Induced Plasma". United States. doi:10.1021/acs.jpca.7b11994.
@article{osti_1426133,
title = {Effects of Plume Hydrodynamics and Oxidation on the Composition of a Condensing Laser-Induced Plasma},
author = {Weisz, David G. and Crowhurst, Jonathan C. and Finko, Mikhail S. and Rose, Timothy P. and Koroglu, Batikan and Trappitsch, Reto and Radousky, Harry B. and Siekhaus, Wigbert J. and Armstrong, Michael R. and Isselhardt, Brett H. and Azer, Magdi and Curreli, Davide},
abstractNote = {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.},
doi = {10.1021/acs.jpca.7b11994},
journal = {Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory},
number = 6,
volume = 122,
place = {United States},
year = {2018},
month = {2}
}