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

Abstract

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.

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:
Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1426133
Report Number(s):
LLNL-JRNL-741043
Journal ID: ISSN 1089-5639; TRN: US1802225
Grant/Contract Number:  
AC52-07NA27344
Resource 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
Country of Publication:
United States
Language:
English
Subject:
42 ENGINEERING; 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 70 PLASMA PHYSICS AND FUSION

Citation Formats

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., 2018. 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. Thu . "Effects of Plume Hydrodynamics and Oxidation on the Composition of a Condensing Laser-Induced Plasma". United States. doi:10.1021/acs.jpca.7b11994. https://www.osti.gov/servlets/purl/1426133.
@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}
}

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Figures / Tables:

Figure 1 Figure 1: Emission spectra acquired at 550 ns, 3050 ns, 5050 ns, and 9050 ns after ablation of the SrZrO3 target in air. At 550 ns, the spectrum is dominated by Zr atomic emission, though features assigned to ZrO are present. The peak at ~585 nm marked with an asteriskmore » may either be a ZrO emission band or atomic emission from an unidentified impurity. The feature at ~597 nm marked with an asterisk is likely from SrO as it persists at late times and appears readily in the ablation of SrO (Supplementary Materials), though it lies close to a strong Sr atomic emission line. At 3050 ns post-ablation, ZrO emission bands are clearly evident, which give way to the prominent SrO “orange band” at later times. The two persistent atomic lines between 588-600 nm seen at 9050 ns are highly-intense sodium D1 and D2 lines (589.6 nm and 589.0 nm, respectively).« less

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