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Title: Laser-driven hydrothermal process studied with excimer laser pulses

Abstract

Previously, we discovered [Mariella et al., J. Appl. Phys. 114, 014904 (2013)] that modest-fluence/modest-intensity 351-nm laser pulses, with insufficient fluence/intensity to ablate rock, mineral, or concrete samples via surface vaporization, still removed the surface material from water-submerged target samples with confinement of the removed material, and then dispersed at least some of the removed material into the water as a long-lived suspension of nanoparticles. We called this new process, which appears to include the generation of larger colorless particles, “laser-driven hydrothermal processing” (LDHP) [Mariella et al., J. Appl. Phys. 114, 014904 (2013)]. Now, we report that we have studied this process using 248-nm and 193-nm laser light on submerged concrete, quartzite, and obsidian, and, even though light at these wavelengths is more strongly absorbed than at 351 nm, we found that the overall efficiency of LDHP, in terms of the mass of the target removed per Joule of laser-pulse energy, is lower with 248-nm and 193-nm laser pulses than with 351-nm laser pulses. Given that stronger absorption creates higher peak surface temperatures for comparable laser fluence and intensity, it was surprising to observe reduced efficiencies for material removal. We also measured the nascent particle-size distributions that LDHP creates in themore » submerging water and found that they do not display the long tail towards larger particle sizes that we had observed when there had been a multi-week delay between experiments and the date of measuring the size distributions. This is consistent with transient dissolution of the solid surface, followed by diffusion-limited kinetics of nucleation and growth of particles from the resulting thin layer of supersaturated solution at the sample surface.« less

Authors:
ORCiD logo [1];  [1];  [1];  [1];  [1];  [2];  [3];  [3]
+ Show Author Affiliations
  1. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
  2. Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering
  3. Sandia National Lab. (SNL-CA), Livermore, CA (United States)
Publication Date:
Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Sandia National Lab. (SNL-CA), Livermore, CA (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA); USDOD Defense Threat Reduction Agency (DTRA); USDOE Office of Science (SC), Basic Energy Sciences (BES)
Contributing Org.:
U.S. Geological Survey, Menlo Park, CA (United States)
OSTI Identifier:
1458622
Report Number(s):
LLNL-JRNL-698703
Journal ID: ISSN 0021-8979; 829464; TRN: US1901483
Grant/Contract Number:  
AC52-07NA27344
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Applied Physics
Additional Journal Information:
Journal Volume: 122; Journal Issue: 7; Journal ID: ISSN 0021-8979
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; thermodynamic processes; metalloids; lasers; solid surfaces; chemical analysis; gemstones; chemical compounds; metamorphic petrology

Citation Formats

Mariella, Raymond, Rubenchik, Alexander, Fong, Erika, Norton, Mary, Hollingsworth, William, Clarkson, James, Johnsen, Howard, and Osborn, David L. Laser-driven hydrothermal process studied with excimer laser pulses. United States: N. p., 2017. Web. doi:10.1063/1.4999306.
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Mariella, Raymond, Rubenchik, Alexander, Fong, Erika, Norton, Mary, Hollingsworth, William, Clarkson, James, Johnsen, Howard, & Osborn, David L. Laser-driven hydrothermal process studied with excimer laser pulses. United States. https://doi.org/10.1063/1.4999306
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Mariella, Raymond, Rubenchik, Alexander, Fong, Erika, Norton, Mary, Hollingsworth, William, Clarkson, James, Johnsen, Howard, and Osborn, David L. Mon . "Laser-driven hydrothermal process studied with excimer laser pulses". United States. https://doi.org/10.1063/1.4999306. https://www.osti.gov/servlets/purl/1458622.
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@article{osti_1458622,
title = {Laser-driven hydrothermal process studied with excimer laser pulses},
author = {Mariella, Raymond and Rubenchik, Alexander and Fong, Erika and Norton, Mary and Hollingsworth, William and Clarkson, James and Johnsen, Howard and Osborn, David L.},
abstractNote = {Previously, we discovered [Mariella et al., J. Appl. Phys. 114, 014904 (2013)] that modest-fluence/modest-intensity 351-nm laser pulses, with insufficient fluence/intensity to ablate rock, mineral, or concrete samples via surface vaporization, still removed the surface material from water-submerged target samples with confinement of the removed material, and then dispersed at least some of the removed material into the water as a long-lived suspension of nanoparticles. We called this new process, which appears to include the generation of larger colorless particles, “laser-driven hydrothermal processing” (LDHP) [Mariella et al., J. Appl. Phys. 114, 014904 (2013)]. Now, we report that we have studied this process using 248-nm and 193-nm laser light on submerged concrete, quartzite, and obsidian, and, even though light at these wavelengths is more strongly absorbed than at 351 nm, we found that the overall efficiency of LDHP, in terms of the mass of the target removed per Joule of laser-pulse energy, is lower with 248-nm and 193-nm laser pulses than with 351-nm laser pulses. Given that stronger absorption creates higher peak surface temperatures for comparable laser fluence and intensity, it was surprising to observe reduced efficiencies for material removal. We also measured the nascent particle-size distributions that LDHP creates in the submerging water and found that they do not display the long tail towards larger particle sizes that we had observed when there had been a multi-week delay between experiments and the date of measuring the size distributions. This is consistent with transient dissolution of the solid surface, followed by diffusion-limited kinetics of nucleation and growth of particles from the resulting thin layer of supersaturated solution at the sample surface.},
doi = {10.1063/1.4999306},
journal = {Journal of Applied Physics},
number = 7,
volume = 122,
place = {United States},
year = {Mon Aug 21 00:00:00 EDT 2017},
month = {Mon Aug 21 00:00:00 EDT 2017}
}
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https://doi.org/10.1063/1.4999306
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