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Title: Origin and effect of film sub-stoichiometry on ultraviolet, ns-laser damage resistance of hafnia single layers

Abstract

Understanding the origin of laser damage-prone precursors in high index materials such as hafnia holds the key to the development of laser damage-resistant multilayer dielectric coated optics for high power and energy laser systems. In this study, we investigate the source of sub-stoichiometry, a potent laser damage precursor, in hafnia films produced by an ion beam sputtering (IBS) deposition method and the effect of such defects on the film performance upon ns ultraviolet (UV) laser (8 ns, 355 nm) exposure. Chemical analysis of data obtained via Rutherford backscattering spectroscopy (RBS) suggests that hafnia films deposited at two different planetary locations from the same deposition run exhibit anisotropic and location-dependent stoichiometries. While the oxygen-to-hafnium ratio is at the stoichiometric value of 2 for the hafnia film at the edge location, the ratio is significantly deviated and is 1.7 for that deposited at the planetary center. The sub-stoichiometric hafnia films display a much lower 1-on-1 damage onset at 1.6 ± 0.2 J/cm2 compared to 2.3 ± 0.2 J/cm2 in a stoichiometric film. The low damage performance films also have an over three times higher damage density at fluences above initiation. Coupled with Monte Carlo simulations, we reveal that sub-stoichiometry is primarily attributedmore » to preferential removal of oxygen during film deposition by the bombardment of energetic reflected argon neutrals. The resulting oxygen deficiencies create the sub-bandgap states which facilitate the strong laser energy coupling and reduce the resistance to laser-induced damage in the hafnia single layer films.« less

Authors:
; ; ; ORCiD logo; ; ; ;
Publication Date:
Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA); USDOE Laboratory Directed Research and Development (LDRD) Program
OSTI Identifier:
1604518
Alternate Identifier(s):
OSTI ID: 1605530
Report Number(s):
LLNL-JRNL-790581
Journal ID: ISSN 2159-3930
Grant/Contract Number:  
AC52-07NA27344
Resource Type:
Published Article
Journal Name:
Optical Materials Express
Additional Journal Information:
Journal Name: Optical Materials Express Journal Volume: 10 Journal Issue: 4; Journal ID: ISSN 2159-3930
Publisher:
Optical Society of America (OSA)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Lasers

Citation Formats

Harthcock, Colin, Qiu, S. Roger, Mirkarimi, Paul B., Negres, Raluca A., Guss, Gabe, Menor, Marlon G., Bhowmik, Gourav, and Huang, Mengbing. Origin and effect of film sub-stoichiometry on ultraviolet, ns-laser damage resistance of hafnia single layers. United States: N. p., 2020. Web. doi:10.1364/OME.389416.
Harthcock, Colin, Qiu, S. Roger, Mirkarimi, Paul B., Negres, Raluca A., Guss, Gabe, Menor, Marlon G., Bhowmik, Gourav, & Huang, Mengbing. Origin and effect of film sub-stoichiometry on ultraviolet, ns-laser damage resistance of hafnia single layers. United States. doi:https://doi.org/10.1364/OME.389416
Harthcock, Colin, Qiu, S. Roger, Mirkarimi, Paul B., Negres, Raluca A., Guss, Gabe, Menor, Marlon G., Bhowmik, Gourav, and Huang, Mengbing. Fri . "Origin and effect of film sub-stoichiometry on ultraviolet, ns-laser damage resistance of hafnia single layers". United States. doi:https://doi.org/10.1364/OME.389416.
@article{osti_1604518,
title = {Origin and effect of film sub-stoichiometry on ultraviolet, ns-laser damage resistance of hafnia single layers},
author = {Harthcock, Colin and Qiu, S. Roger and Mirkarimi, Paul B. and Negres, Raluca A. and Guss, Gabe and Menor, Marlon G. and Bhowmik, Gourav and Huang, Mengbing},
abstractNote = {Understanding the origin of laser damage-prone precursors in high index materials such as hafnia holds the key to the development of laser damage-resistant multilayer dielectric coated optics for high power and energy laser systems. In this study, we investigate the source of sub-stoichiometry, a potent laser damage precursor, in hafnia films produced by an ion beam sputtering (IBS) deposition method and the effect of such defects on the film performance upon ns ultraviolet (UV) laser (8 ns, 355 nm) exposure. Chemical analysis of data obtained via Rutherford backscattering spectroscopy (RBS) suggests that hafnia films deposited at two different planetary locations from the same deposition run exhibit anisotropic and location-dependent stoichiometries. While the oxygen-to-hafnium ratio is at the stoichiometric value of 2 for the hafnia film at the edge location, the ratio is significantly deviated and is 1.7 for that deposited at the planetary center. The sub-stoichiometric hafnia films display a much lower 1-on-1 damage onset at 1.6 ± 0.2 J/cm2 compared to 2.3 ± 0.2 J/cm2 in a stoichiometric film. The low damage performance films also have an over three times higher damage density at fluences above initiation. Coupled with Monte Carlo simulations, we reveal that sub-stoichiometry is primarily attributed to preferential removal of oxygen during film deposition by the bombardment of energetic reflected argon neutrals. The resulting oxygen deficiencies create the sub-bandgap states which facilitate the strong laser energy coupling and reduce the resistance to laser-induced damage in the hafnia single layer films.},
doi = {10.1364/OME.389416},
journal = {Optical Materials Express},
number = 4,
volume = 10,
place = {United States},
year = {2020},
month = {3}
}

Journal Article:
Free Publicly Available Full Text
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DOI: https://doi.org/10.1364/OME.389416

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