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Title: Compositional dependence of linear and nonlinear optical response in crystalline hafnium zirconium oxide thin films

Abstract

Composition dependence of second harmonic generation, refractive index, extinction coefficient, and optical bandgap in 20 nm thick crystalline Hf1–xZrxO2 (0 ≤ x ≤ 1) thin films is reported here. The refractive index exhibits a general increase with increasing ZrO2 content with all values within the range of 1.98–2.14 from 880 nm to 400 nm wavelengths. A composition dependence of the indirect optical bandgap is observed, decreasing from 5.81 eV for HfO2 to 5.17 eV for Hf0.4Zr0.6O2. The bandgap increases for compositions with x > 0.6, reaching 5.31 eV for Hf0.1Zr0.9O2. Second harmonic signals are measured for 880 nm incident light. The magnitude of the second harmonic signal scales with the magnitude of the remanant polarization in the composition series. Film compositions that display near zero remanent polarizations exhibit minimal second harmonic generation while those with maximum remanent polarization also display the largest second harmonic signal. The results are discussed in the context of ferroelectric phase assemblage in the hafnium zirconium oxide films and demonstrate a path toward a silicon-compatible integrated nonlinear optical material.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [4]; ORCiD logo [4];  [4];  [4];  [1]; ORCiD logo [1];  [3];  [3]; ORCiD logo [3]
+ Show Author Affiliations
  1. Univ. of Virginia, Charlottesville, VA (United States)
  2. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Center for Integrated Nanotechnologies (CINT)
  3. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
  4. James Madison Univ., Harrisonburg, VA (United States)
Publication Date:
Research Org.:
Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States). Center for Integrated Nanotechnologies (CINT)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA); National Science Foundation (NSF); USDOE Laboratory Directed Research and Development (LDRD) Program; Semiconductor Research Corporation (SRC)
OSTI Identifier:
1670742
Alternate Identifier(s):
OSTI ID: 1638538
Report Number(s):
SAND-2020-7338J
Journal ID: ISSN 0021-8979; 687447; TRN: US2204196
Grant/Contract Number:  
AC04-94AL85000; ACI-1548562; NA0003525
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Applied Physics
Additional Journal Information:
Journal Volume: 128; Journal Issue: 3; Journal ID: ISSN 0021-8979
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Second harmonic generation; Ferroelectric materials; Optical absorption; Nonlinear optics; Density functional theory; Band gap; Crystal structure; Thin films

Citation Formats

Ihlefeld, Jon F., Luk, Ting S., Smith, Sean W., Fields, Shelby S., Jaszewski, Samantha T., Hirt, Daniel M., Riffe, Will T., Bender, Scott, Constantin, Costel, Ayyasamy, Mukil V., Balachandran, Prasanna V., Lu, Ping, Henry, Michael David, and Davids, Paul S. Compositional dependence of linear and nonlinear optical response in crystalline hafnium zirconium oxide thin films. United States: N. p., 2020. Web. doi:10.1063/5.0012175.
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Ihlefeld, Jon F., Luk, Ting S., Smith, Sean W., Fields, Shelby S., Jaszewski, Samantha T., Hirt, Daniel M., Riffe, Will T., Bender, Scott, Constantin, Costel, Ayyasamy, Mukil V., Balachandran, Prasanna V., Lu, Ping, Henry, Michael David, & Davids, Paul S. Compositional dependence of linear and nonlinear optical response in crystalline hafnium zirconium oxide thin films. United States. https://doi.org/10.1063/5.0012175
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Ihlefeld, Jon F., Luk, Ting S., Smith, Sean W., Fields, Shelby S., Jaszewski, Samantha T., Hirt, Daniel M., Riffe, Will T., Bender, Scott, Constantin, Costel, Ayyasamy, Mukil V., Balachandran, Prasanna V., Lu, Ping, Henry, Michael David, and Davids, Paul S. Wed . "Compositional dependence of linear and nonlinear optical response in crystalline hafnium zirconium oxide thin films". United States. https://doi.org/10.1063/5.0012175. https://www.osti.gov/servlets/purl/1670742.
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@article{osti_1670742,
title = {Compositional dependence of linear and nonlinear optical response in crystalline hafnium zirconium oxide thin films},
author = {Ihlefeld, Jon F. and Luk, Ting S. and Smith, Sean W. and Fields, Shelby S. and Jaszewski, Samantha T. and Hirt, Daniel M. and Riffe, Will T. and Bender, Scott and Constantin, Costel and Ayyasamy, Mukil V. and Balachandran, Prasanna V. and Lu, Ping and Henry, Michael David and Davids, Paul S.},
abstractNote = {Composition dependence of second harmonic generation, refractive index, extinction coefficient, and optical bandgap in 20 nm thick crystalline Hf1–xZrxO2 (0 ≤ x ≤ 1) thin films is reported here. The refractive index exhibits a general increase with increasing ZrO2 content with all values within the range of 1.98–2.14 from 880 nm to 400 nm wavelengths. A composition dependence of the indirect optical bandgap is observed, decreasing from 5.81 eV for HfO2 to 5.17 eV for Hf0.4Zr0.6O2. The bandgap increases for compositions with x > 0.6, reaching 5.31 eV for Hf0.1Zr0.9O2. Second harmonic signals are measured for 880 nm incident light. The magnitude of the second harmonic signal scales with the magnitude of the remanant polarization in the composition series. Film compositions that display near zero remanent polarizations exhibit minimal second harmonic generation while those with maximum remanent polarization also display the largest second harmonic signal. The results are discussed in the context of ferroelectric phase assemblage in the hafnium zirconium oxide films and demonstrate a path toward a silicon-compatible integrated nonlinear optical material.},
doi = {10.1063/5.0012175},
journal = {Journal of Applied Physics},
number = 3,
volume = 128,
place = {United States},
year = {Wed Jul 15 00:00:00 EDT 2020},
month = {Wed Jul 15 00:00:00 EDT 2020}
}
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https://doi.org/10.1063/5.0012175
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