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.
Ihlefeld, Jon F., et al. "Compositional dependence of linear and nonlinear optical response in crystalline hafnium zirconium oxide thin films." Journal of Applied Physics, vol. 128, no. 3, Jul. 2020. https://doi.org/10.1063/5.0012175
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. (2020). Compositional dependence of linear and nonlinear optical response in crystalline hafnium zirconium oxide thin films. Journal of Applied Physics, 128(3). https://doi.org/10.1063/5.0012175
Ihlefeld, Jon F., Luk, Ting S., Smith, Sean W., et al., "Compositional dependence of linear and nonlinear optical response in crystalline hafnium zirconium oxide thin films," Journal of Applied Physics 128, no. 3 (2020), https://doi.org/10.1063/5.0012175
@article{osti_1670742,
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 others},
title = {Compositional dependence of linear and nonlinear optical response in crystalline hafnium zirconium oxide thin films},
annote = {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},
url = {https://www.osti.gov/biblio/1670742},
journal = {Journal of Applied Physics},
issn = {ISSN 0021-8979},
number = {3},
volume = {128},
place = {United States},
publisher = {American Institute of Physics (AIP)},
year = {2020},
month = {07}}
Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States). Center for Integrated Nanotechnologies (CINT)
Sponsoring Organization:
USDOE National Nuclear Security Administration (NNSA); National Science Foundation (NSF); USDOE Laboratory Directed Research and Development (LDRD) Program; Semiconductor Research Corporation (SRC)
Grant/Contract Number:
AC04-94AL85000; NA0003525
OSTI ID:
1670742
Alternate ID(s):
OSTI ID: 1638538
Report Number(s):
SAND--2020-7338J; 687447
Journal Information:
Journal of Applied Physics, Journal Name: Journal of Applied Physics Journal Issue: 3 Vol. 128; ISSN 0021-8979