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Title: Large Enhancements in Optical and Piezoelectric Properties in Ferroelectric Zn 1‐ x Mg x O Thin Films through Engineering Electronic and Ionic Anharmonicities

Abstract

Multifunctionality as a paradigm requires materials exhibiting multiple superior properties. Integrating second-order optical nonlinearity and large bandgap with piezoelectricity can, for example, enable broadband, strain-tunable photonics. Though very different phenomena at distinct frequencies, both second-order optical nonlinearity and piezoelectricity are third-rank polar tensors present only in acentric crystal structures. However, simultaneously enhancing both phenomena is highly challenging since it involves competing effects with tradeoffs. Recently, a large switchable ferroelectric polarization of ≈80 μC cm–2 was reported in Zn1-xMgxO films. Here, ferroelectric Zn1-xMgxO is demonstrated to be a platform that hosts simultaneously a 30% increase in the electronic bandgap, a 50% enhancement in the second harmonic generation (SHG) coefficients, and a near 200% improvement in the piezoelectric coefficients over pure ZnO. These enhancements are shown to be due to a 400% increase in the electronic anharmonicity and a ≈200% decrease in the ionic anharmonicity with Mg substitution. Precisely controllable periodic ferroelectric domain gratings are demonstrated down to 800 nm domain width, enabling ultraviolet quasi-phase-matched optical harmonic generation as well as domain-engineered piezoelectric devices.

Authors:
ORCiD logo [1];  [1];  [2];  [1];  [3];  [1];  [1];  [1];  [4];  [1];  [5];  [1]; ORCiD logo [6]
  1. Department of Materials Science and Engineering The Pennsylvania State University University Park PA 16802 USA
  2. Center for Nanophase Materials Sciences Oak Ridge National Laboratory Oak Ridge TN 37831 USA
  3. Department of Engineering Science and Mechanics The Pennsylvania State University University Park PA 16802 USA
  4. Department of Materials Science and Engineering The Pennsylvania State University University Park PA 16802 USA, Department of Engineering Science and Mechanics The Pennsylvania State University University Park PA 16802 USA, Department of Mathematics The Pennsylvania State University University Park PA 16802 USA
  5. Department of Materials Science and Engineering The Pennsylvania State University University Park PA 16802 USA, Materials Research Institute The Pennsylvania State University University Park PA 16802 USA
  6. Department of Materials Science and Engineering The Pennsylvania State University University Park PA 16802 USA, Department of Engineering Science and Mechanics The Pennsylvania State University University Park PA 16802 USA, Materials Research Institute The Pennsylvania State University University Park PA 16802 USA, Department of Physics Pennsylvania State University University Park PA 16802 USA
Publication Date:
Research Org.:
Pennsylvania State Univ., University Park, PA (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1975316
Alternate Identifier(s):
OSTI ID: 1975491; OSTI ID: 1983517; OSTI ID: 2333853
Grant/Contract Number:  
SC0021118; DMR-2133373; DMR-2210933; AC05-00OR22725; DMR-2011839
Resource Type:
Published Article
Journal Name:
Advanced Physics Research
Additional Journal Information:
Journal Name: Advanced Physics Research Journal Volume: 2 Journal Issue: 12; Journal ID: ISSN 2751-1200
Publisher:
Wiley Blackwell (John Wiley & Sons)
Country of Publication:
Germany
Language:
English
Subject:
36 MATERIALS SCIENCE; bandgaps; ferroelectricity; piezoelectricity; second harmonic generation; thin films; ZnO

Citation Formats

Zu, Rui, Ryu, Gyunghyun, Kelley, Kyle P., Baksa, Steven M., Jacques, Leonard C., Wang, Bo, Ferri, Kevin, He, Jingyang, Chen, Long‐Qing, Dabo, Ismaila, Trolier‐McKinstry, Susan, Maria, Jon‐Paul, and Gopalan, Venkatraman. Large Enhancements in Optical and Piezoelectric Properties in Ferroelectric Zn 1‐ x Mg x O Thin Films through Engineering Electronic and Ionic Anharmonicities. Germany: N. p., 2023. Web. doi:10.1002/apxr.202300003.
Zu, Rui, Ryu, Gyunghyun, Kelley, Kyle P., Baksa, Steven M., Jacques, Leonard C., Wang, Bo, Ferri, Kevin, He, Jingyang, Chen, Long‐Qing, Dabo, Ismaila, Trolier‐McKinstry, Susan, Maria, Jon‐Paul, & Gopalan, Venkatraman. Large Enhancements in Optical and Piezoelectric Properties in Ferroelectric Zn 1‐ x Mg x O Thin Films through Engineering Electronic and Ionic Anharmonicities. Germany. https://doi.org/10.1002/apxr.202300003
Zu, Rui, Ryu, Gyunghyun, Kelley, Kyle P., Baksa, Steven M., Jacques, Leonard C., Wang, Bo, Ferri, Kevin, He, Jingyang, Chen, Long‐Qing, Dabo, Ismaila, Trolier‐McKinstry, Susan, Maria, Jon‐Paul, and Gopalan, Venkatraman. Wed . "Large Enhancements in Optical and Piezoelectric Properties in Ferroelectric Zn 1‐ x Mg x O Thin Films through Engineering Electronic and Ionic Anharmonicities". Germany. https://doi.org/10.1002/apxr.202300003.
@article{osti_1975316,
title = {Large Enhancements in Optical and Piezoelectric Properties in Ferroelectric Zn 1‐ x Mg x O Thin Films through Engineering Electronic and Ionic Anharmonicities},
author = {Zu, Rui and Ryu, Gyunghyun and Kelley, Kyle P. and Baksa, Steven M. and Jacques, Leonard C. and Wang, Bo and Ferri, Kevin and He, Jingyang and Chen, Long‐Qing and Dabo, Ismaila and Trolier‐McKinstry, Susan and Maria, Jon‐Paul and Gopalan, Venkatraman},
abstractNote = {Multifunctionality as a paradigm requires materials exhibiting multiple superior properties. Integrating second-order optical nonlinearity and large bandgap with piezoelectricity can, for example, enable broadband, strain-tunable photonics. Though very different phenomena at distinct frequencies, both second-order optical nonlinearity and piezoelectricity are third-rank polar tensors present only in acentric crystal structures. However, simultaneously enhancing both phenomena is highly challenging since it involves competing effects with tradeoffs. Recently, a large switchable ferroelectric polarization of ≈80 μC cm–2 was reported in Zn1-xMgxO films. Here, ferroelectric Zn1-xMgxO is demonstrated to be a platform that hosts simultaneously a 30% increase in the electronic bandgap, a 50% enhancement in the second harmonic generation (SHG) coefficients, and a near 200% improvement in the piezoelectric coefficients over pure ZnO. These enhancements are shown to be due to a 400% increase in the electronic anharmonicity and a ≈200% decrease in the ionic anharmonicity with Mg substitution. Precisely controllable periodic ferroelectric domain gratings are demonstrated down to 800 nm domain width, enabling ultraviolet quasi-phase-matched optical harmonic generation as well as domain-engineered piezoelectric devices.},
doi = {10.1002/apxr.202300003},
journal = {Advanced Physics Research},
number = 12,
volume = 2,
place = {Germany},
year = {Wed May 24 00:00:00 EDT 2023},
month = {Wed May 24 00:00:00 EDT 2023}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1002/apxr.202300003

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