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

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

doi:10.1002/apxr.202300003

Title: Large Enhancements in Optical and Piezoelectric Properties in Ferroelectric Zn _1‐ _x Mg _x O Thin Films through Engineering Electronic and Ionic Anharmonicities

Journal Article · Wed May 24 00:00:00 EDT 2023 · Advanced Physics Research

DOI:https://doi.org/10.1002/apxr.202300003· OSTI ID:1975316

^[1]; Ryu, Gyunghyun ^[1]; Kelley, Kyle P. ^[2]; Baksa, Steven M. ^[1]; Jacques, Leonard C. ^[3]; Wang, Bo ^[1]; Ferri, Kevin ^[1]; He, Jingyang ^[1]; Chen, Long‐Qing ^[4]; Dabo, Ismaila ^[1]; Trolier‐McKinstry, Susan ^[5]; Maria, Jon‐Paul ^[1];

^[6]

Department of Materials Science and Engineering The Pennsylvania State University University Park PA 16802 USA
Center for Nanophase Materials Sciences Oak Ridge National Laboratory Oak Ridge TN 37831 USA
Department of Engineering Science and Mechanics The Pennsylvania State University University Park PA 16802 USA
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
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
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

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 Zn_1-xMg_xO films. Here, ferroelectric Zn_1-xMg_xO 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.

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Research Organization:: Pennsylvania State Univ., University Park, PA (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: SC0021118; DMR-2133373; DMR-2210933; AC05-00OR22725; DMR-2011839

OSTI ID:: 1975316

Alternate ID(s):: OSTI ID: 1975491; OSTI ID: 1983517; OSTI ID: 2333853

Journal Information:: Advanced Physics Research, Journal Name: Advanced Physics Research Vol. 2 Journal Issue: 12; ISSN 2751-1200

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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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

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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