Volume 21, Issue 9 2410260
Research Article

Phase Coexistence Induced Giant Dielectric Tunability and Electromechanical Response in PbZrO3 Epitaxial Thin Films

Wanli Zhang

Wanli Zhang

State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing, 100084 China

Key Laboratory of Micro Nano Optoelectronic Devices and Intelligent Perception Systems, Yangtze Normal University, Chongqing, 408100 China

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Xinpeng Mou

Xinpeng Mou

Key Laboratory of Key Film Materials & Application for Equipment (Hunan Province), School of Materials Science and Engineering, Xiangtan University, Xiangtan, Hunan, 411105 China

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Yunpeng Ma

Yunpeng Ma

State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing, 100084 China

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Yi Zheng

Yi Zheng

State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing, 100084 China

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Sixu Wang

Sixu Wang

State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing, 100084 China

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Liang Shu

Liang Shu

State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing, 100084 China

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Ziwan Du

Ziwan Du

State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing, 100084 China

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Chenguang Deng

Chenguang Deng

State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing, 100084 China

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Qiong Yang

Corresponding Author

Qiong Yang

Key Laboratory of Key Film Materials & Application for Equipment (Hunan Province), School of Materials Science and Engineering, Xiangtan University, Xiangtan, Hunan, 411105 China

E-mail: [email protected]; [email protected]; [email protected]; [email protected]

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Rong Yu

Corresponding Author

Rong Yu

State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing, 100084 China

E-mail: [email protected]; [email protected]; [email protected]; [email protected]

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Jing-Feng Li

Corresponding Author

Jing-Feng Li

State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing, 100084 China

E-mail: [email protected]; [email protected]; [email protected]; [email protected]

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Qian Li

Corresponding Author

Qian Li

State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing, 100084 China

E-mail: [email protected]; [email protected]; [email protected]; [email protected]

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First published: 17 January 2025

Abstract

PbZrO3 (PZO) thin films, as a classic antiferroelectric material, have attracted tremendous attention for their excellent dielectric, electromechanical, and thermal switching performances. However, several fundamental questions remain unresolved, particularly the existence of an intermediate phase during the transition from the antiferroelectric (AFE) to ferroelectric (FE) state. Here, a phase coexistence configuration of an orthorhombic AFE phase and a tetragonal-like (T-like) phase is reported in epitaxial antiferroelectric PZO thin films, with thickness ranging from 16 to 110 nm. This configuration is evidenced both macroscopically by distinct shoulder-cape-shaped dielectric behavior and microscopically through scanning transmission electron microscopy (STEM) analysis. Remarkably, a 49 nm PZO film achieves an ultrahigh dielectric tunability of 90.1%, while a 59 nm film exhibits significant electromechanical strain of 0.66%. Microscopically, HAADF-STEM reveals the presence of the intermediate phase with a dipole arrangement of vertically diagonal up-up-down-down pattern, and first-principles calculations further confirm the role of this intermediate phase during AFE-to-FE phase transition, which is responsible for the unusual dielectric peaks of ɛr-E curves. These findings not only enhance the understanding of phase transition in antiferroelectric materials but also exhibit great potential for high-performance tunable and nano-electromechanical device applications.

Conflict of Interest

The authors declare no conflict of interest.

Data Availability Statement

The data that support the findings of this study are available from the corresponding author upon reasonable request.

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