Compositionally-graded ferroelectric thin films by solution epitaxy produce excellent dielectric stability

Ruian Zhang; Chen Lin; Hongliang Dong; Haojie Han; Yu Song; Yiran Sun; Yue Wang; Zijun Zhang; Xiaohe Miao; Yongjun Wu; Zhe Ren; Qiaoshi Zeng; Houbing Huang; Jing Ma; He Tian; Zhaohui Ren; Gaorong Han

doi:10.1038/s41467-024-55411-7

Compositionally-graded ferroelectric thin films by solution epitaxy produce excellent dielectric stability

Nat Commun. 2025 Jan 2;16(1):98. doi: 10.1038/s41467-024-55411-7.

Authors

Ruian Zhang^#¹, Chen Lin^#^{1

2}, Hongliang Dong^#³, Haojie Han⁴, Yu Song^{5

6}, Yiran Sun¹, Yue Wang⁴, Zijun Zhang⁷, Xiaohe Miao⁸, Yongjun Wu¹, Zhe Ren⁹, Qiaoshi Zeng^{10

11}, Houbing Huang^{5

6}, Jing Ma⁴, He Tian^{12

13}, Zhaohui Ren^{14

15}, Gaorong Han¹⁶

Affiliations

¹ State Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027, China.
² Key Laboratory of Intelligent Sensing Materials and Chip Integration Technology of Zhejiang Province, Hangzhou Innovation Institute of Beihang University, Hangzhou, 310051, China.
³ Center for High Pressure Science and Technology Advanced Research, Shanghai, 201203, China.
⁴ State Key Lab of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing, 100084, China.
⁵ School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081, China.
⁶ Advanced Research Institute of Multidisciplinary Science, Beijing Institute of Technology, Beijing, 100081, China.
⁷ Center of Electron Microscopy, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027, China.
⁸ Instrumentation and Service Center for Physical Sciences, Westlake University, Hangzhou, 310024, China.
⁹ Multi-discipline Research Center, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, 100049, China.
¹⁰ Center for High Pressure Science and Technology Advanced Research, Shanghai, 201203, China. [email protected].
¹¹ Shanghai Key Laboratory of Material Frontiers Research in Extreme Environments (MFree), Institute for Shanghai Advanced Research in Physical Sciences (SHARPS), Shanghai, 201203, China. [email protected].
¹² State Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027, China. [email protected].
¹³ Center of Electron Microscopy, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027, China. [email protected].
¹⁴ State Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027, China. [email protected].
¹⁵ Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering, Taiyuan, 030024, China. [email protected].
¹⁶ State Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027, China. [email protected].

^# Contributed equally.

Abstract

The composition in ferroelectric oxide films is decisive for optimizing properties and device performances. Controlling a composition distribution in these films by a facile approach is thus highly desired. In this work, we report a solution epitaxy of PbZr_xTi_1-xO₃ films with a continuous gradient of Zr concentration, realized by a competitive growth at ~220 °C. These intriguing films demonstrate a frequency-independent of dielectric permittivity below 100 kHz from room-temperature to 280 °C. In particular, the permittivity of the films can be largely regulated from 100 to 50 by slightly varying Zr compositional gradient. These results were revealed to arise from a built-in electric field within the films due to a coupling between the composition gradient and unidirectional spontaneous polarization. Our findings may pave a way to prepare compositionally-graded ferroelectric films by a solution approach, which is promising for practical dielectric, pyroelectric and photoelectric technical applications.

Abstract

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