Solution epitaxy of polarization-gradient ferroelectric oxide films with colossal photovoltaic current

Chen Lin, Zijun Zhang, Zhenbang Dai, Mengjiao Wu, Shi Liu, Jialu Chen, Chenqiang Hua, Yunhao Lu, Fei Zhang, Hongbo Lou, Hongliang Dong, Qiaoshi Zeng, Jing Ma, Xiaodong Pi, Dikui Zhou, Yongjun Wu, He Tian (), Andrew M. Rappe, Zhaohui Ren () and Gaorong Han ()
Additional contact information
Chen Lin: Zhejiang University
Zijun Zhang: Zhejiang University
Zhenbang Dai: University of Pennsylvania
Mengjiao Wu: Zhejiang University
Shi Liu: Westlake University
Jialu Chen: Zhejiang University
Chenqiang Hua: Zhejiang University
Yunhao Lu: Zhejiang University
Fei Zhang: Center for High Pressure Science and Technology Advanced Research
Hongbo Lou: Center for High Pressure Science and Technology Advanced Research
Hongliang Dong: Center for High Pressure Science and Technology Advanced Research
Qiaoshi Zeng: Center for High Pressure Science and Technology Advanced Research
Jing Ma: Tsinghua University
Xiaodong Pi: Zhejiang University
Dikui Zhou: Zhejiang University
Yongjun Wu: Zhejiang University
He Tian: Zhejiang University
Andrew M. Rappe: University of Pennsylvania
Zhaohui Ren: Zhejiang University
Gaorong Han: Zhejiang University

Nature Communications, 2023, vol. 14, issue 1, 1-9

Abstract: Abstract Solution growth of single-crystal ferroelectric oxide films has long been pursued for the low-cost development of high-performance electronic and optoelectronic devices. However, the established principles of vapor-phase epitaxy cannot be directly applied to solution epitaxy, as the interactions between the substrates and the grown materials in solution are quite different. Here, we report the successful epitaxy of single-domain ferroelectric oxide films on Nb-doped SrTiO3 single-crystal substrates by solution reaction at a low temperature of ~200 oC. The epitaxy is mainly driven by an electronic polarization screening effect at the interface between the substrates and the as-grown ferroelectric oxide films, which is realized by the electrons from the doped substrates. Atomic-level characterization reveals a nontrivial polarization gradient throughout the films in a long range up to ~500 nm because of a possible structural transition from the monoclinic phase to the tetragonal phase. This polarization gradient generates an extremely high photovoltaic short-circuit current density of ~2.153 mA/cm2 and open-circuit voltage of ~1.15 V under 375 nm light illumination with power intensity of 500 mW/cm2, corresponding to the highest photoresponsivity of ~4.306×10−3 A/W among all known ferroelectrics. Our results establish a general low-temperature solution route to produce single-crystal gradient films of ferroelectric oxides and thus open the avenue for their broad applications in self-powered photo-detectors, photovoltaic and optoelectronic devices.

Date: 2023
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DOI: 10.1038/s41467-023-37823-z

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