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

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 interac...

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Main Authors: 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, Gaorong Han
Format: Article
Language:English
Published: Nature Portfolio 2023-04-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-023-37823-z
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author 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
Gaorong Han
author_facet 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
Gaorong Han
author_sort Chen Lin
collection DOAJ
description 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.
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spelling doaj.art-c4d6058302914c7c998c8aca9a53a42b2023-04-30T11:21:53ZengNature PortfolioNature Communications2041-17232023-04-011411910.1038/s41467-023-37823-zSolution epitaxy of polarization-gradient ferroelectric oxide films with colossal photovoltaic currentChen Lin0Zijun Zhang1Zhenbang Dai2Mengjiao Wu3Shi Liu4Jialu Chen5Chenqiang Hua6Yunhao Lu7Fei Zhang8Hongbo Lou9Hongliang Dong10Qiaoshi Zeng11Jing Ma12Xiaodong Pi13Dikui Zhou14Yongjun Wu15He Tian16Andrew M. Rappe17Zhaohui Ren18Gaorong Han19State Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang UniversityCenter of Electron Microscope, School of Materials Science and Engineering, Zhejiang UniversityDepartment of Chemistry, University of PennsylvaniaState Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang UniversityKey Laboratory for Quantum Materials of Zhejiang Province, Department of Physics, School of Science, Westlake UniversityState Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang UniversityZhejiang Province Key Laboratory of Quantum Technology and Device, Department of physics, Zhejiang UniversityState Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang UniversityCenter for High Pressure Science and Technology Advanced ResearchCenter for High Pressure Science and Technology Advanced ResearchCenter for High Pressure Science and Technology Advanced ResearchCenter for High Pressure Science and Technology Advanced ResearchState Key Lab of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua UniversityState Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang UniversityState Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang UniversityState Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang UniversityCenter of Electron Microscope, School of Materials Science and Engineering, Zhejiang UniversityDepartment of Chemistry, University of PennsylvaniaState Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang UniversityState Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang UniversityAbstract 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.https://doi.org/10.1038/s41467-023-37823-z
spellingShingle 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
Gaorong Han
Solution epitaxy of polarization-gradient ferroelectric oxide films with colossal photovoltaic current
Nature Communications
title Solution epitaxy of polarization-gradient ferroelectric oxide films with colossal photovoltaic current
title_full Solution epitaxy of polarization-gradient ferroelectric oxide films with colossal photovoltaic current
title_fullStr Solution epitaxy of polarization-gradient ferroelectric oxide films with colossal photovoltaic current
title_full_unstemmed Solution epitaxy of polarization-gradient ferroelectric oxide films with colossal photovoltaic current
title_short Solution epitaxy of polarization-gradient ferroelectric oxide films with colossal photovoltaic current
title_sort solution epitaxy of polarization gradient ferroelectric oxide films with colossal photovoltaic current
url https://doi.org/10.1038/s41467-023-37823-z
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