Epitaxial CsPbBr3/CdS Janus Nanocrystal Heterostructures for Efficient Charge Separation

Author:

Qiu Hengwei1,Li Fu1,He Shan23,Shi Ran4,Han Yaoyao23,Abudukeremu Hannikezi1,Zhang Lin4,Zhang Yan5,Wang Song1,Liu Wangyu1,Ma Chao1,Fang Honghua5,Long Run4,Wu Kaifeng23,Zhang Hao1ORCID,Li Jinghong1

Affiliation:

1. Department of Chemistry Center for BioAnalytical Chemistry Key Laboratory of Bioorganic Phosphorus Chemistry & Chemical Biology of Ministry of Education Tsinghua University Beijing 100084 China

2. State Key Laboratory of Molecular Reaction Dynamics Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian 116023 China

3. University of the Chinese Academy of Sciences Beijing 100049 China

4. College of Chemistry Key Laboratory of Theoretical & Computational Photochemistry of Ministry of Education Beijing Normal University Beijing 100875 China

5. Department of Precision Instrument State Key Laboratory of Precision Measurement Technology & Instruments Tsinghua University Beijing 100084 China

Abstract

AbstractEpitaxial heterostructures of colloidal lead halide perovskite nanocrystals (NCs) with other semiconductors, especially the technologically important metal chalcogenides, can offer an unprecedented level of control in wavefunction design and exciton/charge carrier engineering. These NC heterostructures are ideal material platforms for efficient optoelectronics and other applications. Existing methods, however, can only yield heterostructures with random connections and distributions of the two components. The lack of epitaxial relation and uniform geometry hinders the structure–function correlation and impedes the electronic coupling at the heterointerface. This work reports the synthesis of uniform, epitaxially grown CsPbBr3/CdS Janus NC heterostructures with ultrafast charge separation across the electronically coupled interface. Each Janus NC contains a CdS domain that grows exclusively on a single {220} facet of CsPbBr3 NCs. Varying reaction parameters allows for precise control in the sizes of each domain and readily modulates the optical properties of Janus NCs. Transient absorption measurements and modeling results reveal a type II band alignment, where photoexcited electrons rapidly transfer (within ≈9 picoseconds) from CsPbBr3 to CdS. The promoted charge separation and extraction in epitaxial Janus NCs leads to photoconductors with drastically improved (approximately three orders of magnitude) responsivity and detectivity, which is promising for ultrasensitive photodetection.

Funder

National Natural Science Foundation of China

National Key Research and Development Program of China

China Postdoctoral Science Foundation

Natural Science Foundation of Beijing Municipality

Publisher

Wiley

Subject

General Physics and Astronomy,General Engineering,Biochemistry, Genetics and Molecular Biology (miscellaneous),General Materials Science,General Chemical Engineering,Medicine (miscellaneous)

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