journal article·2022-07

Dangling Octahedra Enable Edge States in 2D Lead Halide Perovskites

Yan Qin, Zhi‐Gang Li, Fei‐Fei Gao, Haisheng Chen, Xiang Li, Bin Xu, Qian Li, Xingxing Jiang, Wei Li, Xiang Wu, Zewei Quan, Lei Ye, Yang Zhang, Zheshuai Lin, Laurent Pedesseau, Jacky Even, Peixiang Lu, Xian‐He Bu

Advanced Materials· Volume 34· Issue 29
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Abstract

Abstract The structural reconstruction at the crystal layer edges of 2D lead halide perovskites (LHPs) leads to unique edge states (ES), which are manifested by prolonged carrier lifetime and reduced emission energy. These special ES can effectively enhance the optoelectronic performance of devices, but their intrinsic origin and working mechanism remain elusive. Here it is demonstrated that the ES of a family of 2D Ruddlesden–Popper LHPs [BA2CsPb2Br7, BA2MAPb2Br7, and BA2MA2Pb3Br10 (BA = butylammonium; MA = methylammonium)] arise from the rotational symmetry elevation of the PbBr6 octahedra dangling at the crystal layer edges. These dangling octahedra give rise to localized electronic states that enable an effective transport of electrons from the interior to layer edges, and the population of electrons in both the interior states and the ES can be manipulated via controlling the external fields. Moreover, the abundant phonons, activated by the dangling octahedra, can interact with electrons to facilitate radiative recombination, counterintuitive to the suppressive role commonly observed in conventional semiconductors. This work unveils the intrinsic atomistic and electronic origins of ES in 2D LHPs, which can stimulate the exploration of ES‐based exotic optoelectronic properties and the corresponding design of high‐performance devices for these emergent low‐dimensional semiconductors.
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Research context

OpenAlex topics: Perovskite Materials and Applications · 2D Materials and Applications · Semiconductor Quantum Structures and Devices

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

School of Materials Science and Engineering Tianjin Key Laboratory of Metal and Molecule‐Based Material Chemistry Nankai University Tianjin 300350 China

School of Physics and Wuhan National Laboratory for Optoelectronics Huazhong University of Science and Technology Wuhan 430074 China

Institute of Modern Optics and Tianjin Key Laboratory of Micro‐Scale Optical Information Science and Technology Nankai University Tianjin 300350 China

State Key Laboratory of Geological Processes and Mineral Resources China University of Geosciences Wuhan 430074 China

Department of Chemistry Academy for Advanced Interdisciplinary Studies and Shenzhen Engineering Research Center for Frontier Materials Synthesis at High Pressures Southern University of Science and Technology (SUSTech) Shenzhen 518055 China

Technical Institute of Physics and Chemistry Chinese Academy of Sciences Beijing 100190 China

School of Optical and Electronic Information Huazhong University of Science and Technology Wuhan 430074 China

Univ Rennes INSA Rennes CNRS Institut FOTON UMR 6082 Rennes F‐35000 France

Funding

National Natural Science Foundation of China · Fundamental Research Funds for the Central Universities · Natural Science Foundation of Tianjin City · Higher Education Discipline Innovation Project · Institut Universitaire de France

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