journal article·2024-10-11

Layer Distortion Engineering for Spontaneous Charge Separation in Two-Dimensional Perovskites

Chunyi Zhao, Jingwen Bao, Yan Gao, Xianchang Yan, Fengke Sun, Hui Cheng, Longwen Chen, Haifeng Lv, Guanxin Yao, Xianyi Zhang, Wenming Tian, Shengye Jin, Xiaojun Wu, Qi Sun, Zhou Lu

ACS Energy Letters· Volume 9· Issue 10
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Abstract

Charge separation in highly confined type-I two-dimensional (2D) perovskites with a single inorganic layer ( n = 1) remains challenging due to their excessive exciton binding energy. Herein, we engineer the layer distortion within Ruddlesden–Popper (RP) type perovskites ( n = 1) by tailoring the sizes of the cycloalkylamine ligands. The perovskite layers are more distorted and corrugated to accommodate the highly compact yet rigid cyclopropylammonium and cyclobutylammonium, facilitating the formation of Pb–Pb and I–I ionic dimers as self-localizing sites for charge carriers. Consequently, spontaneous electron–hole separation as well as a long-lived (>1 μs) intrinsic quantum confined Stark effect (QCSE) is achieved using the thresholdless optical pump and without applying any external electric field, yielding an unprecedent amount of the photoinduced bandgap energy lowering. This work opens up new possibilities of efficient charge separation in type-I 2D quantum wells for the photovoltaic and nonlinear optical modulation applications.
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Research context

OpenAlex topics: Perovskite Materials and Applications · Chalcogenide Semiconductor Thin Films · Quantum Dots Synthesis And Properties

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

Affiliations

Anhui Province Key Laboratory for Control and Applications of Optoelectronic Information Materials, School of Physics and Electronic Information, the Key Laboratory of Functional Molecular Solids, Ministry of Education, and Anhui Engineering Research Center of Carbon Neutrality, Anhui Normal University, Wuhu 241002, China

State Key Laboratory of Molecular Reaction Dynamics and the Dynamic Research Center for Energy and Environmental Materials, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China

Key Laboratory of Materials Modification by Laser, Ion and Electron Beams (Ministry of Education), School of Physics, School of Microelectronics, Dalian University of Technology, Dalian 116024, China

School of Chemistry and Material Sciences, Key Laboratory of Precision and Intelligent Chemistry, CAS Key Laboratory of Materials for Energy Conversion, and Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), University of Science and Technology of China, Hefei, Anhui 230026, China

Funding

Dalian Institute of Chemical Physics, Chinese Academy of Sciences · University Natural Science Research Project of Anhui Province · Natural Science Foundation of Liaoning Province · National Science Fund for Distinguished Young Scholars · State Key Laboratory of Molecular Reaction Dynamics · Fundamental Research Funds for the Central Universities · National Natural Science Foundation of China · Natural Science Foundation of Anhui Province · Chinese Academy of Sciences · University Annual Scientific Research Plan of Anhui Province · University Synergy Innovation Program of Anhui Province

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