Layer Distortion Engineering for Spontaneous Charge Separation in Two-Dimensional Perovskites
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.
Authors
- Guanxin Yao (ORCID: https://orcid.org/0000-0003-2800-5041)
- Xiaojun Wu (ORCID: https://orcid.org/0000-0003-3606-1211)
- Jingwen Bao
- Qi Sun (ORCID: https://orcid.org/0000-0002-7092-0705)
- Xianchang Yan
- Shengye Jin (ORCID: https://orcid.org/0000-0003-2001-2212)
- Longwen Chen (ORCID: https://orcid.org/0000-0002-6837-4936)
- Wenming Tian (ORCID: https://orcid.org/0000-0003-0235-6652)
- Fengke Sun
- Chunyi Zhao
- Zhou Lu (ORCID: https://orcid.org/0000-0001-8527-0381)
- Haifeng Lv (ORCID: https://orcid.org/0000-0001-9491-6367)
- Xianyi Zhang (ORCID: https://orcid.org/0000-0003-4850-0672)
- Hui Cheng (ORCID: https://orcid.org/0009-0003-9566-9072)
- Yan Gao (ORCID: https://orcid.org/0000-0003-0192-8786)
Institutions
- University of Science and Technology of China (CN)
- Dalian Institute of Chemical Physics (CN)
- Chinese Academy of Sciences (CN)
- Dalian University of Technology (CN)
- Collaborative Innovation Center of Chemistry for Energy Materials (CN)
- Anhui Normal University (CN)
Publication Details
- Journal
- ACS Energy Letters
- Published
- 2024-09-20
- DOI
- https://doi.org/10.1021/acsenergylett.4c02099
- Citations
- 6
- Primary Topic
- Perovskite Materials and Applications
- Type
- article
- Field-Weighted Citation Impact
- 1.25
Funders
- National Natural Science Foundation of China
- Chinese Academy of Sciences
- Natural Science Foundation of Liaoning Province
- State Key Laboratory of Molecular Reaction Dynamics
- Dalian Institute of Chemical Physics
- Natural Science Foundation of Anhui Province
- University Natural Science Research Project of Anhui Province
- Fundamental Research Funds for the Central Universities
- National Science Fund for Distinguished Young Scholars