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Revealing the Mechanism of Pressure-Induced Emission in Layered Silver-Bismuth Double Perovskites |
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| Authors: | Dr Long Zhang Shuoxue Li Huaiyang Sun Qiwen Jiang Yue Wang Dr Yuanyuan Fang Prof Ying Shi Prof?Dr Defang Duan Prof Kai Wang Prof Hong Jiang Dr Laizhi Sui Prof Guorong Wu Prof Kaijun Yuan Prof Bo Zou |
| Institution: | 1. State Key Laboratory of Superhard Materials, College of Physics, Jilin University, Changchun, 130012 China
Contribution: Conceptualization (lead), ?Investigation (lead), Writing - original draft (lead), Writing - review & editing (lead);2. College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871 China Contribution: ?Investigation (supporting);3. State Key Laboratory of Superhard Materials, College of Physics, Jilin University, Changchun, 130012 China Contribution: Software (supporting);4. State Key Laboratory of Superhard Materials, College of Physics, Jilin University, Changchun, 130012 China Contribution: ?Investigation (supporting);5. Institute of Atomic and Molecular Physics, Jilin University, Changchun, 130012 China Contribution: ?Investigation (supporting);6. State Key Laboratory of Superhard Materials, College of Physics, Jilin University, Changchun, 130012 China;7. College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871 China;8. State Key Laboratory of Molecular Reaction Dynamics and Dalian Coherent Light Source, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023 China;9. State Key Laboratory of Molecular Reaction Dynamics and Dalian Coherent Light Source, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023 China Contribution: ?Investigation (supporting) |
| Abstract: | Pressure-induced emission (PIE) associated with self-trapping excitons (STEs) in low-dimensional halide perovskites has attracted great attention for better materials-by-design. Here, using 2D layered double perovskite (C6H5CH2CH2NH3+)4AgBiBr8 as a model system, we advance a fundamental physicochemical mechanism of the PIE from the perspective of carrier dynamics and excited-state behaviors of local lattice distortion. We observed a pressure-driven STE transformation from dark to bright states, corresponding a strong broadband Stokes-shifted emission. Further theoretical analysis demonstrated that the suppressed lattice distortion and enhanced electronic dimensionality in the excited-state play an important role in the formation of stabilized bright STEs, which could manipulate the self-trapping energy and lattice deformation energy to form an energy barrier between the potential energy curves of ground- and excited-state, and enhance the electron-hole orbital overlap, respectively. |
| Keywords: | Carrier Dynamics Excited State Mechanism Perovskite Pressure-Induced Emission |