Revealing the Mechanism of Pressure‐Induced Emission in Layered Silver‐Bismuth Double Perovskites

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 physicochemi...

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Published in:Angewandte Chemie International Edition 2023-03, Vol.62 (14), p.e202301573-n/a
Main Authors: Zhang, Long, Li, Shuoxue, Sun, Huaiyang, Jiang, Qiwen, Wang, Yue, Fang, Yuanyuan, Shi, Ying, Duan, Defang, Wang, Kai, Jiang, Hong, Sui, Laizhi, Wu, Guorong, Yuan, Kaijun, Zou, Bo
Format: Article
Language:English
Subjects:
Bismuth
Broadband
Carrier Dynamics
Distortion
Emission analysis
Emissions
Excited State
Excitons
Mechanism
Perovskite
Perovskites
Potential energy
Pressure
Pressure-Induced Emission
Theoretical analysis
Trapping
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Summary: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. A pressure‐driven self‐trapping exciton transformation from dark to bright state was achieved in low‐dimensional halide perovskites, revealing the physicochemical mechanism of pressure‐induced emission.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.202301573