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

Angew Chem Int Ed Engl. 2023 Mar 27;62(14):e202301573. doi: 10.1002/anie.202301573. Epub 2023 Feb 24.

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 (C6 H5 CH2 CH2 NH3 + )4 AgBiBr8 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.