Atomistic Mechanism of Broadband Emission in Metal Halide Perovskites

Broadband emission is attributed to the formation of self-trapped excitons (STEs) due to the strong electron–phonon coupling. Interestingly, it has been observed in only certain three-dimensional and low-dimensional metal halide perovskites. In this study, we show by density functional theory calculation that a low electronic dimensionality is a prerequisite for the formation of STE and, therefore, broadband emission. We further show that multiple STE structures exist in each perovskite exhibiting broadband emission. However, only the STE with Jahn–Teller-like octahedral distortion is mainly responsible for the observed broadband emission, though it may not be the lowest-energy structure. Lastly, our results provide important insights for designing perovskite materials for broadband emissions with preferred chromaticity coordinator or color temperature.