Yutong Zhang, Yuanyuan Guo, Minjun Feng, Shuyi Lin, Cheng Yang, Deyu Li, Yuexing Xia, Yiyang Gong, Xiaotian Bao, Yangguang Zhong, Zhiyong Zhang, Yubo Tian, Wenna Du, Shuai Yue, Bo Wu, Jun Xing, Jun Yin, Jianhui Fu, Xinfeng Liu
Efficient tuning of structural distortion is an attractive approach for regulating self-trapped excitons emission properties of two-dimensional halide perovskites. Nevertheless, it remains elusive as to how the structural distortion is related with such emission. Here, we elucidate the relationship between structural distortion and the emission behavior of self-trapped excitons in two-dimensional lead bromide perovskites (R-NH3)2PbBr4 (where R is the cyclic carbon group). We reveal that rather than the octahedral tilting distortion, the lone pair activity-induced Jahn-Teller distortion plays a significant role in self-trapped excitons emission. Consequently, with growing ring size of cyclic organic cation, the increased Jahn-Teller distortion results in a larger relative self-trapped excitons emission due to the enhanced short-range Holstein electron-phonon coupling strength. Our work clarifies the controversy of the structural distortion correlation on self-trapped excitons emission and provides valuable insights for structural engineering in white-light emitting applications of two-dimensional perovskites. Leveraging electron-phonon coupling allows for modulating self-trapped exciton formation for broadband white-light emission. Using transient spectroscopy and DFT calculations, Zhang et al. correlate the structural distortion with self-trapped exciton formation in 2D halide perovskites.