Real-time observation of the buildup of polaron in α-FAPbI<sub>3</sub>.

Yue, Xingyu; Wang, Chunwei; Zhang, Bo; Zhang, Zeyu; Xiong, Zhuang; Zu, Xinzhi; Liu, Zhengzheng; Hu, Zhiping et al. · Nat Commun · 2023

basic_science · Level V

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Abstract

The formation of polaron, i.e., the strong coupling process between the carrier and lattice, is considered to play a crucial role in benefiting the photoelectric performance of hybrid organic-inorganic halide perovskites. However, direct observation of the dynamical formation of polarons occurring at time scales within hundreds of femtoseconds remains a technical challenge. Here, by terahertz emission spectroscopy, we demonstrate the real-time observation of polaron formation process in FAPbI<sub>3</sub> films. Two different polaron resonances interpreted with the anharmonic coupling emission model have been studied: P1 at ~1 THz relates to the inorganic sublattice vibration mode and the P2 at ~0.4 THz peak relates to the FA<sup>+</sup> cation rotation mode. Moreover, P2 could be further strengthened than P1 by pumping the hot carriers to the higher sub-conduction band. Our observations could open a door for THz emission spectroscopy to be a powerful tool in studying polaron formation dynamics in perovskites.