Atomically Resolved Electrically Active Intragrain Interfaces in Perovskite Semiconductors
2022
Cai, Songhua | Dai, Jun | Shao, Zhipeng | Rothmann, Mathias Uller | Jia, Yinglu | Gao, Caiyun | Hao, Mingwei | Pang, Shuping | Wang, Peng | Lau, Shu Ping | Zhu, Kai | Berry, Joseph J. | Herz, Laura M. | Zeng, Xiao Cheng | Zhou, Yuanyuan
Deciphering the atomic and electronic structures of interfaces is key to developing state-of-the-art perovskite semiconductors. However, conventional characterization techniques have limited previous studies mainly to grain-boundary interfaces, whereas the intragrain-interface microstructures and their electronic properties have been much less revealed. Herein using scanning transmission electron microscopy, we resolved the atomic-scale structural information on three prototypical intragrain interfaces, unraveling intriguing features clearly different from those from previous observations based on standalone films or nanomaterial samples. These intragrain interfaces include composition boundaries formed by heterogeneous ion distribution, stacking faults resulted from wrongly stacked crystal planes, and symmetrical twinning boundaries. The atomic-scale imaging of these intragrain interfaces enables us to build unequivocal models for the ab initio calculation of electronic properties. Our results suggest that these structure interfaces are generally electronically benign, whereas their dynamic interaction with point defects can still evoke detrimental effects. This work paves the way toward a more complete fundamental understanding of the microscopic structure–property–performance relationship in metal halide perovskites.
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