CsAc-Mediated Dynamic Reconstruction of Chloride Perovskite Films for High-Performance Self-Powered Near-UV Photodetectors

作者：Ronghuan Liu, Zhaojin Wang, Ziwei Zheng, Xiaobing Tang, Renjun Guo, Xuanyu Zhang, Peter Müller‐Buschbaum, Hai Zhou, Kai Wang, Xiao Wei Sun · 发表于：The Journal of Physical Chemistry Letters · 年份：2025 · DOI：10.1021/acs.jpclett.5c02192 · 被引用次数：3 · 研究领域：Perovskite Materials and Applications、Solid-state spectroscopy and crystallography、Ga2O3 and related materials

Methylammonium lead chloride perovskite (MAPbCl 3 ), with its wide bandgap of ∼3 eV, exhibits unique advantages for near-UV to UV optoelectronic devices. However, the fast crystallization kinetics and significant solubility differences of MAPbCl 3 precursors in solvents cause discontinuous films with high surface defect densities, severely limiting device performance. This study introduces a solution mediated dissolution recrystallization strategy to address the aforementioned issues, namely, employing a CsAc/methanol solution to dynamically reconstruct preformed MAPbCl 3 films. During this process, Cs + doping regulates the crystallization kinetics and suppresses the formation of pinholes caused by nonequilibrium crystallization, and Ac – anions passivate grain boundaries and surface defects through coordination. This synergistic approach yields dense, high-quality Cs 0 . 35 MA 0 . 65 PbCl 3 polycrystalline films. The resulting self-powered photodetector demonstrates exceptional performance under 405 nm laser excitation: an on/off ratio of 1.38 × 10 6, responsivity of 0.278 A/W, detectivity of 3.49 × 10 12 Jones, and a response time of 16 μs. These metrics significantly surpass those of previously reported solution-processed counterparts. This work offers a new pathway for fabricating high-quality chloride-based perovskite films and facilitates their application in optoelectronic devices such as transparent solar cells and radiation detectors.