Defect passivation and crystallization modulation in methylammonium-free wide-bandgap perovskites for all-perovskite tandem solar cells.

Jia, Xuefei; Zhang, Kaicheng; Gao, Xiaofeng; Liao, Xufeng; Yang, Yujie; Li, Weisheng; Lv, Xiaojing; Zhao, Xinyu et al. · Sci Adv · 2025

basic_science · Level V

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Abstract

Wide-bandgap (WBG; >1.65 electron volts) perovskites based on iodine-bromine (I-Br) mixed halides are critical components of perovskite-based tandem solar cells (TSCs). However, the uncontrolled crystallization dynamics of Br-rich species lead to reduced grain sizes and high defect densities in WBG perovskite films. Herein, a multifunctional additive 3,4,5-trifluorobenzamide (TFBZ) was introduced to enhance the crystallinity and passivate defects of the methylammonium (MA)-free WBG perovskite films. The TFBZ demonstrates superior passivation capability compared to benzamide, effectively mitigating both iodine vacancies and undercoordinated Pb<sup>2+</sup> defects via fluorine-enhanced interactions. In addition, the fluorine substituents in TFBZ could form N-H···F hydrogen bonds with formamidinium iodide to retard the crystallization rate of the perovskite. This proposed method is effective in defect passivation and crystal growth modulation for both 1.67- and 1.79-electron volt MA-free WBG perovskites, enabling the fabrication of MA-free all-perovskite TSCs with an encouraging power conversion efficiency of 29.01% (certified at 28.52%).