Crystallization Control Based on the Regulation of Solvent–Perovskite Coordination for High‐Performance Ambient Printable FAPbI₃ Perovskite Solar Cells

Abstract

The critical requirement for ambient-printed formamidinium lead iodide (FAPbI₃ ) lies in the control of nucleation-growth kinetics and defect formation behavior, which are extensively influenced by interactions between the solvent and perovskite. Here, a strategy is developed that combines a cosolvent and an additive to efficiently tailor the coordination between the solvent and perovskite. Through in situ characterizations, the direct crystallization from the sol-gel phase to α-FAPbI₃ is illustrated. When the solvent exhibits strong interactions with the perovskite, the sol-gel phases cannot effectively transform into α-FAPbI₃ , resulting in a lower nucleation rate and confined crystal growth directions. Consequently, it becomes challenging to fabricate high-quality void-free perovskite films. Conversely, weaker solvent-perovskite coordination promotes direct crystallization from sol-gel phases to α-FAPbI₃ . This process exhibits more balanced nucleation-growth kinetics and restrains the formation of defects and microstrains in situ. This strategy leads to improved structural and optoelectronic properties within the FAPbI₃ films, characterized by more compact grain stacking, smoother surface morphology, released lattice strain, and fewer defects. The ambient-printed FAPbI₃ perovskite solar cells fabricated using this strategy exhibit a remarkable power conversion efficiency of 24%, with significantly reduced efficiency deviation and negligible decreases in the stabilized output.