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

Abstract

AbstractThe 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.