Complex Additive‐Assisted Crystal Growth and Phase Stabilization of α‐FAPbI3 Film for Highly Efficient, Air‐Stable Perovskite Photovoltaics

Abstract

Abstract Solution‐processed formamidinium lead iodide (FAPbI3) perovskite is entropically metastable, and it exhibits condition‐induced crystal polymorphism. Under an ambient atmosphere, the photoactive black α‐FAPbI3 converts easily to photoinactive yellow δ‐FAPbI3. This α → δ phase degradation is further accelerated upon exposure to high temperature/humidity, directly threatening the performance and stability of perovskite solar cells (PSCs). Herein, cesium iodide‐lead iodide:dimethyl sulfoxide (CsI‐PbI2:DMSO) complex is introduced as a phase stabilizer to modulate the crystallization of α‐FAPbI3 perovskite from δ‐FAPbI3 precursor and simultaneously, serve as a defect passivator to suppress trap states formation. Theoretical simulations and experimental results reveal the pivotal role of complex additive in optimizing the energy band alignment and optoelectronic properties of α‐FAPbI3 perovskite and most importantly, hindering the α → δ phase transition. The best PSC device based on the additive‐engineered perovskite film achieves an efficiency of ≈21.9%, which is ≈11% higher than that of its pristine counterpart (≈19.8%). In addition, the incorporation of CsI‐PbI2:DMSO complex remarkably enhances the long‐term stability and photostability of the PSCs by inhibiting ion migrations and preserving the α‐phase in FAPbI3 perovskite. The additive engineering presented herein offers a route to produce FAPbI3‐based PSCs with improved performance, stability, and reproducibility.

Keywords

• charge transfer
• defect passivation
• optical simulation
• optoelectronic
• phase transformation