Molecular Engineering of Organic Spacer Cations for Efficient and Stable Formamidinium Perovskite Solar Cell

Abstract Low dimensional (LD) perovskite materials generally exhibit superior chemical stability against ambient moisture and thermal stress than that of 3D perovskites. Recently, LD perovskite has been used as a passivation layer on the surface of 3D perovskite grains. Although various LD perovskites have been developed focusing on their hydrophobicity, the impact of crystal structure of LD perovskite on the photovoltaic performance of perovskite solar cell (PSC) is still uncertain. In this work, the effects of the structural characteristics of LD perovskites on the crystal formation of formamidinium lead triiodide (α‐FAPbI₃) and on the optoelectrical properties of PSCs are elucidated. The phase‐transformation kinetics of FAPbI₃ mixed with LD perovskites is studied using the Johnson–Mehl–Avrami–Kolmogorov model. It is found that the arrangement of PbI₆ octahedra in the LD perovskite changes the rate of α‐FAPbI₃ formation. Facilitated nucleation of α‐FAPbI₃ at the LD/FAPbI₃ interface results in minimal structural disorder and prolonged charge‐carrier lifetimes. As a result, the PSC with the optimized LD perovskite structure exhibits a power conversion efficiency of 21.25% from a reverse current–voltage scan, and stabilized efficiency of 19.95% with excellent ambient stability without being encapsulated.