Enhancing Performance and Stability of Perovskite Solar Cells with a Novel Formamidine Group Additive

Abstract Perovskite materials, particularly FAPbI 3 , have emerged as promising candidates for solar energy conversion applications. However, these materials are plagued by well‐known defects and suboptimal film quality. Enhancing crystallinity and minimizing defect density are therefore essential steps in the development of high‐performance perovskite solar cells. In this study, 1H‐Pyrazole‐1‐carboximidamide hydrochloride (PCH) is introduced into FAPbI 3 perovskite films. The molecular structure of PCH features a pyrazole ring bonded to formamidine (FA). The FA moiety of PCH facilitated the incorporation of this additive into the film lattice, while the negatively charged pyrazole ring effectively passivated positively charged iodine vacancies. The presence of PCH led to the fabrication of an FAPbI 3 device with improved crystallinity, a smoother surface, and reduced defect density, resulting in enhanced V oc and fill factor. A record power conversion efficiency of 24.62% is achieved, along with exceptional stability under prolonged air exposure and thermal stress. The findings highlight the efficacy of PCH as a novel additive for the development of high‐performance perovskite solar cells.