Unraveling the Role of Electron‐Withdrawing Molecules for Highly Efficient and Stable Perovskite Photovoltaic

Electron-withdrawing molecules (EWMs) have exhibited remarkable efficacy in boosting the performance of perovskite solar cells (PSCs). However, the underneath mechanisms governing their positive attributes remain inadequately understood. Herein, we conducted a comprehensive study on EWMs by comparing 2,2'-(2,5-cyclohexadiene-1,4-diylidene) bismalononitrile (TCNQ) and (2,3,5,6-tetrafluoro-2,5-cyclohexadiene-1,4-diylidene) dimalononitrile (F4TCNQ) employed at the perovskite/hole transport layer (HTL) interfaces. Our findings reveal that EWMs simultaneously enhance chemical passivation, interface dipole effect, and chemically binding of the perovskite to the HTL. Notably, F4TCNQ, with its superior electron-withdrawing properties, demonstrates a more pronounced impact. Consequently, PCSs modified with F4TCNQ achieved an impressive power conversion efficiency (PCE) of 25.21 %, while demonstrating excellent long-term stability. Moreover, the PCE of a larger-area perovskite module (14.0 cm