Collaborative Passivation for Dual Charge Transporting Layers Based on 4‐(chloromethyl)benzonitrile Additive toward Efficient and Stable Inverted Perovskite Solar Cells

Poor carrier transport capacity and numerous surface defects of charge transporting layers (CTLs), coupled with misalignment of energy levels between perovskites and CTLs, impact photoelectric conversion efficiency (PCE) of inverted perovskite solar cells (PSCs) profoundly. Herein, a collaborative passivation strategy is proposed based on 4‐(chloromethyl) benzonitrile (CBN) as a solution additive for fabrication of both [6,6]‐phenyl‐C61‐butyric acid methylester (PCBM) and poly(triarylamine) (PTAA) CTLs. This additive can improve wettability of PTAA and reduce the agglomeration of PCBM particles, which enhance the PCE and device stability of the PSCs. As a result, a PCE exceeding 20% with a remarkable short circuit current of 23.9 mA cm−2, and an improved fill factor of 81% is obtained for the CBN‐ modified inverted PSCs. Devices maintain 80% and 70% of the initial PCE after storage under 30% and 85% humidity ambient conditions for 1000 h without encapsulation, as well as negligible light state PCE loss. This strategy demonstrates feasibility of the additive engineering to improve interfacial contact between the CTLs and perovskites for fabrication of efficient and stable inverted PSCs. A comprehensive passivation strategy based on 4‐(chloromethyl) benzonitrile is proposed for defect treatments of both hole and electron transport layers. This additive can improve wettability of poly(triarylamine) and reduce agglomeration of [6,6]‐phenyl‐C61‐butyric acid methylester particles. It also demonstrates improvement of interfacial contact between the charge transport layers and perovskites for fabrication of efficient and stable inverted perovskite solar cells.