Hierarchically Manipulated Charge Recombination for Mitigating Energy Loss in CsPbI2Br Solar Cells

All-inorganic perovskite cesium lead iodide/bromide (CsPbI2Br) is considered as a robust absorber for perovskite solar cells (PSCs) because of its excellent thermal stability that guarantees its long-term operation stability. Efficient CsPbI2Br PSCs are available when obtaining low energy loss, which needs efficient charge generation, less charge recombination, and balanced charge extraction. However, numerous traps in perovskites hinder the photon-electron conversion process. Herein, hierarchical manipulation of charge recombination is proposed for CsPbI2Br PSCs featuring low energy loss. Nonselective trap reduction and selective halogen vacancy passivation are performed using 2,2'-(ethylenedioxy)diethylamine and phenylbutylammonium iodide for the bottom and top contacts, respectively. Because of all-around suppressed charge recombination, balanced charge extraction and suppressed hysteresis are realized. The champion PSC achieves an open-circuit voltage of 1.30 eV, a fill factor of 80.2%, and a power conversion efficiency of 16.6% that is 28.6% higher than that of the reference device. Moreover, the thermostability of PSCs is simultaneously enhanced because of the limited defect-assisted degradation.