Two-Pronged Maneuver of Inner Regulation and Surface Repair for Stable Inorganic Perovskite Solar Cells with Ultralow Open-Circuit Voltage Deficit

Despite inorganic perovskites are suitable for application into tandem solar cells, the unsatisfactory crystal quality and inevitable surface defects of low-temperature fabricated inorganic perovskites lead to undesirable open-circuit voltage (VOC) deficit, which limits the further development of inorganic perovskite solar cells (IPSCs). Herein, dimethylammonium chloride (DMACl) was introduced into perovskite precursor to prolong the solid-state reactions between intermediate phases of DMAPbX3 and Cs4PbX6, and mediate crystallization process of inorganic perovskite, leading to obtain high-quality CsPbI2.75Br0.25 perovskite films without DMA+ residue in perovskite films after annealing. Additionally, the energy level position of perovskite slightly downshift after adding DMACl, narrowing the band offsets between perovskite and carrier transport layers. To further reduce VOC deficit and improve the performance of IPSCs, cesium iodide (CsI) thin layer is evaporated onto the perovskite surface to repair inevitable I-related defects. Ultimately, the VOC and performance of IPSCs are improved without introducing organic components into final perovskite films. A champion photoelectric conversion efficiency of 20.75% is achieved, and the VOC deficit is significantly decreased to 0.382 V, which is the minimum VOC deficit of IPSCs at present. Additionally, the stability of the perovskite films and IPSCs has also been remarkably enhanced. This work provides an effective two-pronged maneuver for CsPbI2.75Br0.25 perovskite films' inner regulation and surface defects repair simultaneously to improve performance of inorganic perovskite solar cells (IPSCs) without introducing organic materials into final perovskite films. Eventually, the efficiency of CsPbI2.75Br0.25 IPSCs is enhanced to 20.75%, the VOC deficit isreduced to 0.382 V, which is the minimum VOC deficit of IPSCs.image (c) 2024 WILEY-VCH GmbH