High‐Purity Inorganic Perovskite Films for Solar Cells with 9.72 % Efficiency

All-inorganic perovskite solar cells with high efficiency and improved stability are promising for commercialization. A multistep solution-processing method was developed to fabricate high-purity inorganic CsPbBr₃ perovskite films for use in efficient solar cells. By tuning the number of deposition cycles (n) of a CsBr solution, the phase conversion from CsPb₂ Br₅ (n ≤3), to CsPbBr₃ (n=4), and Cs₄ PbBr₆ (n≥5) was optimized to achieve vertical- and monolayer-aligned grains. Upon interfacial modification with graphene quantum dots, the all-inorganic perovskite solar cell (without a hole-transporting layer) achieved a power conversion efficiency (PCE) as high as 9.72 % under standard solar illumination conditions. Under challenging conditions, such as 90 % relative humidity (RH) at 25 °C or 80 °C at zero humidity, the optimized device retained 87 % PCE over 130 days or 95 % over 40 days, compared to the initial efficiency.