This study investigates the potential of inorganic perovskite CsPbBr3 as a photovoltaic material, highlighting its superior stability compared to that of organic–inorganic hybrid perovskite materials. Conventional methods for preparing CsPbBr3 perovskite films, such as the two-step method and the dual-source thermal evaporation method, face challenges in obtaining high-purity films due to the decomposition of precursor films and the formation of multiple heterogeneous phases. To address this issue, we synthesized CsPbBr3 powder material using thermal evaporation deposition, which effectively suppressed decomposition and the formation of heterogeneous phases. Consequently, we achieved uniform and dense CsPbBr3 perovskite films. By incorporating energy-band engineering modification with CsPbBr3 quantum dots (QDs), the all-inorganic perovskite solar cells (PSCs) attained a power conversion efficiency (PCE) of 7.01% under standard solar illumination conditions. The device PCE remained at 93% of its initial efficiency under 30% relative humidity conditions for over 100 days, showcasing its durability. The developed method produced an average grain size of 800 nm, resulting in a smooth and uniform film surface, thereby demonstrating the method’s high repeatability. Additionally, the optimized PSCs exhibited a high open-circuit voltage (VOC) with the champion device reaching a VOC of 1.38 V and a PCE of 7.01%. This research presents a robust, efficient, and cost-effective approach for fabricating high-quality all-inorganic PSCs.
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