Composition Engineering of All‐Inorganic Perovskite Film for Efficient and Operationally Stable Solar Cells

Cesium-based inorganic perovskites have recently attracted great research focus due to their excellent optoelectronic properties and thermal stability. However, the operational instability of all-inorganic perovskites is still a main hindrance for the commercialization. Herein, a facile approach is reported to simultaneously enhance both the efficiency and long-term stability for all-inorganic CsPbI_2.5Br_0.5 perovskite solar cells via inducing excess lead iodide (PbI₂) into the precursors. Comprehensive film and device characterizations are conducted to study the influences of excess PbI₂ on the crystal quality, passivation effect, charge dynamics, and photovoltaic performance. It is found that excess PbI₂ improves the crystallization process, producing high-quality CsPbI_2.5Br_0.5 films with enlarged grain sizes, enhanced crystal orientation, and unchanged phase composition. The residual PbI₂ at the grain boundaries also provides a passivation effect, which improves the optoelectronic properties and charge collection property in optimized devices, leading to a power conversion efficiency up to 17.1% with a high open-circuit voltage of 1.25 V. More importantly, a remarkable long-term operational stability is also achieved for the optimized CsPbI_2.5Br_0.5 solar cells, with less than 24% degradation drop at the maximum power point under continuous illumination for 420 h.