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

Abstract

Abstract 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 2.5 Br 0.5 perovskite solar cells via inducing excess lead iodide (PbI 2 ) into the precursors. Comprehensive film and device characterizations are conducted to study the influences of excess PbI 2 on the crystal quality, passivation effect, charge dynamics, and photovoltaic performance. It is found that excess PbI 2 improves the crystallization process, producing high‐quality CsPbI 2.5 Br 0.5 films with enlarged grain sizes, enhanced crystal orientation, and unchanged phase composition. The residual PbI 2 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 2.5 Br 0.5 solar cells, with less than 24% degradation drop at the maximum power point under continuous illumination for 420 h.