The quality of perovskite films plays a crucial role in improving the optoelectronic properties and performance of perovskite solar cells (PSCs). Herein, high‐quality CsxFA1−xPbI3 perovskite films with different compositions (x = 0, 5, 10, and 15) are achieved by controlling the amount of cesium chloride (CsCl) in the respective FAPbI3 precursor solution. The effects of CsCl addition on the morphological and optoelectronic properties of the resulting perovskite films and on the performance of the corresponding devices are systematically studied. Introduction of CsCl into FAPbI3 shows a great potential to stabilize the α‐FAPbI3 perovskite phase by forming CsxFA1−xPbI3 films with improved morphology and carrier lifetimes. With an optimal 10 mol% CsCl additive, the average power conversion efficiency (PCE) is increased from 16.83 ± 0.30% for the reference FAPbI3‐based PSCs to 18.87 ± 0.25% (with a steady‐state PCE of 18.89%). Moreover, the optimized device performance is more stable after 20 days than the controlled one under ≈40% humidity in air.

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Perovskite solar cells (PSCs) have experienced outstanding advances in power conversion efficiencies (PCEs) by employing new electron transport layers (ETLs), interface engineering, optimizing perovskite morphology, and improving charge collection efficiency. In this work, we study the role of a new ultrathin interface layer of titanium nitride (TiN) conformally deposited on a mesoporous TiO2 (mp-TiO2) scaffold using the atomic layer deposition method. Our characterization results revealed that the presence of TiN at the ETL/perovskite interface improves the charge collection as well as reduces the interface recombination. We find that the morphology (grain size) and optical properties of the perovskite film deposited on the optimized mp-TiO2/TiN ETL are improved drastically, leading to devices with a maximum PCE of 19.38% and a high open-circuit voltage (V oc) of 1.148 V with negligible hysteresis and improved environmental (∼40% RH) and thermal (80 °C) stabilities.

Interface engineering has emerged as a great strategy for the fabrication of high efficiency and stable perovskite solar cells (PSCs).