14.1% CsPbI3 Perovskite Quantum Dot Solar Cells via Cesium Cation Passivation

Abstract Surface manipulation of quantum dots (QDs) has been extensively reported to be crucial to their performance when applied into optoelectronic devices, especially for photovoltaic devices. In this work, an efficient surface passivation method for emerging CsPbI 3 perovskite QDs using a variety of inorganic cesium salts (cesium acetate (CsAc), cesium idodide (CsI), cesium carbonate (Cs 2 CO 3 ), and cesium nitrate (CsNO 3 )) is reported. The Cs‐salts post‐treatment can not only fill the vacancy at the CsPbI 3 perovskite surface but also improve electron coupling between CsPbI 3 QDs. As a result, the free carrier lifetime, diffusion length, and mobility of QD film are simultaneously improved, which are beneficial for fabricating high‐quality conductive QD films for efficient solar cell devices. After optimizing the post‐treatment process, the short‐circuit current density and fill factor are significantly enhanced, delivering an impressive efficiency of 14.10% for CsPbI 3 QD solar cells. In addition, the Cs‐salt‐treated CsPbI 3 QD devices exhibit improved stability against moisture due to the improved surface environment of these QDs. These findings will provide insight into the design of high‐performance and low‐trap‐states perovskite QD films with desirable optoelectronic properties.