Detrimental Effect of Unreacted PbI₂ on the Long-Term Stability of Perovskite Solar Cells

Excess/unreacted lead iodide (PbI₂) has been commonly used in perovskite films for the state-of-the-art solar cell applications. However, an understanding of intrinsic degradation mechanisms of perovskite solar cells (PSCs) containing unreacted PbI₂ has been still insufficient and, therefore, needs to be clarified for better operational durability. Here, it is shown that degradation of PSCs is hastened by unreacted PbI₂ crystals under continuous light illumination. Unreacted PbI₂ undergoes photodecomposition under illumination, resulting in the formation of lead and iodine in films. Thus, this photodecomposition of PbI₂ is one of the main reasons for accelerated device degradation. Therefore, this work reveals that carefully controlling the formation of unreacted PbI₂ crystals in perovskite films is very important to improve device operational stability for diverse opto-electronic applications in the future.