In Situ Investigations of Al/Perovskite Interfacial Structures

Interfacial properties of perovskite layers and metal electrodes play a crucial role in device performance and long-term stability of perovskite solar cells. In this work, we performed a comprehensive study of the interfacial structures and ion migration at the interface of a CH₃NH₃PbI₃ perovskite layer and an Al electrode using in situ synchrotron radiation photoemission spectroscopy measurements. It was found that the Al electrode can react with the perovskite layers, leading to the formation of aluminum iodide species and the bonding between Al and N, as well as the reduction of Pb²⁺ ions to metallic Pb species at the interface. Moreover, during the Al deposition, iodide ions can migrate from the CH₃NH₃PbI₃ subsurface to the Al electrode, while the reduced Pb remains at the subsurface. The depth profile photoemission measurements, made by varying the photon energies of incident synchrotron radiation X-rays, demonstrate that the reaction occurs at the Al/CH₃NH₃PbI₃ interface at least with a thickness of ∼3.5 nm below the perovskite surface. This study provides an atomic-level fundamental understanding of the Al/CH₃NH₃PbI₃ interfacial structures and insight into the degradation mechanisms of perovskite solar cells when using Al metal as the electrode.