Amine-Thiol/Selenol Chemistry for Efficient and Stable Perovskite Solar Cells

Abstract

Controlling the crystallization of perovskites is imperative to reduce defect densities in perovskite thin films and extend device lifetimes. In this work, combinations of amine and chalcogenide ligands were introduced in the sequential deposition method to fabricate highly crystalline and oriented formamidinium lead iodide thin films with reduced defect densities and increased charge carrier lifetimes. The dual additives can tune the perovskite intermediate state and control the crystallization, leading to devices with improved efficiencies and stabilities. While thiophenol failed to prevent the amine ligand from degrading the perovskite precursors, benzene selenol combinations with amine ligands drastically changed the solution chemistry to increase the PbI2 conversion to highly crystalline and oriented α-FAPbI3 films with lower defect densities. X-ray photoelectron spectroscopy studies reveal benzene selenol evaporates from the thin film, leaving behind a modified surface, which is associated with the amine additive. These results indicate the amine selection can be used to tune the surface properties. Lastly, we propose a highly tunable I2 reduction strategy using chalcogenide chemistry to help enable the realization of perovskite solar cells with high performance and stability.