Enhancing the Efficiency and Stability of Triple-Cation Perovskite Solar Cells by Eliminating Excess PbI2 from the Perovskite/Hole Transport Layer Interface

Metal halide perovskites are promising contenders for next-generation photovoltaic applications due to their remarkable photovoltaic efficiency and their compatibility with solution-processed fabrication. Among the various strategies to control the crystallinity and the morphology of the perovskite active layer and its interfaces with the transport layers, fabrication of perovskite solar cells from precursor solutions with a slight excess of PbI₂ has become very common. Despite this, the role of such excess PbI₂ is still rather controversial, lacking consensus on its effect on the bulk and interface properties of the perovskite layer. In this work, we investigate the effect of removing the excess PbI₂ from the surface of a triple-cation mixed-halide Cs_0.05(FA_0.83MA_0.17)_0.95Pb(I_0.83Br_0.17)₃ perovskite layer by four different organic salts on their photovoltaic performance and stability. We show that treatments with iodide salts such as methylammonium iodide (MAI) and formamidinium iodide (FAI) can lead to the strongest beneficial effects on solar cell efficiency, charge recombination suppression, and stability while non-iodide salts such as methylammonium bromide (MABr) and methylammonium chloride (MACl) can also provide improvement in terms of charge recombination suppression and stability to a moderate extent in comparison to the untreated sample. Under optimized conditions and continuous solar illumination, the MAI- and FAI-treated devices maintained 81 and 86% of their initial power conversion efficiency (PCEs), respectively, after 100 h of continuous illumination (versus 64% for the untreated solar cell with excess PbI₂). Our study demonstrates that eliminating excess PbI₂ at the perovskite/hole transport layer (HTL) interface by treating the perovskite surface with organic salts is a simple and efficient route to enhance the efficiency, and in particular the stability of perovskite solar cells.