Kulkarni, AshishSarkar, RanjiniAkel, SamahHäser, MariaKlingebiel, BenjaminWuttig, MatthiasWiegand, SimoneChakraborty, SudipSaliba, MichaelKirchartz, Thomas2024-06-122024-06-1220231616-30281616-301X1891559036http://nbn-resolving.de/urn:nbn:de:bsz:93-opus-ds-145226http://elib.uni-stuttgart.de/handle/11682/14522http://dx.doi.org/10.18419/opus-14503Perovskite solar cells employing [4-(3,6-dimethyl-9H-carbazol-9-yl)butyl]phosphonic acid (Me-4PACz) self-assembled monolayer as the hole transport layer have been reported to demonstrate a high device efficiency. However, the poor perovskite wetting on Me-4PACz caused by poor perovskite ink interaction with the underlying Me-4PACz presents significant challenges for fabricating efficient perovskite devices. A triple co-solvent system comprising dimethylformamide (DMF), dimethyl sulfoxide (DMSO), and N-methyl-2-pyrrolidone (NMP) is employed to improve the perovskite ink-Me-4PACz coated substrate interaction and obtain a uniform perovskite layer. In comparison to DMF- and DMSO-based inks, the inclusion of NMP shows considerably higher binding energies of the perovskite ink with Me-4PACz as revealed by density-functional theory calculations. With the optimized triple co-solvent ratio, the perovskite devices deliver high power conversion efficiencies of >20%, 19.5%, and ≈18.5% for active areas of 0.16, 0.72, and 1.08 cm2, respectively. Importantly, this perovskite ink-substrate interaction approach is universal and helps in obtaining a uniform layer and high photovoltaic device performance for other perovskite compositions such as MAPbI3, FA1-xMAxPbI3-yBry, and MA-free FA1−xCsxPbI3-yBry.eninfo:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by/4.0/621.3article2024-04-25