The introduction of carbazole-based self-assembling molecules (SAMs) as hole transport layers (HTLs) has been a key step in the development of highly efficient perovskite-based solar cells. To this date, most SAM-related studies have focused on the optimization and understanding of SAMs by changing system parameters before or during the SAM formation process. Postdeposition treatments, like a washing step or annealing treatment, are commonly utilized but have not yet been thoroughly investigated and optimized. In this study, we investigated these treatments systematically for the SAM [4-(3,6-dimethyl-9H-carbazol-9-yl)butyl]phosphonic acid (Me-4PACz) as the HTL in perovskite/silicon tandem solar cells. Our results highlight that postdeposition treatments present an easy way to tune the thickness and orientation of the molecules in a SAM layer, helping to create dense and highly ordered monolayers. Besides that, we introduced cyclic voltammetry as a characterization technique for SAMs, which provides quantitative information about fundamental SAM properties such as surface coverage or electron blocking capability.
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