How varying surface wettability of different PEDOT:PSS formulations and their mixtures affects perovskite crystallization and the efficiency of inverted perovskite solar cells

The physico-chemical interaction, surface, and electrical properties of hole transport layers (HTLs) significantly affect the wettability and film crystallization of the deposited perovskite and the corresponding performance of inverted perovskite solar cells (PSCs). One of the most frequently used HTLs for inverted PSCs is poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS). Various commercial PEDOT:PSS formulations have already been tested as HTLs. Until now mixtures of these remained rather unexplored. In this study, three commercially available PEDOT:PSS formulations (PH, PH1000, and AI4083), as well as three mixtures (PH:PH1000, PH:AI4083, and PH:PH1000:AI4083; in a 1 : 1 and 1 : 1 : 1 ratios) were used as HTLs to investigate the crystallization of perovskite films and the performance of associated PSCs. Of the three formulations, PEDOT:PSS PH showed better perovskite crystallization, resulting in better solar cell performance followed by both PH:AI4083 and PH:PH1000:AI4083 layers. The pioneering work on mixing PEDOT:PSS resulted in new combinations of PEDOT:PSS, with new properties (work function, surface wettability, and roughness) which are very important parameters for perovskite crystallization and corresponding device efficiencies and stabilities. All PSCs that use the mixed PEDOT:PSS as HTLs revealed higher fill factor and open-circuit voltage values above 900 mV, which is not the same except for PEDOT:PSS PH. As a result, we believe that such a mixing strategy could aid in the creation of various PEDOT:PSS combinations with tuneable properties for certain applications.