The Impact of a Dynamic Two‐Step Solution Process on Film Formation of Cs0.15(MA0.7FA0.3)0.85PbI3 Perovskite and Solar Cell Performance

This paper provides deep understanding of the formation mechanism of perovskite film fabricated by sequential solution‐based methods. It compares two sequential spin‐coating methods for Cs0.15(MA0.7FA0.3)0.85PbI3 perovskite. First is the “static process,” with a stoppage between the two spin‐coating steps (1st PbI2‐CsI‐dimethyl sulfoxide (DMSO)‐dimethylformamide (DMF) and 2nd methylammonium iodide (MAI)‐formamidinium iodide (FAI)‐isopropyl alcohol). Second is the “dynamic process,” where the 2nd precursor is dispensed while the substrate is still spinning from the 1st step. For the first time, such a dynamic process is used for Cs0.15(MA0.7FA0.3)0.85PbI3 perovskite. Characterizations reveal improved film formation with the dynamic process due to the “retainment” of DMSO‐complex necessary for the intermediate phase which i) promotes intercalation between precursors and ii) slows down perovskite crystallization for full conversion. The comparison on as‐deposited perovskite before annealing indicates a more ordered film using this dynamic process. This results in a thicker, more uniform film with higher degree of preferred crystal orientation and higher carrier lifetime after annealing. Therefore, dynamic‐processed devices present better performance repeatability, achieving a higher average efficiency of 17.0% compared to static ones (15.0%). The new insights provided by this work are important for perovskite solar cells processed sequentially as the process has greater flexibility in resolving solvent incompatibility, allowing separate optimizations and allowing different deposition methods. This paper investigates the formation mechanism of Cs0.15(MA0.7FA0.3)0.85PbI3 perovskite fabricated by a dynamic sequential solution process. It is revealed that motion dispense for the 2nd deposition step “suspends” the dimethyl sulfoxide (DMSO)‐complex necessary for the intermediate phase i) promoting intercalation between precursors and ii) slowing down perovskite crystallization for full conversion, resulting in film with higher uniformity and better electrical properties.