Fluorinated Polythiophenes with Alkylthiophene Side Chains Boosting the Performance of Wide Bandgap Perovskite Solar Cells

Wide bandgap (WBG) perovskite solar cells (PSCs) provide their merit of high voltage output but are faced with the overdeepened valence band and the notorious phase segregation. Herein, two alkylthiophene-substituted polythiophenes (PT4T-0F and PT4T-2F) are applied as the interfacial layer for the WBG (1.72 eV) PSCs. Compared with PT4T-0F, PT4T-2F with fluoride (F) on thiophene units in a conjugated backbone exhibits more planar configuration, higher hole mobility, and deeper highest occupied molecular orbital energy. By using PT4T-2F as an additive in antisolvent, crystal growth of FA0.83Cs0.17Pb(I0.7Br0.3)3 is successfully mediated, resulting in high ratio (100) plane exposure of the WBG perovskites, and defect passivation is simultaneously realized. The optimized device presents a high open-circuit voltage of 1.23 V and a power conversion efficiency of 19.20%. The long-term stabilities under moisture and thermal conditions are both improved. This work offers an ideal interlayer material for WBG PSC engineering and further provides a simple process to integrate simultaneous crystal mediation and interface optimization.