High Open-Circuit Voltage: Fabrication of Formamidinium Lead Bromide Perovskite Solar Cells Using Fluorene–Dithiophene Derivatives as Hole-Transporting Materials

Four different fluorene–dithiophene derivative-based hole-transporting materials (HTMs) (SO7–10) have been synthesized via a facile route and were successfully used in the fabrication of formamidinium lead bromide perovskite solar cells. Detailed characterization of the new compounds was carried out through 1H/13C NMR spectroscopy, mass spectrometry, ultraviolet–visible and photoluminescence spectroscopy, and cyclic voltammetry. Under AM1.5 G illumination, the mesoscopic CH(NH2)2PbBr3 perovskite solar cell employing SO7 as the HTM displayed an outstanding photovoltage (Voc) of 1.5 V with an efficiency (η) of 7.1%. The photovoltaic performance is on par with the device using the state-of-the-art Spiro-OMeTAD as HTM, which delivered a Voc of 1.47 V and a maximum η of 6.9%. A density functional theory approach with GW simulations including spin–orbit coupling and electrochemical measurements revealed deeper highest occupied molecular orbital levels for newly synthesized fluorene–dithiophene derivatives, whic...