Elucidating the Role of a Tetrafluoroborate‐Based Ionic Liquid at the n‐Type Oxide/Perovskite Interface

Abstract Halide perovskites are currently one of the most heavily researched emerging photovoltaic materials. Despite achieving remarkable power conversion efficiencies, perovskite solar cells have not yet achieved their full potential, with the interfaces between the perovskite and the charge‐selective layers being where most recombination losses occur. In this study, a fluorinated ionic liquid (IL) is employed to modify the perovskite/SnO 2 interface. Using Kelvin probe and photoelectron spectroscopy measurements, it is shown that depositing the perovskite onto an IL‐treated substrate results in the crystallization of a perovskite film which has a more n‐type character, evidenced by a decrease of the work function and a shift of the Fermi level toward the conduction band. Photoluminescence spectroscopy and time‐resolved microwave conductivity are used to investigate the optoelectronic properties of the perovskite grown on neat and IL‐modified surfaces and it is found that the modified substrate yields a perovskite film which exhibits an order of magnitude lower trap density than the control. When incorporated into solar cells, this interface modification results in a reduction in the current–voltage hysteresis and an improvement in device performance, with the best performing devices achieving steady‐state PCEs exceeding 20%.