Unraveling the Surface State of Photovoltaic Perovskite Thin Film

Recently, most of the highly efficient perovskite optoelectronic devices have been reported to employ effective surface passivation strategies, further confirming the significance of surface states in regulating their device performance. Therefore, an in-depth understanding and a systematic approach toward comprehensive investigations on perovskite surface states are urgently required. Here, we present methodical studies toward understanding the surface states in perovskite thin films utilizing a molecular “positively charged defect indicator” strategy. In formamidinium (FA)-methylammonium (MA) mixed-cation perovskite thin films, a nonuniform distribution of cations is uncovered with FA cations being close to the top and MA close to the bottom of the film, which leads to unique surface defect energetics. Antisite FA_I was found to become a dominant deep trap on the surface of this system. As a result, a surface recombination velocity as low as 20 cm/s was achieved in such FA-based perovskite photovoltaic devices.