▎ 摘　　要

Owing to their record-breaking energy conversion efficiencies, hybrid organometallic perovskites have emerged as the most promising light absorbers and ambipolar carrier transporters for solution-processable solar cells. Simultaneously, due to its exceptional electron mobility, graphene represents a prominent candidate for replacing transparent conducting oxides. Thus, it is possible that combining these wonder materials may propel the efficiency toward the Schokley-Queisser limit. Here, using first-principles calculations on graphene-CH3NH3PbI3 interfaces, we find that graphene suppresses the octahedral tilt in the very first perovskite monolayer, leading to a nanoscale ferroelectric distortion with a permanent polarization of 3 mC/m(2). This interfacial ferroelectricity drives electron extraction from the perovskite and hinders electron-hole recombination by keeping the electrons and holes separated. The interfacial ferroelectricity identified here simply results from the interplay between graphene's planar structure and CH3NH3PbI3's octahedral connectivity; therefore, this mechanism may be effective in a much broader class of perovskites, with potential applications in photovoltaics and photocatalysis.