Reduced Interface‐Mediated Recombination for High Open‐Circuit Voltages in CH3NH3PbI3 Solar Cells

Perovskite solar cells with all‐organic transport layers exhibit efficiencies rivaling their counterparts that employ inorganic transport layers, while avoiding high‐temperature processing. Herein, it is investigated how the choice of the fullerene derivative employed in the electron‐transporting layer of inverted perovskite cells affects the open‐circuit voltage ( V OC ). It is shown that nonradiative recombination mediated by the electron‐transporting layer is the limiting factor for the V OC in the cells. By inserting an ultrathin layer of an insulating polymer between the active CH 3 NH 3 PbI 3 perovskite and the fullerene, an external radiative efficiency of up to 0.3%, a V OC as high as 1.16 V, and a power conversion efficiency of 19.4% are realized. The results show that the reduction of nonradiative recombination due to charge‐blocking at the perovskite/organic interface is more important than proper level alignment in the search for ideal selective contacts toward high V OC and efficiency.