Reducing Surface Recombination Velocities at the Electrical Contacts Will Improve Perovskite Photovoltaics

We explore the effects of nonradiative recombination at the extracting contacts on the achievable performance of halide perovskite photovoltaic cells. First, we perform device simulations using standard drift-diffusion models with experimental semiconductor parameters matching those of methylammonium lead triiodide (MAPbI3). We quantify the range of surface recombination velocities (SRVs) that would allow this archetypal perovskite to reach power conversion efficiencies of 27%. In particular, for contacts with well-aligned energy levels, SRVs of ∼1–10 cm/s should enable open-circuit voltages of 1.30 V, within 96% of the Shockley–Queisser limit. Next, we use time-resolved photoluminescence to experimentally determine the SRVs on 14 different common electron- and hole-extracting contacts, including TiO2, SnO2, ZnO, PCBM, ITIC, ICBA, TPBi, PEDOT:PSS, PTAA, PVK, NiO, MoO3, WO3, and spiro-OMeTAD. These results point the way to the selection and rational engineering of better contacts as a means to achieve higher efficiencies in perovskite solar cells.