Abstract
With close to 100% internal quantum efficiency over the absorption spectrum, photocurrents in perovskite solar cells (PSCs) are at their practical limits. It is therefore imperative to improve open-circuit voltages (VOC) in order to go beyond the current 100 mV loss-in-potential. Identifying and suppressing recombination bottlenecks in the device stack will ultimately drive the voltages up. In this work, we investigate in depth the recombination at the different interfaces in a PSC, including the charge selective contacts and the effect of grain boundaries. We find that the density of grain boundaries and the use of tunneling layers in a highly efficient PSC do not modify the recombination dynamics at 1 sun illumination. Instead, the recombination is strongly dominated by the dopants in the hole transporting material (HTM), spiro-OMeTAD and PTAA. The reduction of doping concentrations for spiro-OMeTAD yielded VOC's as high as 1.23 V in contrast to PTAA, which systematically showed slightly lower voltages. This work shows that a further suppression of non-radiative recombination is possible for an all-low-temperature PSC, to yield a very low loss-in-potential similar to GaAs, and thus paving the way towards higher than 22% efficiencies.