Beyond Bulk Lifetimes: Insights into Lead Halide Perovskite Films from Time-Resolved Photoluminescence

Careful interpretation of time-resolved photoluminescence (TRPL) measurements can substantially improve our understanding of the complex nature of charge-carrier processes in metal-halide perovskites, including, for instance, charge separation, trapping, and surface and bulk recombination. In this work, we demonstrate that TRPL measurements combined with powerful analytical models and additional supporting experiments can reveal insights into the charge-carrier dynamics that go beyond the determination of minority-charge-carrier lifetimes. While taking into account doping and photon recycling in the absorber layer, we investigate surface and bulk recombination (trap-assisted, radiative, and Auger) by means of the shape of photoluminescence transients. The observed long effective lifetime indicates high material purity and good passivation of perovskite surfaces with exceptionally low surface recombination velocities on the order of about 10 cm/s. Finally, we show how to predict the potential open-circuit voltage for a device with ideal contacts based on the transient and steady-state photoluminescence data from a perovskite absorber film and including the effect of photon recycling.