Quantifying recombination and charge carrier extraction in halide perovskites via hyperspectral time-resolved photoluminescence imaging

Identifying sources of nonradiative recombination and quantifying charge carrier extraction in halide perovskite solar cells are important in further developing this thin-film technology. Steady-state and time-resolved photoluminescence (TRPL), in combination with analytical modeling, have emerged as non-destructive tools to achieve the desired results. However, the exact location of the recombination and charge carrier extraction losses in devices is often obscured by various competing processes when photoluminescence measurements are analyzed. Here, we show via absolute-photon-calibrated hyperspectral photoluminescence and TRPL imaging how surface passivation and inhomogeneities at interfaces impact the photoluminescence quantum yields and minority carrier lifetimes. Laser illumination from the perovskite and glass/TiO2 sides allows us to disentangle changes in surface recombination velocity from the charge carrier extraction at the electron transport layer. We find that charge extraction is spatially modulated due to an inhomogeneous mesoporous (mp)-TiO2 film thickness. Our results show that the mp-TiO2 layer is not fully optimized since the electronic properties are spatially modified, leading to lateral changes in quasi-Fermi-level splitting, minority carrier lifetime and, consequently, a reduction in open-circuit voltage.