Perovskite Solar Cells with Carbon-based Electrodes - Quantification of Losses and Strategies to Overcome Them

Carbon-based electrodes represent a promising approach to improve stability and up-scalability of perovskite photovoltaics. The temperature at which these contacts are processed defines the absorber grain size of the perovskite solar cell: in cells with low-temperature carbon-based electrodes (L-CPSCs), layer-by-layer deposition is possible, allowing perovskite crystals to be large (>100 nm), while in cells with high-temperature carbon-based contacts (H-CPSCs), crystals are constrained to 10-20 nm in size. To enhance the power conversion efficiency of these devices, the main loss mechanisms are identified for both systems. Measurements of charge carrier lifetime, quasi-Fermi level splitting (QFLS) and light-intensity-dependent behavior, supported by numerical simulations, clearly demonstrate that H-CPSCs strongly suffer from non-radiative losses in the perovskite absorber, primarily due to numerous grain boundaries. In contrast, large crystals of L-CPSCs provide a long carrier lifetime (1.8 µs) and exceptionally high QFLS of 1.21 eV for an absorber bandgap of 1.6 eV. These favorable characteristics explain the remarkable open-circuit voltage of over 1.1 V in hole-selective layer-free L-CPSCs. However, the low photon absorption and poor charge transport in these cells limit their potential. Finally, effective strategies are provided to reduce non-radiative losses in H-CPSCs, transport losses in L-CPSCs, and to improve photon management in both cell types.