23.5% efficient monolithic perovskite/organic tandem solar cells based on an ultra-thin metal-like metal-oxide interconnect.

Abstract Multi-junction solar cells provide an avenue to overcome fundamental efficiency limits of single-junction devices. The facile bandgap tunability of metal-halide perovskite solar cells renders them attractive building blocks for multi-junction architectures. Combinations with crystalline silicon and copper indium gallium selenide (CIGS) cells have been reported. All-perovskite tandem cells have likewise shown promising results. Meanwhile, narrow-gap non-fullerene acceptors (NFA) have revived the area of organic solar cells (OSCs) and unlocked skyrocketing efficiencies. Organic and perovskite semiconductors share similar processing technologies, which renders them attractive partners in multi junction architectures. As of yet, perovskite/organic tandem cells show subpar efficiencies of 20 per cent, limited by the low open circuit voltage (Voc) of wide-gap perovskite cells and losses introduced by the interconnect between the sub-cells. Here, we demonstrate two-terminal p-i-n perovskite/organic tandem cells with an efficiency of 23.5 per cent and a high Voc of 2.15 volts, operating near the levels predicted by a semi-empirical model. The perovskite sub-cells with optimized charge extraction layers afford an unsurpassed combination of a high Voc and fill-factor. The organic back-cells provide a high external quantum efficiency in the near-infrared. In surprising contrast to paradigmatic concerns about limited photostability of non-fullerene cells, we evidence an outstanding operational stability if excitons are predominantly generated on the NFA, which is the case in a tandem cell, where the illumination is spectrally filtered by the perovskite cell. A novel interconnect based on an ultra-thin (1.5 nanometers) metal like indium oxide layer offers unprecedented low optical/electrical losses. This work sets a new milestone for perovskite/organic tandem devices, that outperform the best p-i-n perovskite single junctions and are at par with perovskite/CIGS and all-perovskite multi-junctions. Perovskite/organic tandem architectures bear a realistic potential to reach an efficiency above 31%.