Highly Efficient Monolithic Tandem Solar Cells with Metal-Halide Perovskites

Integrating metal halide perovskite top cells with bottom cells formed by crystalline silicon or low band gap perovskites into monolithic tandem devices has recently attracted increased attention due to the high efficiency potential and application relevance of these cell architectures. Here we present our recent results on monolithic tandem combinations of perovskite top-cells with crystalline silicon, and Sn-Pb perovskites as well as tandem relevant aspects of perovskite single junction solar cells.
In 2020, we have shown that self-assembled monolayers (SAM) could be implemented as appropriate hole selective contacts. The implementation of new generation SAM molecules enabled further reduction of non-radiative recombination losses with high open circuit voltages and fill factor. By fine-tuning the SAM molecular structure even further, the photostability of perovskite composition with tandem-ideal band gaps of 1.68 eV could be enhanced by reduction of defect density and fast hole extraction. That enabled a certified efficiency for perovskite/silicon tandems at 29.15%.

By optical optimizations, we could further improve this value to 29.80% in 2021. Periodic nanotextures were used that show a reduction in reflection losses in comparison to planar tandems, with the new devices being less sensitive to deviations from optimum layer thicknesses. The nanotextures also enable a greatly increased fabrication yield from 50% to 95%. Moreover, the open-circuit voltage is improved by 15 mV due to the enhanced optoelectronic properties of the perovskite top cell on top of the nanotexture.

In the end of 2022, we enabled a new world record for perovskite/silicon tandem solar cells at 32.5% efficiency. We demonstrated that an additional surface treatment strongly reduces interface recombination and improves the band alignment with the C60 electron transporting material. With these modifications, single junction solar cells show high open circuit voltages of up to 1.28 V in a p-i-n configuration, and we achieve 2.00 V in monolithic tandem solar cells. A comparable surface treatment was also applied to 1.80 eV band gap perovskites to enable Voc values of 1.35 V and these were integrated into monolithic all-perovskite tandem solar cells enabling a certified efficiency of 27.5%.

In addition to the experimental material and device development, also main scientific and technological challenges and empirical efficiency limits as well as advanced analysis methods will be discussed for perovskite based tandem solar cells. In addition, results on upscaling and stability of these industrial relevant tandem solar cells by thermal evaporation will be shown.