Proceedings of International Conference on Hybrid and Organic Photovoltaics (HOPV23)
DOI: https://doi.org/10.29363/nanoge.hopv.2023.204
Publication date: 30th March 2023
The most promising technological application of perovskite solar cells (PSCs) relies on the implementation of single junction perovskite photovoltaic devices in tandem architectures, either as Si-perovskite or all-perovskite. Notoriously, wide-gap perovskites (⁓1.7-1.8 eV) required for such solar cell design are reported to suffer from larger open-circuit voltage (VOC) losses compared to the narrower gap counterparts. We recently demonstrated that these energy losses are associated with strong interface recombination due to an energy misalignment between the perovskite and charge transport layers (CTL), resulting in the external VOC being lower compared to the internal quasi-Fermi level splitting (QFLS) of the same device. While at the p-interface there is a large variety of transport materials that can be used to mitigate this problem (metal oxides, polymers, and self-assembled monolayers), at the n-interface, fullerenes have been the only successful option so far. Due to this limitation, the non-radiative recombination losses at the n-interface are one of the major limitations of wide-gap perovskite solar cells. We also showed that interface passivations (such as GuaBr and ImBr) can reduce non-radiative recombination at this interface and close the QFLS-VOC mismatch. However, perovskite surface passivation methods can be highly sensitive to the type of perovskite and potentially hard to scale up. In this study, instead of using surface passivations or replacing the fullerenes ETL with other electron transport materials, we propose a simple approach to specifically tune the alignment of the electron-transport layer (ETL) by blending different fullerene derivatives in various ratios. We find that fine-tuning the blend ratio of the fullerenes allows for targeting preferential energetic alignment between the ETL and the perovskite layer, drastically reducing the VOC losses while keeping excellent charge transport. By inserting a thin interlayer of this blend between perovskite and C60 in 1.8 eV pin MA-free perovskite devices, we achieve VOCs up to 1.32 V and FF close to 84%, resulting in PCEs approaching 19%, among the highest reported for this bandgap. Importantly, by utilizing a PLQY spectral imaging technique on full devices, we find that the energetic mismatch between QFLS and VOC is effectively reduced when the fullerenes blend ratio is fully optimized. To confirm this point, drift-diffusion simulations modelling devices implementing these different blends show the same QFLS-VOC mismatch reduction when the perovskite and ETL are energetically aligned. We also demonstrate that our approach is fully compatible with perovskite tandem solar cells and potentially allows us to provide ideal alignment for a large variety of perovskite bandgaps. Our study shows that with appropriate interface design, it is possible to access the full QFLS potential of the perovskite material achieving high VOCs. As such, we demonstrate a simple and flexible method to optimize the solar cell architecture for perovskite with different bandgaps without the need of finding specific ETL materials for each perovskite bandgap.