TY - JOUR A1 - Lang, Felix A1 - Köhnen, Eike A1 - Warby, Jonathan A1 - Xu, Ke A1 - Grischek, Max A1 - Wagner, Philipp A1 - Neher, Dieter A1 - Korte, Lars A1 - Albrecht, Steve A1 - Stolterfoht, Martin T1 - Revealing fundamental efficiency limits of monolithic perovskite/silicon tandem photovoltaics through subcell characterization JF - ACS Energy Letters N2 - Perovskite/silicon tandem photovoltaics (PVs) promise to accelerate the decarbonization of our energy systems. Here, we present a thorough subcell diagnosis methodology to reveal deep insights into the practical efficiency limitations of state-of-the-art perovskite/silicon tandem PVs. Our subcell selective intensity-dependent photoluminescence (PL) and injection-dependent electroluminescence (EL) measurements allow independent assessment of pseudo-V-OC and power conversion efficiencies (PCEs) for both subcells. We reveal identical metrics from PL and EL, which implies well-aligned energy levels throughout the entire cell. Relatively large ideality factors and insufficient charge extraction, however, cause each a fill factor penalty of about 6% (absolute). Using partial device stacks, we then identify significant losses in standard perovskite subcells due to bulk and interfacial recombination. Lastly, we present strategies to minimize these losses using triple halide (CsFAPb(IBrCI)(3)) based perovskites. Our results give helpful feedback for device development and lay the foundation toward advanced perovskite/silicon tandem PVs capable of exceeding 33% PCE. Y1 - 2021 U6 - https://doi.org/10.1021/acsenergylett.1c01783 SN - 2380-8195 VL - 6 IS - 11 SP - 3982 EP - 3991 PB - American Chemical Society CY - Washington ER - TY - JOUR A1 - Zu, Fengshuo A1 - Warby, Jonathan A1 - Stolterfoht, Martin A1 - Li, Jinzhao A1 - Shin, Dongguen A1 - Unger, Eva A1 - Koch, Norbert T1 - Photoinduced energy-level realignment at interfaces between organic semiconductors and metal-halide perovskites JF - Physical review letters N2 - In contrast to the common conception that the interfacial energy-level alignment is affixed once the interface is formed, we demonstrate that heterojunctions between organic semiconductors and metal-halide perovskites exhibit huge energy-level realignment during photoexcitation. Importantly, the photoinduced level shifts occur in the organic component, including the first molecular layer in direct contact with the perovskite. This is caused by charge-carrier accumulation within the organic semiconductor under illumination and the weak electronic coupling between the junction components. Y1 - 2021 U6 - https://doi.org/10.1103/PhysRevLett.127.246401 SN - 0031-9007 SN - 1079-7114 VL - 127 IS - 24 PB - American Physical Society CY - College Park ER -