High Open-Circuit Voltage Perovskite/Organic Tandem Solar Cells and Photocathodes via Interface Engineering

Le résumé fourni par la source

Perovskite/organic tandem architectures provide a versatile platform for achieving high photovoltage and efficient solar-energy conversion, yet their performance and operational stability are critically constrained by electronic losses and chemical instability at buried hole-selective interfaces, particularly in wide-bandgap perovskite top cells. Here, we present interface engineering strategies that address these limitations by simultaneously controlling interfacial energetics, chemical robustness, and strain evolution in tandem systems spanning photovoltaics and photoelectrochemistry. A multi-functional hole-selective layer based on blended phosphonic acid self-assembled molecules is shown to homogenize surface potential, improve energy level alignment, and suppress lattice strain and light-induced phase segregation in wide bandgap perovskites, enabling perovskite/organic tandem solar cells with open-circuit voltage ( V oc) exceeding 2.2 V, fill factors above 84%, and efficiencies approaching 25%. In addition, a chemically stabilized self-assembled monolayer formed via potassium carbonate mediated deprotonation of carbazole-based phosphonic acids yields solvent-resistant and strongly anchored hole-selective interfaces that minimize non-radiative recombination and preserve interfacial integrity during perovskite processing. This robust interfacial chemistry further enables the first transparent, metal-free perovskite/organic tandem photocathode capable of stable operation in aqueous electrolyte, delivering photovoltages above 2.1 V with external quantum efficiency validated photocurrent generation. Together, these results establish chemically engineered hole selective interfaces as a unifying and scalable design principle for high V oc tandem photovoltaics and integrated solar-to-chemical energy conversion systems.

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