We demonstrate that a poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate)/diindenoperylene (PEDOT:PSS/DIP) interfacial bilayer could serve as a structural template to enable the morphological control of bulk heterojunctions (BHJs) by co-evaporation of tetraphenyldibenzoperiflanthene:fullerene (DBP:C), which greatly improves the device performances. Especially, we show that isolated crystalline domains of C can be well-controlled at the nanoscale during the co-evaporation. Photoluminescence spectra indicate the realization of DIP/DBP cascade energy architecture, which significantly facilitates both the energy transfer and photocurrent generation. In addition, with bias-dependent external quantum efficiency analysis, we reveal that such a cascade energy device architecture greatly suppresses the energy recombination in both carrier and exciton transfer, resulting in a high open-circuit voltage and a high fill factor. By carefully optimizing the interfacial and BHJ layers, we achieved a high-performance organic photovoltaic cell with a power conversion efficiency of 5.0 ± 0.3%.
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