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Chandrabose, Sreelakshmi; Chen, Kai; Barker, Alex J; Sutton, Joshua J; Prasad, Shyamal K. K; Zhu, Jingshuai; Zhou, Jiadong; Gordon, Keith C; Xie, Zengqi; Zhan, Xiaowei; Hodgkiss, Justin M
Journal of the American Chemical Society, 05/2019, Letnik: 141, Številka: 17Journal Article
Modest exciton diffusion lengths dictate the need for nanostructured bulk heterojunctions in organic photovoltaic (OPV) cells; however, this morphology compromises charge collection. Here, we reveal rapid exciton diffusion in films of a fused-ring electron acceptor that, when blended with a donor, already outperforms fullerene-based OPV cells. Temperature-dependent ultrafast exciton annihilation measurements are used to resolve a quasi-activationless exciton diffusion coefficient of at least 2 × 10–2 cm2/s, substantially exceeding typical organic semiconductors and consistent with the 20–50 nm domain sizes in optimized blends. Enhanced three-dimensional diffusion is shown to arise from molecular and packing factors; the rigid planar molecular structure is associated with low reorganization energy, good transition dipole moment alignment, high chromophore density, and low disorder, all enhancing long-range resonant energy transfer. Relieving exciton diffusion constraints has important implications for OPVs; large, ordered, and pure domains enhance charge separation and transport, and suppress recombination, thereby boosting fill factors. Further enhancements to diffusion lengths may even obviate the need for the bulk heterojunction morphology.
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