On the molecular origin of charge separation at the donor-acceptor interface
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Fullerene-based acceptors have dominated organic solar cells for almost two decades. It is only within the last few years that alternative acceptors rival their dominance, introducing much more flexibility in the optoelectronic properties of these material blends. However, a fundamental physical understanding of the processes that drive charge separation at organic heterojunctions is still missing but urgently needed to direct further material improvements. Here we use a combined experimental and theoretical approach to understand the intimate mechanisms by which molecular structure contributes to exciton dissociation, charge separation, and charge recombination at the donor-acceptor (D-A) interface. We use model systems comprised of polythiophene-based donor and rylene diimide-based acceptor polymers and perform a detailed density functional theory (DFT) investigation. The results point to the roles that geometric deformations and direct-contact intermolecular polarization play in establishing a driving force (energy gradient) for the optoelectronic processes taking place at the interface. A substantial impact for this driving force is found to stem from polymer deformations at the interface, a finding that can clearly lead to new design approaches in the development of the next generation of conjugated polymers and small molecules.
Sini , G , Schubert , M , Risko , C , Roland , S , Lee , O , Chen , Z , Richter , T , Dolfen , D , Coropceanu , V , Ludwigs , S , Scherf , U , Facchetti , A , Fréchet , J & Neher , D 2018 , ' On the molecular origin of charge separation at the donor-acceptor interface ' , Advanced Energy Materials , vol. 8 , no. 12 , 1702232 . https://doi.org/10.1002/aenm.201702232
Advanced Energy Materials
© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. This work has been made available online in accordance with the publisher’s policies. This is the author created, accepted version manuscript following peer review and may differ slightly from the final published version. The final published version of this work is available at https://doi.org/10.1002/aenm.201702232