LAUSR

ConspectusConjugated polymers for application in organic solar cells (OSCs) have been developed from poly(phenylenevinylene) to poly(3-hexylthiophene) and then to "donor-acceptor" structures, providing power conversion efficiencies (PCEs) over 18% when blending with the electron acceptor as a two-component photoactive layer. Besides, graft-structural double-cable conjugated polymers that use an electron donor as conjugated backbones and an electron acceptor as pendant side units are one kind of conjugated polymer, in which charge carriers are generated in a single polymer. Therefore, double-cable conjugated polymers can be used as a single photoactive layer in single-component OSCs (SCOSCs). The covalently linked electron donor and acceptor enable double-cable polymers to maintain stable microstructures during long-term operation compared to two-component systems, which is very important for OSCs toward large-area applications. However, SCOSCs based on double-cable conjugated polymers provided PCEs below 3% in a long period, which is lagging far behind PCEs of two-component OSCs. The key reason for this is the limited number of chemical structures and the difficulty to tune the morphology in these polymers.In this Account, we provide an overview about our efforts on developing new double-cable conjugated polymers with rylene diimides as side units, and how to realize high PCEs in SCOSC devices. The studies start from developing a "functionalization-polymerization" method to synthesize the polymers containing rylene diimide acceptors, so that large amounts of double-cable conjugated polymers with distinct physical and electrochemical properties were obtained. Then, we will discuss how to control the nanophase separation in the crystalline region and optimize the miscibility in the amorphous region of double-cable polymers, simultaneously facilitating exciton dissociation and charge transport. With these efforts, a high PCE of 8.4% has been obtained, representing the record PCE in SCOSCs. In addition, the physical process and the stability of SCOSCs will be discussed. We hope that this account will inspire many innovative studies in this field and push the PCEs of SCOSCs to a new stage.