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Double‐cable conjugated polymers with near‐infrared (NIR) electron acceptors are synthesized for use in single‐component organic solar cells (SCOSCs). Through the development of a judicious synthetic pathway, the highly sensitive nature of the 2‐(3‐oxo‐2,3‐dihydroinden‐1‐ylidene)malononitrile (IC)‐based electron acceptors in basic and protonic solvents is overcome. In addition, an asymmetric design motif is adopted to optimize the packing of donor and acceptor segments, enhancing charge separation efficiency. As such, the new double‐cable polymers are successfully applied in SCOSCs, providing an efficiency of over 10 % with a broad photo response from 300 to 850 nm and exhibiting excellent thermal/light stability. These results demonstrate the powerful design of NIR‐acceptor‐based double‐cable polymers and will enable SCOSCs to enter a new stage. [ABSTRACT FROM AUTHOR]

We developed a series of highly crystalline double‐cable conjugated polymers for application in single‐component organic solar cells (SCOSCs). These polymers contain conjugated backbones as electron donor and pendant perylene bisimide units (PBIs) as electron acceptor. PBIs are connected to the backbone via alkyl units varying from hexyl (C6H12) to eicosyl (C20H40) as flexible linkers. For double‐cable polymers with short linkers, the PBIs tend to stack in a head‐to‐head fashion, resulting in large d‐spacings (e.g. 64 Å for the polymer P12 with C12H24 linker) along the lamellar stacking direction. When the length of the linker groups is longer than a certain length, the PBIs instead adopt a more ordered packing likely via H‐aggregation, resulting in short d‐spacings (e.g. 50 Å for the polymer P16 with C16H32 linker). This work highlights the importance of linker length on the molecular packing of the acceptor units and the influences on the photovoltaic performance of SCOSCs. [ABSTRACT FROM AUTHOR]