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The Intrinsic Role of the Fusion Mode and Electron-Deficient Core in Fused-Ring Electron Acceptors for Organic Photovoltaics.

The A-DA'D-A fused-ring electron acceptors featuring an angular fusion mode and electron-deficient core has significantly boosted the progress of organic solar cells. Herein, to reveal the intrinsic role of the peculiar A-DA'D-A structure, we have investigated the optoelectronic and excited state dynamics properties of a representative A-DA'D-A acceptor of Y6 in comparison with its A-D-A counterparts having different fusion modes. The results show that the angular fusion mode incorporation of electron-deficient core results in deeper and delocalized frontier orbitals, endowing Y6 with enhanced and red-shifted light absorption. Moreover, the angular fusion mode reduces electron-vibration couplings, accounting for the faster exciton diffusion, exciton dissociation, and electron transport for Y6. Notably, the exciton dissociation process can be further promoted by introducing the electron-deficient core, enabling efficient charge generation at low driving forces for the Y6-based devices.