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Abstract Adjusting the energy levels and fibrillar morphology is paramount to enhancing the power conversion efficiency (PCE) of organic solar cells (OSCs). In the present study, an increase in the open‐circuit voltage ( V OC ) is facilitated through the elongation of the alkyl chain within AQx (namely AQx‐8), aiming to decrease the free volume ratio (FVR). This reduction in FVR attenuates electron‐phonon coupling, thereby augmenting emission efficiency and diminishing the non‐radiative energy loss (Δ E nr ). To further refine the energy levels and morphological characteristics, the external undecyl chain of AQx‐8 is substituted with a shorter carbon chain and cyclohexane noted for its considerable steric hindrance (AQx‐H). This alteration significantly mitigates intermolecular aggregation, expands the bandgap, and elevates the lowest unoccupied molecular orbital (LUMO) energy level, culminating in an elevated V OC of 0.923 V in devices based on AQx‐H. Morphological analysis reveals that blends based on AQx‐H exhibit an enhanced multi‐length‐scale fibrillar structure, which is conducive to exciton dissociation and charge transport, thereby contributing to a high fill factor (FF) nearing 80%. Consequently, this study reports one of the highest binary PCEs documented, standing at 19.5% (with certification at 19.0%).
Zeng et al. (Thu,) studied this question.