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Photoinduced intermolecular charge transfer (PICT) determines the voltage loss in bulk heterojunction (BHJ) organic photovoltaics (OPVs), and this voltage loss can be minimized by inducing efficient PICT, which requires energy‐state matching between the donor and acceptor at the BHJ interfaces. Thus, both geometrically and energetically accessible delocalized state matching at the hot energy level is crucial for achieving efficient PICT. In this study, an effective method for quantifying the hot state matching of OPVs was developed. The degree of energy‐state matching between the electron donor and acceptor at BHJ interfaces was quantified using a mismatching factor (MF) calculated from the modified optical density of the BHJ. Furthermore, the correlation between the open‐circuit voltage (Voc) of the OPV device and energy‐state matching at the BHJ interface was investigated using the calculated MF. The OPVs with small absolute MF values exhibited high Voc values. This result clearly indicates that the energy‐state matching between the donor and acceptor is crucial for achieving a high Voc in OPVs. Because the MF indicates the degree of energy‐state matching, which is a critical factor for suppressing energy loss, it can be used to estimate the Voc loss in OPVs. [ABSTRACT FROM AUTHOR]

For advancing next‐generation optoelectronics, a versatile strategy for fabricating π‐conjugated polymer (π‐CP)/chiral‐small molecule (SM) hybrid films through co‐crystallization‐mediated chirality transfer is reported. The transfer of optical chirality from 1,1′‐binaphthyl–2,2′‐diamine (BN), a representative chiral inducer SM, to thin films of various achiral π‐CPs, including non‐fluorene π‐CPs, is achieved by simply blending the π‐CPs with BN using aromatic organic solvents. The resulting π‐CP/chiral‐SM hybrid films exhibit chiroptical responses at the main electronic absorption bands of various π‐CPs. Studies of the morphology, crystalline structure, and phase‐separation structure of a representative hybrid system of poly(3‐hexylthiophene) (P3HT) and BN reveal that these hybrid films exhibit a characteristic lamellar structure where the π‐CPs co‐crystallize with chiral BN molecules, facilitated by aromatic solvent‐assisted intermolecular π–π interactions. In‐depth photophysical analysis suggests that BN molecules co‐crystallized in the P3HT lamellar structure induce asymmetrically misaligned transition dipoles along the P3HT conjugated backbone, transferring optical chirality from BN to P3HT under circularly polarized light illumination. As a proof‐of‐concept, chiroptical photodiodes based on π‐CP/chiral‐SM hybrid films and printed micropatterns, exhibiting a distinguishable photocurrent response depending on the direction of circularly polarized light are successfully demonstrated. [ABSTRACT FROM AUTHOR]