Local Antiaromaticity‐Mediated Chiral Donor–Acceptor Strategy for Efficient Circularly Polarized Luminescence

Abstract

ABSTRACT Achieving highly efficient circularly polarized luminescence in organic light‐emitting diodes remains a fundamental challenge, because conventional chiral‐perturbation strategies are intrinsically limited by weak electronic coupling between chiral units and the emissive center. To address this limitation, a local antiaromaticity‐mediated chiral donor‐acceptor strategy is introduced. By integrating a locally antiaromatic chiral donor with one or two electron‐accepting triazine units, donor–acceptor and acceptor–donor–acceptor architectures are constructed that exhibit hybridized local and charge‐transfer excited states and enable hot‐exciton channels. Unlike conventional designs, the antiaromatic chiral donor directly contributes to the frontier molecular orbitals and excited‐state spin density distribution, inducing pronounced helical charge redistribution at the emissive center during charge‐transfer excitation. The localized antiaromatic character further strengthens the magnetic transition dipole moment, providing a synergistic amplification of circularly polarized emission. As a result, the optimized emitter ABH‐2TRZ affords deep‐blue circularly polarized electroluminescence with a dissymmetry factor of +7.4 × 10 −3 , a maximum external quantum efficiency of 6.38%, and color coordinates of (0.154, 0.089), close to the deep‐blue display standard. This work establishes antiaromatic chiral donors as an effective platform for high‐performance circularly polarized optoelectronic materials.