Local Antiaromaticity-Mediated Chiral Donor-Acceptor Strategy for Efficient Circularly Polarized Luminescence.

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, 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.