High-Performance Circular Polarization Multiple-Resonance\nTADF Molecules with Enhanced Long-Range Charge Transfer Based on Chiral\nParacyclophane

Circularly polarized multiple-resonance\nthermally activated delayed\nfluorescence (CP-MR-TADF) materials have received widespread attention\nin recent years, but it remains a formidable challenge to design high-performance\nCP-MR-TADF emitters concurrently exhibiting high quantum efficiency,\nnarrowband emission, and high dissymmetry factor (<i>g</i>). Here, we perform an in-depth theoretical investigation on the\nCP-MR-TADF materials based on [2.2] paracyclophane (pCp) derivatives.\nThe MR-based materials with enhanced long-range charge transfer (LRCT)\ncharacteristics upon excitation show increased <i>g</i> values\nowing to the coaxial dominated transition components of the transition\nelectric dipole moment (TEDM) and the transition magnetic dipole moment\n(TMDM) but inevitably result in the loss of narrowband emission performance.\nFurthermore, the newly designed molecules by fusing the peripheral\nbenzene units of MR cores within the planar chiral pCp bridge maintain\nnarrowband emissions and exhibit increased <i>g</i> values\non the order of 1 × 10<sup>–3</sup>. These findings with\nrich physical insights on the structure–performance relation\nof chiral paracyclophane-based molecules should provide important\nclues for designing high-performance chiral materials.