Programming Helical Charge-Trapping Superstructures for High-Performance White Circularly Polarized Luminescence and...

Chiral organic phosphors with asymmetric electronic configurations and divergent orbital angular momenta are fundamental building blocks for circularly polarized luminescence (CPL) materials, holding great promise for colored LEDs and displays. However, realizing high-purity, high-efficiency white CPL (W-CPL) and circularly polarized long-persistent luminescence (CP-LPL) in a single luminophore remains a formidable challenge. Herein, we report a duplex photopolymerization strategy to construct helical liquid-crystalline charge-trapping chiral architectures, integrating supramolecular cholesteric assembly and in situ olefin photopolymerization. Insulating alkene linkages barely disturb intrinsic singlet-triplet distributions and phosphorescence. Dual covalent/noncovalent crosslinking enhances polymer rigidity, stabilizes triplet excitons, and forms chiral exciplexes to produce high-performance W-CPL from combined fluorescence and phosphorescence. The optimized helical polymer delivers a 0.34 s CP-RTP lifetime, ∼20 s afterglow, 39% quantum efficiency, and giant g_{p h o s} factors (+1.24, -1.40) via charge trapping and chiral light reflection. Chiral FRET further enables yellow/orange/red/NIR CP-LPL. This chiral exciplex polymer resists moisture, solvents, and heat, showing broad application potential in CP-WLEDs and 3D anti-counterfeiting.