Achieving robust cholesteric liquid crystal polymer networks with high luminescence dissymmetry factor

Circularly polarized luminescence (CPL) is a key enabling technology for next-generation photonics, yet developing materials combining high stability, brightness, and dissymmetry factor (g_lum) remains a formidable challenge. A promising strategy involves solidifying highly-ordered emissive liquid crystals into robust polymer networks, but this process is often hindered by polymerization-induced stress that destroys the delicate chiral architecture. Here, we establish design principles to overcome this paradox through a synergistic co-design of monomer and network. We discover that fluorene-based monomers combining core planarity and segmental flexibility facilitate near-ideal helical assembly, achieving an exceptional fluidic g_lum of 0.60. Critically, employing a topologically-matched bifunctional crosslinker minimizes network stress, successfully preserving this elite performance to yield a robust thermoset with a record-high final g_lum of 0.54. In this work, we show that this rational strategy effectively bridges the gap between ideal fluidic systems and practical solid-state materials, paving the way for advanced chiroptical applications.