Polymerization-with-assembly enables homogeneous circularly polarized luminescence structures

Semiconductor quantum dots (QDs) with circularly polarized luminescence (CPL) characteristics hold significant promise for a range of applications, including information security, three-dimensional (3D) display, quantum computing, and spintronics. Recent approaches combining QDs with chiral liquid crystal assemblies have demonstrated amplified CPL performance (specifically, luminescence dissymmetry factor, g_lum > 10^–1). However, the inherent fluidity and alignment sensitivity of chiral liquid crystals, along with QD aggregation and phase separation, continue to hinder the uniformity and long-term stability of these systems. In this work, we developed an in-situ helical co-assembly polymerization strategy that covalently incorporated InP-based QDs into chiral liquid crystal polymer templates, forming QD-based polymeric superhelical structures. We synthesized high-quality InP/ZnSeS/ZnS QDs and functionalized their surfaces with polymerizable groups to enable reactivity. By precisely tuning the photonic bandgap of the chiral liquid crystal polymers, we achieved chiral parented templates with high chiroptical activity overlapping full-visible-spectrum. Through covalent crosslinking with the QDs, a polymer network was formed, resulting in a maximum g_lum of 1.0. This polymerization-with-assembly approach offers exceptionally flexible and precise control over both the composition and architecture of superhelical materials, paving the way for high-quality CPL materials with broad applications in advanced technologies.