Chiral Polymer Dots Show Unexpected Versatility of Highly Ordered Self‐Assembly into Chiroptical Liquid Crystals, Ultra‐Thin Films, and Long‐Ribbons

Abstract Compared to the organic counterparts, chiral self‐assembly of nanomaterials shows persistency to kinetic factors such as solvent environments, and consequently, dynamic modulation of self‐assembly and functions remains major challenge. Here, it is shown that alkylated, chiral polymer dots (c‐PDs) give highly ordered self‐assemblies with amplified chirality adaptive to solvent environments, and one‐to‐many hierarchical aggregation can be realized. The c‐PDs tended to self‐assemble into nanohelices with cubic packing in the solid state, which, thanks to the thermo‐responsiveness, transformed into thermic liquid crystals upon heating. Cotton effects and circularly polarized luminescence evidenced the chirality transfer from central chirality to supramolecular chirality. At the air‐water interface, the c‐PDs are self‐assembled into monolayers, which further stack into multiple layers with chirality transfer and highly ordered packing. In addition, undergoing a good/poor solvent exchange, the c‐PDs afforded ultra‐long microribbons up to a length scale of millimeters, which are constituted by the bilayer lamellar stacking. The versatile chiral self‐assembly modalities with long‐range ordered packing arrays of carbonized c‐PDs via solvent strategy are realized. This feature is comparable to the organic species, although the c‐PDs have no atomic precise structures. This work would surely expand the applications of quantum dot ordered self‐assembly with adaptiveness to kinetic factors.