Inversion of Circularly Polarized Luminescence in the Left‐Handed Chitosan‐Templated Co‐assemblies

Abstract Circularly polarized luminescence (CPL) materials are attractive due to their unique applications in fields such as 3D displays, information encryption, and chiroptical switches. Natural biomolecules‐based CPL materials are gaining plenty of attention due to their chiral diversity and sustainability. However, it is still challenging to construct CPL materials with opposite CPL signs from a single natural biomolecule due to its inherent chirality. Here, chiral assemblies with opposite CPL signs using chitosan oligosaccharide (COS) and achiral luminescent dyes are successfully prepared. It is found that COS can serve as a chiral template to induce the ordered assembly of the dyes along the polymer chain through electrostatic attraction interaction. It is demonstrated experimentally that the structural planarity of the dye molecules is crucial for the formation of chiral co‐assemblies. Interestingly, the left‐handed COS‐templated co‐assemblies can emit CPL with opposite handedness, which is controlled by the helicity degree of the co‐assemblies. This study not only deepens the understanding of the complex assembly of natural biomacromolecules but also provides new insights into the design and construction of CPL materials.