Exploring the Circular Polarization Capacity from Chiral Cellulose Nanocrystal Films for a Photo‐Controlled Chiral Helix of Supramolecular Polymers

Abstract Circularly polarized light (CPL) is key to asymmetric photochemistry as it could impart the chiral organization information into chemical products. Here, we demonstrate the circular polarization capacity of chiral cellulose nanocrystal (CNC) films to trigger photo‐alignment of achiral supramolecular polymers into helical structures. Right‐handed transmitted (T‐) CPL was generated from self‐assembled CNC films, which induced amorphous azobenzene (Azo) supramolecular polymers into chiral structures. The chiral induction effect of T‐CPL is enhanced on Azo polymers with longer spacers. The absorptive dissymmetry factor ( g abs ) values of liquid‐crystal supramolecular polymers can be amplified significantly (over 10 times) after T‐CPL irradiation. Moreover, by integrating carbon dots into CNC films, CPL emission with a considerable luminescence dissymmetry factor ( g lum ) up to −0.66 was achieved, and it could be used for the photo‐alignment of Azo polymers with high chiroptical properties. This work provides new insight for the photo modulation of supramolecular polymers by CPL‐active materials.