Structural Color Out of the Blue: A Quantitative Framework for the Self-Assembly Kinetics of Cholesteric Cellulosic Mesophases

• Published in: Biomacromolecules 2024-08, Vol.25 (8), p.4977-4990
• Main Authors: Fine, Simona G., Branovsky, Sara E., Chazot, Cécile A. C.
• Format: Article
• Language: English
• ISSN: 1525-7797; 1526-4602; 1526-4602
• DOI: 10.1021/acs.biomac.4c00411

Cholesteric mesophases based on cellulose ethers, such as ethyl cellulose and hydroxypropyl cellulose, have been studied widely for their remarkable ability to display macroscopic structural color. However, the typical time scales involved in the multiscale self-assembly of cholesteric liquid crystals, from individual nanoscale helical arrangements to discrete microscopic domains, and their dependence on the gel’s viscoelastic properties remain underexplored. Here, we establish a quantitative relationship between the kinetics of structural color formation after shear deformation and cholesteric order development at the nano- and microscales. Utilizing rheology in tandem with static and time-resolved reflectivity measurements, we underscore the strong influence of polymer diffusivity and chain elasticity on self-assembly kinetics in cholesteric cellulose ether gels. We show that our phenomenological model can be employed to assess the structure–property relationships of multiple polysaccharide systems, elucidating key design guidelines for the development and processing of structurally colored cholesteric mesophases.