Quantification of Optical Chirality in Cellulose Nanocrystal Films Prepared by Shear-Coating

Evaporation-induced-self-assembly is widely used to produce chiral cellulose nanocrystal (CNC) free-standing films reflecting left-handed polarized light. Research on supported chiral CNC films is rather scarce. The reflection and/or transmission of unpolarized light are the most common optical techniques used to characterize the selective reflection of CNC films whereas the use of techniques to quantify chiral properties is limited. Here, the fabrication of chiral CNC films supported on glass substrates by a shear-coating method, as well as a full characterization of their polarization properties, are reported. Optical chirality is evidenced in films, showing a brilliant blue structural color when viewed through a left-handed polarizer and darkness through a right-handed polarizer. Mueller-matrix data in the reflection and transmission modes are used to quantitatively characterize the structural origin of color in the films. The quantification of the linear and circular birefringence, as well as circular dichroism, is performed by analytical inversion of the Mueller matrix data in the transmission mode and regression analysis using Tellegen constitutive equations. The equivalence of the two methods to quantify the structural chirality in CNC films is demonstrated. The swelling of films in water and kinetics during drying is studied by reflection spectroscopy.