Coupling of long-wavelength density fluctuations to orientations in cellulose nanocrystal suspensions under external fields

Abstract

Motivated by the development of cellulose-based functional materials, we investigate the microscopic dynamics of suspensions of cellulose nanocrystals (CNCs) at different ionic strengths, both in the absence and in the presence of AC electric fields and for various temperatures. A concentration of 5 wt % of the CNCs is chosen for which the dispersions are in the full chiral-nematic state at low ionic strengths. Dynamic light scattering is used to characterize the wave vector-dependent decay rates of number-density fluctuations. Contrary to an isotropic suspension, the dispersion relations (the wave vector dependence of the correlation-function decay rates) as obtained by means of depolarized light scattering are found to exhibit anomalous behavior. The dispersion relations, both without and with an external field, exhibit minima at small wave vectors, which is attributed to coupling of translational motion to the orientation of the CNCs, shown in the chiral-nematic state. The location of the minima is found to weakly depend on ionic strength and shifts significantly towards larger wave vectors upon applying an external electric field for sufficiently high ionic strengths. Finally, preliminary results are presented for smaller length-scale density fluctuations (at larger wave vectors) as a function of temperature, revealing the anisotropic mobilities in the chiral-nematic state of CNCs.