Collective diffusion of colloidal hard rods in smectic liquid crystals: effect of particle anisotropy

Abstract

We study the layer-to-layer diffusion in smectic-A liquid crystals of colloidal hard rods with different length-to-diameter ratios using computer simulations. The layered arrangement of the smectic phase yields a hopping-type diffusion due to the presence of permanent barriers and transient cages. Remarkably, we detect stringlike clusters composed of interlayer rods moving cooperatively along the nematic director. Furthermore, we find that the structural relaxation in equilibrium smectic phases shows interesting similarities with that of out-of-equilibrium supercooled liquids, although there the particles are kinetically trapped in transient rather than permanent cages. Additionally, at fixed packing fraction we find that the barrier height increases with increasing particle anisotropy, and hence the dynamics is more heterogeneous and non-Gaussian for longer rods, yielding a lower diffusion coefficient along the nematic director and smaller clusters of interlayer particles that move less cooperatively. At fixed barrier height, the dynamics becomes more non-Gaussian and heterogeneous for longer rods that move more collectively giving rise to a higher diffusion coefficient along the nematic director.