Non-monotonic response of a sheared magnetic liquid crystal to an external field

Abstract

Utilizing molecular dynamics simulations, we report a non-monotonic dependence of the shear stress on the strength of an external magnetic field ($H$) in a liquid-crystalline mixture of magnetic and non-magnetic anisotropic particles. This non-monotonic behavior is in sharp contrast with the well-studied monotonic $H$-dependency of the shear stress in conventional ferrofluids, where the shear stress increases with $H$ until it reaches a saturation value. We relate the origin of this non-monotonicity to the competing effects of particle alignment along the shear-induced direction, on the one hand, and the magnetic field direction, on the other hand. To isolate the role of these competing effects, we consider a two-component mixture composed of particles with effectively identical steric interactions, where the orientations of a small fraction, i.e.\ the magnetic ones, are coupled to the external magnetic field. By increasing $H$ from zero, the orientations of the magnetic particles show a Fr\'{e}ederickz-like transition and eventually start deviating from the shear-induced orientation, leading to an increase in shear stress. Upon further increase of $H$, a demixing of the magnetic particles from the non-magnetic ones occurs which leads to a drop in shear stress, hence creating a non-monotonic response to $H$. Unlike the equilibrium demixing phenomena reported in previous studies, the demixing observed here is neither due to size-polydispersity nor due to a wall-induced nematic transition. Based on a simplified Onsager analysis, we rather argue that it occurs solely due to packing entropy of particles with different shear- or magnetic-field-induced orientations.