Shear-thinning of molecular fluids in Couette flow

Abstract

We use non-equilibrium molecular dynamics simulations, the Boltzmann equation, and continuum thermomechanics to investigate and characterize the shear-thinning behavior of molecular fluids undergoing Couette flow, interacting via a Lennard-Jones (LJ) potential. In particular, we study the shear-stress under steady-state conditions and its dependency on fluid density and applied shear-strain rate. Motivated by kinetic theory, we propose a rheological equation of state that fits observed system responses exceptionally well and captures the extreme shear-thinning effect. We notice that beyond a particular strain-rate threshold, the fluid exhibits shear-thinning, the degree of which is dependent on the density and temperature of the system. In addition, we obtain a shear-rate dependent model for the viscosity which matches the well established Cross viscosity model. We demonstrate how this model arises naturally from the Boltzmann equation and possesses an inherent scaling parameter that unifies the rheological properties of the LJ fluid. We compare our model with those in the literature. Finally, we formulate a dissipation function modeling the LJ fluid as a quasilinear fluid.