The non-equilibrium behaviour of concentrated colloidal dispersions is studied by Stokesian Dynamics, a general molecular-dynamics-like technique for simulating particles suspended in a viscous fluid. The simulations are of a suspension of monodisperse Brownian hard spheres in simple shear flow as a function of the Péclet number, Pe, which measures the relative importance of shear and Brownian forces. Three clearly defined regions of behaviour are revealed. There is first a Brownian-motion-dominated regime (Pe ≤ 1) where departures from equilibrium in structure and diffusion are small, but the suspension viscosity shear thins dramatically. When the Brownian and hydrodynamic forces balance (Pe ≈ 10), the dispersion forms a new ‘phase’ with the particles aligned in ‘strings’ along the flow direction and the strings are arranged hexagonally. This flow-induced ordering persists over a range of Pe and, while the structure and diffusivity now vary considerably, the rheology remains unchanged. Finally, there is a hydrodynamically dominated regime (Pe > 200) with a dramatic change in the long-time self-diffusivity and the rheology. Here, as the Péclet number increases the suspension shear thickens owing to the formation of large clusters. The simulation results are shown to agree well with experiment
