Dynamical density functional theory for dense suspensions of colloidal hard spheres

Abstract

We study structural relaxation of colloidal hard spheres undergoing Brownian motion using dynamical density functional theory. Contrary to the partial linearization route [Stopper {\em et al.}, Phys. Rev. E {\bf 92}, 022151 (2015)] which amounts to using different free energy functionals for the self and distinct part of the van Hove function $G(r,t)$, we put forward a unified description employing a single functional for both components. To this end, interactions within the self part are removed via the zero-dimensional limit of the functional with a quenched self component. In addition, we make use of a theoretical result for the long-time mobility in hard-sphere suspensions, which we adapt to the inhomogeneous fluid. Our results for $G(r,t)$ are in excellent agreement with numerical simulations even in the dense liquid phase. In particular, our theory accurately yields the crossover from free diffusion at short times to the slower long-time diffusion in a crowded environment.

References in corpus (4)

• Density functional theory for hard-sphere mixtures: the White-Bear version Mark II
• Non-equilibrium sedimentation of colloids on the particle scale
• The van Hove distribution function for Brownian hard spheres: dynamical test particle theory and computer simulations for bulk dynamics
• Modeling diffusion in colloidal suspensions by dynamical density functional theory using fundamental measure theory of hard spheres

Cited by in corpus (2)

• Universality in Driven and Equilibrium Hard Sphere Liquid Dynamics
• Superadiabatic forces in the dynamics of the one-dimensional Gaussian core model