title: Numerical study of long-time dynamics and ergodic-nonergodic transitions in dense simple fluids.
abstract: Since the mid-1980s, mode-coupling theory (MCT) has been the de facto theoretic description of dense fluids and the transition from the fluid state to the glassy state. MCT, however, is limited by the approximations used in its construction and lacks an unambiguous mechanism to institute corrections. We use recent results from a new theoretical framework--developed from first principles via a self-consistent perturbation expansion in terms of an effective two-body potential--to numerically explore the kinetics of systems of classical particles, specifically hard spheres governed by Smoluchowski dynamics. We present here a full solution for such a system to the kinetic equation governing the density-density time correlation function and show that the function exhibits the characteristic two-step decay of supercooled fluids and an ergodic-nonergodic transition to a dynamically arrested state. Unlike many previous numerical studies--and in stark contrast to experiment--we have access to the full time and wave-number range of the correlation function with great precision and are able to track the solution unprecedentedly close to the transition, covering nearly 15 decades in scaled time. Using asymptotic approximation techniques analogous to those developed for MCT, we fit the solution to predicted forms and extract critical parameters. We find complete qualitative agreement with known glassy behavior (e.g. power-law divergence of the α-relaxation time scale in the ergodic phase and square-root growth of the glass form factors in the nonergodic phase), as well as some limited quantitative agreement [e.g. the transition at packing fraction η*=0.60149761(10)], consistent with previous static solutions under this theory and with comparable colloidal suspension experiments. However, most importantly, we establish that this new theory is able to reproduce the salient features seen in other theories, experiments, and simulations but has the advantages of being derived from first principles and possessing a clear mechanism for making systematic corrections.
authors.affiliation: The James Franck Institute and the Department of Physics, The University of Chicago, Chicago, Illinois 60637, USA.
authors.forename: David D
authors.initials: DD
authors.lastname: McCowan