Universal Longtime Dynamics in Dense Simple Fluids

TL;DR

This paper investigates the universal long-time dynamics of dense simple fluids near the glass transition, demonstrating that different microscopic dynamics share the same nonergodic states and extending mode-coupling theory with a systematic perturbation approach.

Contribution

It develops a systematic perturbation theory for dense fluids, showing universality of nonergodic states and extending mode-coupling theory beyond phenomenology.

Findings

Nonergodic states are universal across different dynamics.

Higher-order loop corrections do not significantly alter nonergodic parameters.

A systematic perturbation expansion can be constructed for dense fluid dynamics.

Abstract

There appears to be a longtime, very slowly evolving state in dense simple fluids which, for high enough density, approaches a glassy nonergodic state. The nature of the nonergodic state can be characterized by the associated static equilibrium state. In particular, systems driven by Smoluchowski or Newtonian dynamics share the same static equilibrium and nonergodic states. That these systems share the same nonergodic states is a highly nontrivial statement and requires establishing a number of results. In the high-density regime one finds that an equilibrating system decays via a three-step process identified in mode-coupling theory (MCT). For densities greater than a critical density one has time-power-law decay with exponents a and b. There are sets of linear fluctuation dissipation relations (FDRs) which connect the cumulants of these two fields. The form of the FDRs is the same for both Smoluchowski or Newtonian dynamics. While we show this universality of nonergodic states within perturbation theory, we expect it to be true more generally. The nature of the approach to the nonergodic state has been suggested by MCT. It has been a point of contention that MCT is a phenomenological theory and not a systematic theory with prospects for improvement. Recently a systematic theory has been developed. It naturally allows one to calculate self-consistently density cumulants in a perturbation expansion in a pseudo-potential. At leading order one obtains a kinetic kernel quadratic in the density. This is a "one-loop" theory like MCT. At this one-loop level one finds vertex corrections which depend on the three-point equilibrium cumulants. Here we assume these vertex-corrections can be ignored and focus on the higher-order loops. We show that one can sum up all of the loop contributions. The higher-order loops do not change the nonergodic state parameters substantially.