Qualitatively different collective and single particle dynamics in a supercooled liquid

TL;DR

This paper develops a nonlinear hydrodynamics model for binary mixtures, revealing that single particle dynamics can remain fluid-like even when collective density fluctuations freeze at the ergodic-nonergodic transition.

Contribution

It introduces a non-perturbative approach showing that tagged particle correlations decay at the ENE transition, contrasting with traditional mode coupling theory predictions.

Findings

Tagged particle correlation decays to zero at ENE transition.

Collective density fluctuations freeze at ENE transition.

Self diffusion constant extrapolation does not indicate the ENE transition.

Abstract

The equations of fluctuating nonlinear hydrodynamics for a two component mixture are obtained with a proper choice of slow variables which correspond to the conservation laws in the system. Using these nonlinear equations we construct the basic equations of the mode coupling theory (MCT) and consequent ergodic-nonergodic (ENE) transition in a binary mixture. The model is also analyzed in the one component limit of the mixture to study the dynamics of a tagged particle in the sea of identical particles. According to the existing MCT, dynamics of the single particle correlation is slaved to that of the collective density fluctuations and hence both correlations freeze simultaneously at the ENE transition. We show here from a non-perturbative approach that at the ENE transition, characterized by the freezing of the long time limit of the dynamic correlation of collective density fluctuations to a nonzero value, the tagged particle correlation still decays to zero. Our result implies that the point at which simulation or experimental data of self diffusion constant extrapolate to zero would not correspond to the ENE transition of simple MCT.