Slow dynamics of a tagged particle in a supercooled liquid

Abstract

The ergodicity-nonergodicity (ENE) transition of the self-consistent mode-coupling theory (MCT) is marked by the point at which the time correlation of collective density fluctuations is not zero in the long-time limit. The nonergodic state, reaching beyond the ENE transition of simple MCT, is characterized by a finite shear modulus. The MCT, formulated in the current set of papers, predicts that the single-particle density correlation, unlike the collective density correlation, decays to zero at long times on either side of the ENE transition. The self-diffusion coefficient remains finite. This differs from the existing MCT results in which both collective and single-particle correlations are simultaniously frozen at the ENE transition. We discuss in this paper mechanisms by which a sharp fall in self-diffusion coefficient may occur within the present model. This overdamping or the so-called adiabatic approximation for the supercooled state does not maintain microscopic momentum conservation. Within this approximation, the self-diffusion constant approaches zero at the ENE transition point. This approximate result, which is similar to the prediction of the existing MCT models, further illustrates the process of cage formation with increase of density. At a qualitative level, our analysis shows that the self-diffusion process depends on the structure as well as short-time transport properties of the supercooled liquid. We solve the integral equations for the nonergodicity parameters to analyze the full implications of the adiabatic approximation.