Glassy dynamics of a binary Voronoi fluid: A mode-coupling analysis

TL;DR

This study investigates the glassy dynamics of a binary Voronoi fluid using molecular dynamics simulations and mode-coupling theory, revealing that many-body interactions do not significantly alter the qualitative dynamic behavior compared to simpler models.

Contribution

First detailed analysis of structural relaxation in a many-body Voronoi fluid using MD and MCT, demonstrating predictive power of static correlations despite complex interactions.

Findings

MCT accurately predicts qualitative dynamic features

Wavevector dependence matches polydisperse hard spheres

Critical temperature overestimated by MCT by about 20%

Abstract

The binary Voronoi mixture is a fluid model whose interactions are local and many-body. Here we perform molecular-dynamics (MD) simulations of an equimolar mixture that is weakly polydisperse and additive. For the first time we study the structural relaxation of this mixture in the supercooled-liquid regime. From the simulations we determine the time- and temperature-dependent scattering functions for a large range of wave vectors, as well as the mean-square displacements of both particle species. We perform a detailed analysis of the dynamics by comparing the MD results with the first-principles-based idealized mode-coupling theory (MCT). To this end, we employ two approaches: fits to the asymptotic predictions of the theory, and fit-parameter-free binary MCT calculations based on static-structure-factor input from the simulations. We find that many-body interactions of the Voronoi mixture do not lead to strong qualitative differences relative to similar analyses carried out for simple liquids with pair-wise interactions. For instance, the fits give an exponent parameter $\lambda \approx 0.746$ comparable to typical values found for simple liquids, the wavevector dependence of the Kohlrausch relaxation time is in good agreement with literature results for polydisperse hard spheres, and the MCT calculations based on static input overestimate the critical temperature, albeit only by a factor of about 1.2. This overestimation appears to be weak relative to other well-studied supercooled-liquid models such as the binary Kob--Andersen Lennard-Jones mixture. Overall, the agreement between MCT and simulation suggests that it is possible to predict several microscopic dynamic properties with qualitative, and in some cases near-quantitative, accuracy based solely on static two-point structural correlations, even though the system itself is inherently governed by many-body interactions.