English

Glassy dynamics of sticky hard spheres beyond the mode-coupling regime

Soft Condensed Matter 2021-08-26 v1 Statistical Mechanics

Abstract

Sticky hard spheres, i.e., hard particles decorated with a short-ranged attractive interaction potential, constitute a relatively simple model with highly non-trivial glassy dynamics. The mode-coupling theory of the glass transition (MCT) offers a qualitative account of the complex reentrant dynamics of sticky hard spheres, but the predicted glass transition point is notoriously underestimated. Here we apply an improved first-principles-based theory, referred to as generalized mode-coupling theory (GMCT), to sticky hard spheres. This theoretical framework seeks to go beyond MCT by hierarchically expanding the dynamics in higher-order density correlation functions -- an approach that may become exact if sufficiently many correlations are taken into account. We predict the phase diagrams from the first few levels of the GMCT hierarchy and the dynamics-related critical exponents, all of which are much closer to the empirical observations than MCT. Notably, the prominent reentrant glassy dynamics, the glass-glass transition, and the higher-order bifurcation singularity classes (A3A_3 and A4A_4) of sticky hard spheres are found to be preserved within GMCT at arbitrary order. Moreover, we demonstrate that when the hierarchical order of GMCT increases, the effect of the short-ranged attractive interactions becomes more evident in the dynamics. This implies that GMCT is more sensitive to subtle microstructural differences than MCT, and that the framework provides a promising first-principles approach to systematically go beyond the MCT regime.

Keywords

Cite

@article{arxiv.2105.06417,
  title  = {Glassy dynamics of sticky hard spheres beyond the mode-coupling regime},
  author = {Chengjie Luo and Liesbeth M. C. Janssen},
  journal= {arXiv preprint arXiv:2105.06417},
  year   = {2021}
}

Comments

Invited contribution for the Soft Matter Emerging Investigators 2021 issue