Decoupling of single-particle and collective dynamics in arrested phase-separating glassy mixtures

Abstract

We investigate the structure and dynamics of a hard colloid-star polymer mixture in the range of its arrested phase separation, where an incipient demixing transition is interfering with a nearby vitrification line, focusing on the protein limit (smaller hard component). Soft-hard mixtures present a rich dynamics, influenced by different parameters such as the concentration of the soft and hard components, the softness of the potential, and the size ratio between the two components. Using coarse-grained molecular dynamics simulations, we characterize the single-particle and collective dynamics of the hard colloidal tracers in the soft glassy matrix. The hard tracers show diffusive behavior of the mean squared displacement accompanied by non-exponential relaxation of the intermediate scattering functions at intermediate length scales and non-Gaussian displacement distributions. Moreover, we show that the system exhibits arrested phase separation, leading to population splitting and decoupling between self- and collective dynamics of the hard colloids. Overall, we demonstrate that the interplay between arrested phase separation and glassiness leads to complex, multiscale phenomena that strongly influence the dynamics of the hard additives in the arrested matrix formed by the soft colloids.