Anomalous Dynamic Arrest in a Mixture of Big and Small Particles

Abstract

We present molecular dynamics simulations on the slow dynamics of a mixture of big and small soft-spheres with a large size disparity. Dynamics are investigated in a broad range of temperature and mixture composition. As a consequence of large size disparity, big and small particles exhibit very different relaxation times. As previously reported for simple models of short-ranged attractive colloids and polymer blends, several anomalous dynamic features are observed: i) sublinear behavior for mean squared displacements, ii) concave-to-convex crossover for density-density correlators, by varying temperature or wavevector, iii) logarithmic decay for specific wavevectors of density-density correlators. These anomalous features are observed over time intervals extending up to four decades, and strongly resemble predictions of the Mode Coupling Theory (MCT) for state points close to higher-order MCT transitions, which originate from the competition between different mechanisms for dynamic arrest. For the big particles we suggest competition between soft-sphere repulsion and depletion effects induced by neighboring small particles. For the small particles we suggest competition between bulk-like dynamics and confinement, respectively induced by neighboring small particles and by the slow matrix of big particles. By increasing the size disparity, a new relaxation scenario arises for the small particles. Self-correlators decay to zero at temperatures where density-density correlations are frozen. The behavior of the latters resembles features characteristic of type-A MCT transitions, defined by a zero value of the critical non-ergodicity parameter.