Dynamic arrest of colloids in porous environments: disentangling crowding and confinement

Abstract

Using numerical simulations we study the slow dynamics of a colloidal hard-sphere fluid adsorbed in a matrix of disordered hard-sphere obstacles. We calculate separately the contributions to the single-particle dynamic correlation functions due to free and trapped particles. The separation is based on a Delaunay tessellation to partition the space accessible to the centres of fluid particles into percolating and disconnected voids. We find that the trapping of particles into disconnected voids of the matrix is responsible for the appearance of a nonzero long-time plateau in the single-particle intermediate scattering functions of the full fluid. The subdiffusive exponent $z$, obtained from the logarithmic derivative of the mean-squared displacement, is observed to be essentially unaffected by the motion of trapped particles: close to the percolation transition, we determined $z\simeq 0.5$ for both the full fluid and the particles moving in the percolating void. Notably, the same value of $z$ is found in single-file diffusion and is also predicted by mode-coupling theory along the diffusion-localisation line. We also reveal subtle effects of dynamic heterogeneity in both the free and the trapped component of the fluid particles, and discuss microscopic mechanisms that contribute to this phenomenon.

arXiv comment18 pages, 12 figures, minor changes

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• Investigating amorphous order in stable glasses by random pinning
• Nonergodicity parameters of confined hard-sphere glasses
• Dynamic heterogeneities and non-Gaussian behavior in two-dimensional randomly confined colloidal fluids
• Microscopic models of mode-coupling theory: the $F_{12}$ scenario
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• Dynamics of fluids in quenched-random potential energy landscapes: a mode-coupling theory approach
• Diffusion of hard sphere fluids in disordered porous media: Enskog theory description
• Deformable hard particles particles confined in a disordered porous matrix
• On the diffusion of hard sphere fluids in disordered porous media: New extended Enskog theory description
• Finite-size effects in the diffusion dynamics of a glass-forming binary mixture with large size ratio