Equilibration and aging of dense soft-sphere glass-forming liquids

Abstract

The recently-developed non-equilibrium extension of the self-consistent generalized Langevin equation theory of irreversible relaxation [Phys. Rev. E (2010) 82, 061503; ibid. 061504] is applied to the description of the irreversible process of equilibration and aging of a glass-forming soft-sphere liquid that follows a sudden temperature quench, within the constraint that the local mean particle density remains uniform and constant. For these particular conditions, this theory describes the non-equilibrium evolution of the static structure factor S(k;t) and of the dynamic properties, such as the self-intermediate scattering function F_S(k,τ;t), where tau is the correlation delay time and t is the evolution or waiting time after the quench. Specific predictions are presented, for the deepest quench (to zero temperature). The predicted evolution of the alpha-relaxation time τ_α(t) as a function of t allows us to define the equilibration time t^{eq}, as the time after which τ_αhas attained its equilibrium value τ_α^{eq}. It is predicted that both, t^{eq}(ϕ) and τ_α^{eq}, diverge as ϕ\to ϕ^{(a)}, where ϕ^{(a)} is the hard-sphere dynamic-arrest volume fraction ϕ^{(a)}\ (\approx 0.582), thus suggesting that the measurement of equilibrium properties at and above ϕ^{(a)} is experimentally impossible.

41 pages, 23 figures

References in corpus (7)

• Probing the equilibrium dynamics of colloidal hard spheres above the mode-coupling glass transition
• The glass transition of dense fluids of hard and compressible spheres
• Dynamic light scattering measurements in the activated regime of dense colloidal hard spheres
• Simplified Self-Consistent Theory of Colloid Dynamics
• Multiple time scales hidden in heterogeneous dynamics of glass-forming liquids
• Overdamped van Hove function of atomic liquids
• First-principles Predictor of the Location of Ergodic-Non-ergodic Transitions

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• Self-consistent generalized Langevin equation theory of the dynamics of multicomponent atomic liquids
• Phase separation and dynamical arrest of protein solutions dominated by short-range attractions
• Non-Equilibrium View of the Amorphous Solidification of Liquids with Competing Interactions
• Structural relaxation, dynamical arrest and aging in soft-sphere liquids
• Non-equilibrium Onsager-Machlup theory
• Spatially heterogeneous dynamics and locally arrested density fluctuations from first-principles
• Dynamics of a suspension of interacting yolk-shell particles