Role of the Lifetime of Dynamical Heterogeneity in the Frequency-Dependent Stokes–Einstein Relation of Supercooled Liquids

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We previously investigated the lifetime of dynamical heterogeneity in supercooled liquids in terms of a four-point, three-time density correlation function via molecular dynamics simulations [Phys. Rev. E 79 (2009) 060501(R); J. Chem. Phys. 133 (2010) 044511]. In this letter, we examine the physical role of the lifetime of dynamicsl heterogeneity in the violation of the Stokes–Einstein (SE) relation by calculating the frequency-dependent viscosity and self-diffusion constant. Our results demonstrate that the SE relation holds up to the time scale at which the non-Gaussian parameter is maximum. Large violations of the SE relation are characterized by time scales longer than the lifetime of the dynamical heterogeneity in highly supercooled liquids.
2010-09-15