Abstract
Dynamical heterogeneity and the decoupling of diffusion and relaxation in a supercooled liquid is investigated via a time-dependent, four-point density correlation function. We show that the main contribution to the corresponding generalized susceptibility χ4(t) in a molecular dynamics simulation of a Lennard-Jones liquid arises from spatial correlations between temporarily localized (“caged”) particles. By comparing χ4(t) with a generalized susceptibility χM(t) related to a correlation function for the squared particle displacements, we demonstrate a connection between dynamical heterogeneity and the decoupling of relaxation and diffusion.
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