Time-dependent four-point density correlation functions in supercooled liquids

Details Time-dependent four-point density correlation functions in supercooled liquids Time-dependent four-point density correlation functions in supercooled liquids

1999-09-07

arxiv.org/abs/cond-mat/9909113v3

Physics

Condensed Matter

Soft Condensed Matter

References updated. Inset added to Figure 3

Scientific paper

Dynamical heterogeneity and the decoupling of diffusion and structural relaxation in a supercooled liquid is investigated in terms of a time-dependent, fourth-order density correlation function. The generalized susceptibility $\chi_4(t)$ corresponding to this correlation function has a maximum at an intermediate time $t_4^*$, and both $t_4^*$ and $\chi_4(t_4^*)$ grow strongly with decreasing temperature. We show that the main contribution to $\chi_4(t)$ arises from spatial correlations between temporarily localized (``caged'') particles. We compare $\chi_4(t)$ with a generalized susceptibility $\chi_M(t)$ related to a correlation function of squared particle displacements, and show that while $t_4^*$ is roughly proportional to the $\alpha$-relaxation time, $t_M^*$ is proportional to the inverse of the self-diffusion coefficient.

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