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

Glotzer, S. C.; Novikov, V. N.; Schroeder, T. B.

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

Authors

Glotzer, S. C.

Novikov, V. N.

Schroeder, T. B.

Description

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 $χ_4(t)$ corresponding to this correlation function has a maximum at an intermediate time $t_4^*$, and both $t_4^*$ and $χ_4(t_4^*)$ grow strongly with decreasing temperature. We show that the main contribution to $χ_4(t)$ arises from spatial correlations between temporarily localized (``caged'') particles. We compare $χ_4(t)$ with a generalized susceptibility $χ_M(t)$ related to a correlation function of squared particle displacements, and show that while $t_4^*$ is roughly proportional to the $α$-relaxation time, $t_M^*$ is proportional to the inverse of the self-diffusion coefficient.
References updated. Inset added to Figure 3