Nonmonotonic Dynamical Correlations beneath the Surface of Glass-Forming Liquids

Collective motion over increasing length scales is a signature of the vitrification process of liquids. We demonstrate how distinct static and dynamic length scales govern the dynamics of vitrifying films. In contrast to a monotonically growing static correlation length, the dynamical correlation length that measures the extent of surface-dynamics acceleration into the bulk displays a striking nonmonotonic temperature evolution that is robust also against changes in detailed interatomic interaction. This nonmonotonic change defines a crossover temperature T_{*} that is distinct from the critical temperature T_{c} of mode-coupling theory. We connect this nonmonotonic change to a morphological change of cooperative rearrangement regions of fast particles, and to the point where the decoupling of fast-particle motion from the bulk relaxation is most sensitive to fluctuations. We propose a rigorous definition of this new crossover temperature T_{*} within a recent extension of mode-coupling theory, the stochastic β-relaxation theory.