Enhanced cooperativity below the caging temperature of glass-forming liquids

Abstract

The utility of a cooperative length scale for describing the dynamics of small molecule glass-formers is shown. Molecular Dynamics and Monte Carlo simulations reveal a distribution of cooperatively moving fractal events below the temperature Ta at which dynamics become caged. Guided by these results, four straightforward methods emerge to recognize Ta in experimental data and quantify the length scale that grows on cooling below Ta. This length scale is consistent with 4-D NMR experiments which are sensitive to the slow moving population.