Mesoscopic two-point collective dynamics of glass-forming liquids

ZQ Shen and JMY Carrillo and BG Sumpter and YY Wang, JOURNAL OF CHEMICAL PHYSICS, 159, 114501 (2023).

DOI: 10.1063/5.0161866

The collective density-density and hydrostatic pressure-pressure correlations of glass-forming liquids are spatiotemporally mapped out using molecular dynamics simulations. It is shown that the sharp rise of structural relaxation time below the Arrhenius temperature coincides with the emergence of slow, nonhydrodynamic collective dynamics on mesoscopic scales. The observed long-range, nonhydrodynamic mode is independent of wave numbers and closely coupled to the local structural dynamics. Below the Arrhenius temperature, it dominates the slow collective dynamics on length scales immediately beyond the first structural peak in contrast to the well-known behavior at high temperatures. These results highlight a key connection between the qualitative change in mesoscopic two-point collective dynamics and the dynamic crossover phenomenon.

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