Fragility and correlated dynamics in supercooled liquids

A Banerjee and DJ Wales, JOURNAL OF CHEMICAL PHYSICS, 153, 124501 (2020).

DOI: 10.1063/5.0015091

A connection between the super-Arrhenius behavior of dynamical properties and the correlated dynamics for supercooled liquids is examined for a well known glass forming binary Lennard-Jones mixture and its repulsive counterpart, the Weeks-Chandler-Andersen potential, over a range of densities. When considering short time nonergodic trajectory segments of a longer ergodic trajectory, we observe that, independent of the potentials and densities, the apparent diffusivity follows Arrhenius behavior until low temperatures. Comparing the two potentials, where the ergodic diffusivities are known to be rather different, we find that the short-time nonergodic part is similar throughout the temperature range. By including a correlation factor in the nonergodic diffusivity, a rescaled value is calculated, which provides a reasonable estimate of the true ergodic diffusivity. The true diffusion coefficient and the correction factor collapse to a master plot for all densities at any given time interval. Hence, our results confirm a strong connection between fragility and dynamical correlation. Published under license by AIP Publishing.

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