Self-induced heterogeneity in deeply supercooled liquids
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A theoretical treatment of deeply supercooled liquids is difficult because their properties emerge from spatial inhomogeneities that are self-induced, transient, and nanoscopic. I use computer simulations to analyse self-induced static and dynamic heterogeneity in equilibrium systems approaching the experimental glass transition. I characterise the broad sample-to-sample fluctuations of salient dynamic and thermodynamic properties in elementary mesoscopic systems. Findings regarding local lifetimes and distributions of dynamic heterogeneity are in excellent agreement with recent single molecule studies. Surprisingly broad thermodynamic fluctuations are also found, which correlate well with dynamics fluctuations, thus providing a local test of the thermodynamic origin of slow dynamics.
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Cited by 2 Pith papers
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Non-Maxwellian Velocity Statistics in Supercooled Liquids and Their Possible Relation to Super-Arrhenius Viscosity
Supercooled liquids exhibit persistent non-Maxwellian velocity distributions with excess kurtosis 0<κ≲0.3 linked via temperature fluctuation width A_bar≈0.08 to super-Arrhenius viscosity across 45 glass formers.
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Non-Maxwellian Velocity Statistics in Supercooled Liquids and Their Possible Relation to Super-Arrhenius Viscosity
Supercooled liquids exhibit persistent non-Maxwellian velocity distributions with excess kurtosis linked to temperature fluctuation width A-bar ~0.08, consistent with viscosity data collapse across 45 glass formers.
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