Journal
SCIENCE ADVANCES
Volume 8, Issue 15, Pages -Publisher
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/sciadv.abm7154
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Funding
- Fonds de la Recherche Scientifique FNRS [T.0184.20]
- Action de Recherche Concertee-ULB [ARC 20061]
- Fondation Jaumotte-Demoulin
- China Scholarship Council [CSC 201807565008]
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This study identifies a molecular process known as Slow Mode (SAP) that is universally observed in liquid dynamics of thin films and is closely connected to high-temperature flow. The findings suggest that measurements of liquid dynamics can be used to predict the equilibration rate in the glassy state.
The rate at which a nonequilibrium system decreases its free energy is commonly ascribed to molecular relaxation processes, arising from spontaneous rearrangements at the microscopic scale. While equilibration of liquids usually requires density fluctuations at time scales quickly diverging upon cooling, growing experimental evidence indicates the presence of a different, alternative pathway of weaker temperature dependence. Such equilibration processes exhibit a temperature-invariant activation energy, on the order of 100 kJ mol(-1). Here, we identify the underlying molecular process responsible for this class of Arrhenius equilibration mechanisms with a slow mode (SAP), universally observed in the liquid dynamics of thin films. The SAP, which we show is intimately connected to high-temperature flow, can efficiently drive melts and glasses toward more stable, less energetic states. Our results show that measurements of liquid dynamics can be used to predict the equilibration rate in the glassy state.
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