Relationship between thermodynamics and dynamics of supercooled liquids

Details Relationship between thermodynamics and dynamics of supercooled liquids Relationship between thermodynamics and dynamics of supercooled liquids

2006-07-18

arxiv.org/abs/cond-mat/0607448v1

Journal of Chemical Physics 125, 076102 (2006)

Physics

Condensed Matter

Statistical Mechanics

to appear in Journal of Chemical Physics

Scientific paper

10.1063/1.2336197

Diffusivity, a measure for how rapidly a fluid self-mixes, shows an intimate, but seemingly fragmented, connection to thermodynamics. On one hand, the "configurational" contribution to entropy (related to the number of mechanically-stable configurations that fluid molecules can adopt) has long been considered key for predicting supercooled liquid dynamics near the glass transition. On the other hand, the excess entropy (relative to ideal gas) provides a robust scaling for the diffusivity of fluids above the freezing point. Here we provide, to our knowledge, the first evidence that excess entropy also captures how supercooling a fluid modifies its diffusivity, suggesting that dynamics, from ideal gas to glass, is related to a single, standard thermodynamic quantity.

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