Excess-entropy scaling in supercooled binary mixtures

被引:55
作者
Bell, Ian H. [1 ]
Dyre, Jeppe C. [2 ]
Ingebrigtsen, Trond S. [2 ]
机构
[1] NIST, Appl Chem & Mat Div, Boulder, CO 80305 USA
[2] Roskilde Univ, Dept Sci & Environm, Glass & Time, IMFUFA, Postbox 260, DK-4000 Roskilde, Denmark
关键词
STOKES-EINSTEIN RELATION; LENNARD-JONES MIXTURE; MODE-COUPLING THEORY; GLASS-TRANSITION; DENSITY-FLUCTUATIONS; MOLECULAR-DYNAMICS; SELF-DIFFUSION; VISCOSITY; LIQUID; POLYDISPERSITY;
D O I
10.1038/s41467-020-17948-1
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Transport coefficients, such as viscosity or diffusion coefficient, show significant dependence on density or temperature near the glass transition. Although several theories have been proposed for explaining this dynamical slowdown, the origin remains to date elusive. We apply here an excess-entropy scaling strategy using molecular dynamics computer simulations and find a quasiuniversal, almost composition-independent, relation for binary mixtures, extending eight orders of magnitude in viscosity or diffusion coefficient. Metallic alloys are also well captured by this relation. The excess-entropy scaling predicts a quasiuniversal breakdown of the Stokes-Einstein relation between viscosity and diffusion coefficient in the supercooled regime. Additionally, we find evidence that quasiuniversality extends beyond binary mixtures, and that the origin is difficult to explain using existing arguments for single-component quasiuniversality. Supercooled liquids near the glass transition show remarkable non-Arrhenius transport phenomena, whose origin is yet to be clarified. Here, the authors use GPU molecular dynamics simulations for various binary mixtures in the supercooled regime to show the validity of a quasiuniversal excess-entropy scaling relation for viscosity and diffusion.
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页数:12
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