Dynamic heterogeneities above and below the mode-coupling temperature: Evidence of a dynamic crossover

被引:50
作者
Flenner, Elijah [1 ]
Szamel, Grzegorz [1 ]
机构
[1] Colorado State Univ, Dept Chem, Ft Collins, CO 80523 USA
基金
美国国家科学基金会;
关键词
LENNARD-JONES MIXTURE; GLASS-FORMING LIQUIDS; SUPERCOOLED LIQUIDS; MOLECULAR-DYNAMICS; TRANSITION; RELAXATION; LENGTH; SUSCEPTIBILITY;
D O I
10.1063/1.4773321
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
We examine dynamic heterogeneities in a model glass-forming fluid, a binary harmonic sphere mixture, above and below the mode-coupling temperature T-c. We calculate the ensemble independent susceptibility chi(4)(tau(alpha)) and the dynamic correlation length. 4(tau(alpha)) at the a-relaxation time tau(alpha) a. We also examine in detail the temperature dependence of ta and the diffusion coefficient D. For higher temperatures, we find that the standard Stokes-Einstein relationship, D similar to tau(-1)(alpha) a, holds, but at lower temperatures a fractional Stokes-Einstein relationship, D similar to tau(-sigma)(alpha) a with sigma = 0.65, emerges. By examining the relationships between tau(alpha), D, chi(4)(tau(alpha)), and xi(4)(tau(alpha)) we determine that the emergence of the fractional Stokes-Einstein relationship is accompanied by a dynamic crossover from tau(alpha) similar to e(k2 xi 4) at higher temperatures to tau(alpha) similar to e(k1 xi 3/2) 4 at lower temperatures. (C) 2013 American Institute of Physics. [http://dx.doi.org/10.1063/1.4773321]
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页数:13
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