Finite-size effects in the dynamics of glass-forming liquids

被引:74
作者
Berthier, Ludovic [1 ,2 ]
Biroli, Giulio [3 ,4 ]
Coslovich, Daniele [1 ,2 ]
Kob, Walter [1 ,2 ]
Toninelli, Cristina [5 ,6 ]
机构
[1] CNRS, UMR 5221, Lab Charles Coulomb, Montpellier, France
[2] Univ Montpellier 2, Montpellier, France
[3] CEA, Inst Phys Theor IPhT, F-91191 Gif Sur Yvette, France
[4] CNRS, URA 2306, F-91191 Gif Sur Yvette, France
[5] Univ Paris 06, CNRS, UMR 7599, Lab Probabil & Modeles Aleatoires, F-75252 Paris 05, France
[6] Univ Paris 07, F-75252 Paris 05, France
来源
PHYSICAL REVIEW E | 2012年 / 86卷 / 03期
关键词
MODE-COUPLING-THEORY; KINETIC ISING-MODEL; MOLECULAR-DYNAMICS; SUPERCOOLED LIQUIDS; SPATIAL CORRELATIONS; TIME SCALES; TRANSITION; LENGTH; LATTICE; SIMULATIONS;
D O I
10.1103/PhysRevE.86.031502
中图分类号
O35 [流体力学]; O53 [等离子体物理学];
学科分类号
070204 ; 080103 ; 080704 ;
摘要
We present a comprehensive theoretical study of finite-size effects in the relaxation dynamics of glass-forming liquids. Our analysis is motivated by recent theoretical progress regarding the understanding of relevant correlation length scales in liquids approaching the glass transition. We obtain predictions both from general theoretical arguments and from a variety of specific perspectives: mode-coupling theory, kinetically constrained and defect models, and random first-order transition theory. In the last approach, we predict in particular a nonmonotonic evolution of finite-size effects across the mode-coupling crossover due to the competition between mode-coupling and activated relaxation. We study the role of competing relaxation mechanisms in giving rise to nonmonotonic finite-size effects by devising a kinetically constrained model where the proximity to the mode-coupling singularity can be continuously tuned by changing the lattice topology. We use our theoretical findings to interpret the results of extensive molecular dynamics studies of four model liquids with distinct structures and kinetic fragilities. While the less fragile model only displays modest finite-size effects, we find a more significant size dependence evolving with temperature for more fragile models, such as Lennard-Jones particles and soft spheres. Finally, for a binary mixture of harmonic spheres we observe the predicted nonmonotonic temperature evolution of finite-size effects near the fitted mode-coupling singularity, suggesting that the crossover from mode-coupling to activated dynamics is more pronounced for this model. Finally, we discuss the close connection between our results and the recent report of a nonmonotonic temperature evolution of a dynamic length scale near the mode-coupling crossover in harmonic spheres.
引用
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页数:17
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