Showing papers by "Walter Kob published in 2012"

Non-monotonic temperature evolution of dynamic correlations in glass-forming liquids

Abstract: Glass-forming liquids are generally thought to relax through a collective rearrangement of domains, correlated over a length scale that increases with decreasing temperature. A numerical study now reveals a surprising twist to the story, claiming that relaxation depends non-monotonically on temperature.

Static point-to-set correlations in glass-forming liquids

Abstract: We analyze static point-to-set correlations in glass-forming liquids. The generic idea is to freeze the position of a set of particles in an equilibrium configuration and to perform sampling in the presence of this additional constraint. Qualitatively different geometries for the confining set of particles are considered and a detailed comparison of resulting static and dynamic correlation functions is performed. Our results reveal the existence of static spatial correlations not detected by conventional two-body correlators, which appear to be decoupled from, and shorter-ranged than, dynamical length scales characterizing dynamic heterogeneity. We find that the dynamics slows down dramatically under confinement, which suggests new ways to investigate the glass transition. Our results indicate that the geometry in which particles are randomly pinned is the best candidate to study static correlations.

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

Abstract: 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.

Reply to "Characterizing dynamic length scales in glass-forming liquids"

Abstract: In their Correspondence, Flenner and Szamel compare the temperature dependence of an alternative dynamic length scale, ξ_4, with that of ξ^dyn, which we studied. Using computer simulations of the same system, they conclude that these two length scales have a different temperature dependence. In particular, ξ_4 does...

Spatial correlations in glass-forming liquids across the mode-coupling crossover

Abstract: We discuss a novel approach, the point-to-set correlation functions, that allows to determine relevant static and dynamic length scales in glass-forming liquids. We find that static length scales increase monotonically when the temperature is lowered, whereas the measured dynamic length scale shows a maximum around the critical temperature of mode-coupling theory. We show that a similar non-monotonicity is found in the temperature evolution of certain finite size effects in the relaxation dynamics. These two independent sets of results demonstrate the existence of a change in the transport mechanism when the glass-former is cooled from moderately to deeply supercooled states across the mode-coupling crossover and clarify the status of the theoretical calculations done at the mean field level.