Locally preferred structures and many-body static correlations in viscous liquids

Abstract

We investigate the influence of static correlations beyond the pair level on the dynamics of selected model glass-formers. We compare the pair structure, angular distribution functions, and statistics of Voronoi polyhedra of two well-known Lennard-Jones mixtures as well as of the corresponding Weeks-Chandler-Andersen variants, in which the attractive part of the potential is truncated. By means of the Voronoi construction we identify the atomic arrangements corresponding to the locally preferred structures of the models. We find that the growth of domains formed by interconnected locally preferred structures signals the onset of the slow dynamics regime and allows to rationalize the different dynamic behaviors of the models. At low temperature, the spatial extension of the structurally correlated domains, evaluated at fixed relaxation time, increases with the fragility of the models and is systematically reduced by truncating the attractions. In view of these results, proper inclusion of many-body static correlations in theories of the glass transition appears crucial for the description of the dynamics of fragile glass-formers.

9 pages, 8 figures, added two tables, minor revisions to the text

References in corpus (34)

• Testing Mode-Coupling Theory for a Supercooled Binary Lennard-Jones Mixture I: The van Hove Correlation Function
• Theory of Structural Glasses and Supercooled Liquids
• Thermodynamic signature of growing amorphous order in glass-forming liquids
• Coarse-grained microscopic model of glass formers
• Rigorous Inequalities between Length and Time Scales in Glassy Systems
• Understanding fragility in supercooled Lennard-Jones mixtures. I. Locally preferred structures
• Controlling crystallization and its absence: Proteins, colloids and patchy models
• Geometric approach to the dynamic glass transition
• Nonperturbative effect of attractive forces in viscous liquids
• A quantitative test of the mode-coupling theory of the ideal glass transition for a binary Lennard-Jones system
• Decoupling of diffusion from structural relaxation and spatial heterogeneity in a supercooled simple liquid
• A repulsive reference potential reproducing the dynamics of a liquid with attractions
• The Geometry of Slow Structural Fluctuations in a Supercooled Binary Alloy
• Lengthscale dependence of dynamic four-point susceptibilities in glass formers
• Mode-Coupling Theory as a Mean-Field Description of the Glass Transition
• Corresponding States of Structural Glass Formers. II
• Colloidal glass transition: Beyond mode-coupling theory
• A critical test of the mode-coupling theory of the glass transition
• Cooperativity Beyond Caging: Generalized Mode Coupling Theory
• Mean-Field Theory, Mode-Coupling Theory, and the Onset Temperature in Supercooled Liquids
• Order in glassy systems
• Growing static and dynamic length scales in a glass-forming liquid
• Crystallization of the Kob-Andersen binary Lennard-Jones liquid
• Stability of supercooled binary liquid mixtures
• Mode-Coupling as a Landau Theory of the Glass Transition
• Locally preferred structure in simple atomic liquids
• Quantitative tests of mode-coupling theory for fragile and strong glass-formers
• The viscous slowing down of supercooled liquids as a temperature-controlled superArrhenius activated process: a description in terms of frustration-limited domains
• The effect of attractions on the local structure of liquids and colloidal fluids
• Statistical Mechanics and Dynamics of a 3-Dimensional Glass-Forming System
• Understanding fragility in supercooled Lennard-Jones mixtures. II. Potential energy surface
• Idealized glass transitions under pressure: dynamics versus thermodynamics
• An operational scheme to determine the locally preferred structure of model liquids
• Comment on "Correlation between Dynamic Heterogeneity and Medium-Range Order in Two-Dimensional Glass-Forming Liquids"

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