Understanding fragility in supercooled Lennard-Jones mixtures. I. Locally preferred structures

Abstract

We reveal the existence of systematic variations of isobaric fragility in different supercooled Lennard-Jones binary mixtures by performing molecular dynamics simulations. The connection between fragility and local structures in the bulk is analyzed by means of a Voronoi construction. We find that clusters of particles belonging to locally preferred structures form slow, long-lived domains, whose spatial extension increases by decreasing temperature. As a general rule, a more rapid growth, upon supercooling, of such domains is associated to a more pronounced super-Arrhenius behavior, hence to a larger fragility.

arXiv comment14 pages, 14 figures, minor revisions, one figure added

References in corpus (20)

• Testing Mode-Coupling Theory for a Supercooled Binary Lennard-Jones Mixture I: The van Hove Correlation Function
• Testing Mode-Coupling Theory for a Supercooled Binary Lennard-Jones Mixture II: Intermediate Scattering Function and Dynamic Susceptibility
• Spatial Correlations of Mobility and Immobility in a Glassforming Lennard-Jones Liquid
• The frustration-based approach of supercooled liquids and the glass transition: a review and critical assessment
• Is the Fragility of a Liquid Embedded in the Properties of its Glass?
• Controlling crystallization and its absence: Proteins, colloids and patchy models
• Scaling of the supercooled dynamics and its relation to the pressure dependences of the dynamic crossover and the fragility of glass-formers
• Tuning of tetrahedrality in a silicon potential yields a series of monatomic (metal-like) glassformers of very high fragility
• Does the interaction potential determine both the fragility of a liquid and the vibrational properties of its glassy state?
• Decoupling of diffusion from structural relaxation and spatial heterogeneity in a supercooled simple liquid
• Disentangling density and temperature effects in the viscous slowing down of glassforming liquids
• Mapping the magic numbers in binary Lennard-Jones clusters
• The favoured cluster structures of model glass formers
• Mean-Field Theory, Mode-Coupling Theory, and the Onset Temperature in Supercooled Liquids
• On the relationship between structure and dynamics in a supercooled liquid
• On the correlation between fragility and stretching in glassforming liquids
• Why liquids are fragile
• Locally preferred structure in simple atomic liquids
• An operational scheme to determine the locally preferred structure of model liquids
• Density effects in a bulk binary Lennard-Jones system

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