Structural signatures of mobility on intermediate time scales in a supercooled fluid

We use computer simulations to explore the manner in which the particle displacements on intermediate time scales in supercooled fluids correlate to their dynamic structural environment. The fluid we study, a binary mixture of hard spheres, exhibits classic signatures of dynamic heterogeneity, including a bifurcated single-particle displacement distribution (i.e., subpopulations of immobile and mobile particles). We find that immobile particles, during the course of their displacements, exhibit stronger average pair correlations to their neighbors than mobile particles, but not necessarily higher average coordination numbers. We discuss how the correlation between structure and single-particle dynamics depends on observation time.

• Publication year

  2009

• Venue

  Journal of Chemical Physics

• Publication date

  2009-11-01

• Fields of study

  Physics, Chemistry

• Identifiers
  DOI 10.1063/1.3414349arXiv 0911.0213
• External record

  Open on Semantic Scholar

• Source metadata

  Semantic Scholar

• No claims are published for this paper.

• No concepts are published for this paper.

• On the study of collective dynamics in supercooled liquids through the statistics of the isoconfigurational ensemble.

  2009cited by this paper
• Composition and concentration anomalies for structure and dynamics of Gaussian-core mixtures.

  2009cited by this paper
• Generalized Rosenfeld scalings for tracer diffusivities in not-so-simple fluids: mixtures and soft particles.

  2009cited by this paper
• Large-amplitude jumps and non-Gaussian dynamics in highly concentrated hard sphere fluids.

  2008cited by this paper
• Study of spatial correlations in a supercooled molecular system.

  2008cited by this paper
• Correlation between dynamic heterogeneity and medium-range order in two-dimensional glass-forming liquids.

  2007cited by this paper
• Dynamical fluctuation effects in glassy colloidal suspensions

  2007cited by this paper
• Structure and dynamics of glass formers: predictability at large length scales.

  2007cited by this paper
• Non-Gaussian effects, space-time decoupling, and mobility bifurcation in glassy hard-sphere fluids and suspensions.

  2006cited by this paper
• Colloidal glass transition observed in confinement.

  2006cited by this paper
• Thermodynamics predicts how confinement modifies the dynamics of the equilibrium hard-sphere fluid.

  2006cited by this paper
• Dynamical heterogeneities in an attraction driven colloidal glass

  2005cited by this paper
• Free volume cannot explain the spatial heterogeneity of Debye–Waller factors in a glass-forming binary alloy

  2005cited by this paper
• Molecular dynamics studies of heterogeneous dynamics and dynamic crossover in supercooled atomic liquids.

  2005cited by this paper
• On the relationship between structure and dynamics in a supercooled liquid

  2005cited by this paper
• Predicting the long-time dynamic heterogeneity in a supercooled liquid on the basis of short-time heterogeneities.

  2005cited by this paper
• Nature of the breakdown in the Stokes-Einstein relationship in a hard sphere fluid.

  2005cited by this paper
• How reproducible are dynamic heterogeneities in a supercooled liquid?

  2004cited by this paper
• Theory and simulation of gelation, arrest and yielding in attracting colloids

  2004cited by this paper
• Spatially heterogeneous dynamics and dynamic facilitation in a model of viscous silica.

  2004cited by this paper
• Comparison of dynamical heterogeneity in hard-sphere and attractive glass formers.

  2004cited by this paper
• Spatially heterogeneous dynamics in supercooled liquids.

  2003cited by this paper
• Spatially heterogeneous dynamics investigated via a time-dependent four-point density correlation function

  2003cited by this paper
• Glassy dynamics of kinetically constrained models

  2002cited by this paper
• Heterogeneous dynamics in liquids: fluctuations in space and time

  2002cited by this paper
• Spatially correlated dynamics in a simulated glass-forming polymer melt: analysis of clustering phenomena.

  2001cited by this paper
• Universal scaling laws of diffusion in a binary fluid mixture.

  2001cited by this paper
• Properties of cage rearrangements observed near the colloidal glass transition.

  2001cited by this paper
• Direct observation of dynamical heterogeneities in colloidal hard-sphere suspensions

  2000cited by this paper
• Direct observation of molecular cooperativity near the glass transition

  2000cited by this paper
• Relaxation in glassforming liquids and amorphous solids

  2000cited by this paper
• Time-dependent, four-point density correlation function description of dynamical heterogeneity and decoupling in supercooled liquids

  2000cited by this paper
• Towards a quantification of disorder in materials: distinguishing equilibrium and glassy sphere packings

  2000cited by this paper
• Spatially heterogeneous dynamics in liquids: insights from simulation

  2000cited by this paper
• Three-dimensional direct imaging of structural relaxation near the colloidal glass transition

  2000cited by this paper
• A quasi-universal scaling law for atomic transport in simple fluids

  1999cited by this paper
• The Origin of Anomalous Diffusion and Non-Gaussian Effects for Hard Spheres: Analysis of Three-Time Correlations

  1999cited by this paper
• Dynamics of highly supercooled liquids: Heterogeneity, rheology, and diffusion

  1998cited by this paper
• Spatial correlations of mobility and immobility in a glass-forming Lennard-Jones liquid.

  1998cited by this paper
• Heterogeneous Diffusion in Highly Supercooled Liquids

  1998cited by this paper
• DYNAMICAL HETEROGENEITIES IN A SUPERCOOLED LENNARD-JONES LIQUID

  1997cited by this paper
• STRINGLIKE COOPERATIVE MOTION IN A SUPERCOOLED LIQUID

  1997cited by this paper
• Consequences of kinetic inhomogeneities in glasses.

  1996cited by this paper
• A universal scaling law for atomic diffusion in condensed matter

  1996cited by this paper
• BREAKDOWN OF THE STOKES-EINSTEIN RELATION IN SUPERCOOLED LIQUIDS

  1995cited by this paper
• Translation-rotation paradox for diffusion in fragile glass-forming liquids.

  1994cited by this paper

• Thermodynamic Insights into Variation in Thermomechanical and Physical Properties of Isotactic Polypropylene: Effect of Shear and Cooling Rates

  2023cites this paper
• Exploring the relationship between softness and excess entropy in glass-forming systems.

  2023cites this paper
• Universal Relation between Entropy and Kinetics.

  2022cites this paper
• On the Relation between Entropy and Kinetics

  2022cites this paper
• Heterogeneous Dynamics in [BMIM][PF6] + Cosolvent Binary Mixtures: Does It Depend Upon Cosolvent Polarity?

  2021cites this paper
• Pathway of orientational symmetry breaking in crystallization of short n-alkane droplets: A molecular dynamics study.

  2020cites this paper
• Scaling of relaxation and excess entropy in plastically deformed amorphous solids

  2020cites this paper
• The Tough Journey of Polymer Crystallization: Battling with Chain Flexibility and Connectivity

  2019cites this paper
• Fifty years of fragility: A view from the cheap seats

  2019cites this paper
• Excess-entropy scaling

  2018cites this paper
• Perspective: Excess-entropy scaling.

  2018cites this paper
• Structural predictor for nonlinear sheared dynamics in simple glass-forming liquids

  2017cites this paper
• Composition Dependence of Dynamic Heterogeneity Time- and Length Scales in [Omim][BF4]/Water Binary Mixtures: Molecular Dynamics Simulation Study.

  2015cites this paper
• Structural correlations and cooperative dynamics in supercooled liquids.

  2012cites this paper
• Roles of bond orientational ordering in glass transition and crystallization

  2011cites this paper
• Bond orientational ordering in a metastable supercooled liquid: a shadow of crystallization and liquid–liquid transition

  2010cites this paper
• Excess entropy scaling of dynamic quantities for fluids of dumbbell-shaped particles.

  2010cites this paper