The role of attractive forces in viscous liquids

Abstract

We present evidence from computer simulation that the slowdown of relaxation of a standard Lennard-Jones glass-forming liquid and that of its reduction to a model with truncated pair potentials without attractive tails is quantitatively and qualitatively different in the viscous regime. The pair structure of the two models is however very similar. This finding, which appears to contradict the common view that the physics of dense liquids is dominated by the steep repulsive forces between atoms, is characterized in detail, and its consequences are explored. Beyond the role of attractive forces themselves, a key aspect in explaining the differences in the dynamical behavior of the two models is the truncation of the interaction potentials beyond a cutoff at typical interatomic distance. This leads us to question the ability of the jamming scenario to describe the physics of glass-forming liquids and polymers.

arXiv comment13 pages, 12 figures

References in corpus (37)

• Jamming at Zero Temperature and Zero Applied Stress: the Epitome of Disorder
• Scaling behavior in the $\beta$-relaxation regime of a supercooled Lennard-Jones mixture
• Mean field theory of hard sphere glasses and jamming
• Dynamics on the Way to Forming Glass: Bubbles in Space-time
• Probing the equilibrium dynamics of colloidal hard spheres above the mode-coupling glass transition
• Thermodynamical Scaling of the Glass Transition Dynamics
• Jamming transitions in amorphous packings of frictionless spheres occur over a continuous range of volume fractions
• The glass transition of dense fluids of hard and compressible spheres
• Scaling out the density dependence of the $\alpha$ relaxation in glassforming polymers
• Strong pressure-energy correlations in van der Waals liquids
• Pressure-energy correlations in liquids. II. Analysis and consequences
• Liquid Limits: The Glass Transition and Liquid-Gas Spinodal Boundaries of Metastable Liquids
• Scaling the alpha-relaxation time of supercooled fragile organic liquids
• Nonperturbative effect of attractive forces in viscous liquids
• Thermodynamic scaling of diffusion in supercooled Lennard-Jones liquids
• Compressing nearly hard sphere fluids increases glass fragility
• Disentangling density and temperature effects in the viscous slowing down of glassforming liquids
• Strong pressure-energy correlations in liquids as a configuration space property: Simulations of temperature down jumps and crystallization
• Pressure-energy correlations in liquids. III. Statistical mechanics and thermodynamics of liquids with hidden scale invariance
• A repulsive reference potential reproducing the dynamics of a liquid with attractions
• Connecting local structure to interface formation: a molecular scale van der Waals theory of nonuniform liquids
• Increasing the density melts ultrasoft colloidal glasses
• Amorphous silica modeled with truncated and screened Coulomb interactions: A molecular dynamics simulation study
• Lengthscale dependence of dynamic four-point susceptibilities in glass formers
• Glass Transition of the Monodisperse Gaussian Core Model
• Locally preferred structures and many-body static correlations in viscous liquids
• Corresponding States of Structural Glass Formers. II
• Influence of the glass transition on the liquid-gas spinodal decomposition
• A critical test of the mode-coupling theory of the glass transition
• Mean-Field Theory, Mode-Coupling Theory, and the Onset Temperature in Supercooled Liquids
• Equivalence of glass transition and colloidal glass transition in the hard-sphere limit
• On the density scaling of liquid dynamics
• Density scaling in viscous liquids: From relaxation times to four-point susceptibilities
• Comment on "Jamming at zero temperature and zero applied stress: The epitome of disorder"
• The effect of attractions on the local structure of liquids and colloidal fluids
• Idealized glass transitions under pressure: dynamics versus thermodynamics
• Equilibrium and non-equilibrium fluctuations in a glass-forming liquid

Cited by in corpus (49)

• Yield Stress Materials in Soft Condensed Matter
• Models and algorithms for the next generation of glass transition studies
• Elastically Cooperative Activated Barrier Hopping Theory of Relaxation in Viscous Fluids. I. General Formulation and Application to Hard Sphere Fluids
• What constitutes a simple liquid?
• Extreme active matter at high densities
• Multiple length and time scales of dynamic heterogeneities in model glass-forming liquids: A systematic analysis of multi-point and multi-time correlations
• The role of structure and entropy in determining differences in dynamics for glass formers with different interaction potentials
• Anomalous glassy dynamics in simple models of dense biological tissue
• Absence of Marginal Stability in a Structural Glass
• Anomalous vibrational properties in the continuum limit of glasses
• Rejuvenation and Memory Effects in a Structural Glass
• Improved reconstructions of random media using dilation and erosion processes
• Attractive versus truncated repulsive supercooled liquids: The dynamics is encoded in the pair correlation function
• Testing "microscopic" theories of glass-forming liquids
• Revealing the Link between Structural Relaxation and Dynamic Heterogeneity in Glass-Forming Liquids
• Microscopic Theory for the Role of Attractive Forces in the Dynamics of Supercooled Liquids
• Nonmonotonic behavior in the dense assemblies of active colloids
• Static triplet correlations in glass-forming liquids: A molecular dynamics study
• Role of the first coordination shell in determining the equilibrium structure and dynamics of simple liquids
• Unraveling the success and failure of mode coupling theory from consideration of entropy
• Approximate scale invariance in particle systems: a large-dimensional justification
• Corroborative evidences of TVgamma-scaling of the alpha-relaxation originating from the primitive relaxation/JG beta relaxation
• Determination of onset temperature from the entropy for fragile to strong liquids
• A Microscopic Theory of Softness in Supercooled Liquids
• Probing the glass transition from structural and vibrational properties of zero-temperature glasses
• Investigating isomorphs with the topological cluster classification
• Effect of total and pair configurational entropy in determining dynamics of supercooled liquids over a range of densities
• Do the repulsive and attractive pair forces play separate roles for the physics of liquids?
• Thermodynamic scaling of dynamics in polymer melts: Predictions from the generalized entropy theory
• Role of attractive forces in the relaxation dynamics of supercooled liquids
• Microscopic Theory of the Influence of Strong Attractive Forces on the Activated Dynamics of Dense Glass and Gel Forming Fluids
• Effect of attractions on correlation length scales in a glass-forming liquid
• Observation and Characterization of the Vestige of the Jamming Transition in a Thermal 3D System
• Shear induced solidification of athermal systems with weak attraction
• Connecting glass-forming ability of binary mixtures of soft particles to equilibrium melting temperatures
• Multi-component generalized mode-coupling theory: Predicting dynamics from structure in glassy mixtures
• Comparing four hard-sphere approximations for the low-temperature WCA melting line
• Tuning Pairwise Potential Can Control the Fragility of Glass-Forming Liquids: From Tetrahedral Network to Isotropic Soft Sphere Models
• Temperature-pressure scaling for air-fluidized grains on approaches to Point J
• A perspective on the fragility of glass-forming liquids
• How attractive and repulsive interactions affect structure ordering and dynamics of glass-forming liquids?
• The correlation between fragility, density and atomic interaction in glass-forming liquids
• Suppressed Density of States in Self-Generated Coulomb Glasses
• The role of the attractive forces in a supercooled liquid
• The potential energy landscape and inherent dynamics of a hard-sphere fluid
• Emergence of cooperatively reorganizing cluster and super-Arrhenius dynamics of fragile supercooled liquids
• To the kinetic theory of dense gases and liquids. Calculation of quasi-equilibrium particle distribution functions by the method of collective variables
• Microscopic Theory of the Elastic Shear Modulus and Length-Scale-Dependent Dynamic Re-Entrancy Phenomena in Very Dense Sticky Particle Fluids
• Structure-Dynamics Correlation and Its Link to Fragility and Dynamic Heterogeneity