Anomalous structure and dynamics of the Gaussian-core fluid

Abstract

It is known that there are thermodynamic states for which the Gaussian-core (GC) fluid displays anomalous properties such as expansion upon isobaric cooling (density anomaly) and increased single-particle mobility upon isothermal compression (self-diffusivity anomaly). We investigate how temperature and density affect its short-range translational structural order, as characterized by the two-body excess entropy. We find that there is a wide range of conditions for which the short-range translational order of the GC fluid decreases upon isothermal compression (structural order anomaly). The origin of the structural anomaly is qualitatively similar to that of other anomalous fluids and is connected to how compression affects static correlations at different length scales. We find that the self-diffusivity of the GC fluid obeys a scaling relationship with the two-body excess entropy that is very similar to the one observed for a variety of simple liquids. One consequence of this relationship is that the state points for which structural, self-diffusivity, and density anomalies of the Gaussian-core fluid occur appear as cascading regions on the temperature-density plane, a phenomenon observed earlier for models of waterlike fluids. There are, however, key differences between the anomalies of GC and waterlike fluids, and we discuss how those can be qualitatively understood by considering the respective interparticle potentials of these models. Finally, we note that the self-diffusivity of the Gaussian-core fluid obeys different scaling laws depending on whether the two-body or total excess entropy is considered. This finding, which deserves more comprehensive future study, appears to underscore the significance of higher-body correlations for the behavior of fluids with bounded interactions.

6 pages, 3 figures

References in corpus (26)

• Molecular structural order and anomalies in liquid silica
• Fluid and solid phases of the Gaussian core model
• Evaluating the Surface Tension Using Grand Canonical Transition Matrix Monte Carlo and Finite-Size Scaling
• Excess entropy, Diffusivity and Structural Order in liquids with water-like anomalies
• Thermodynamics and Dynamics of the Two-Scale Spherically-Symmetric Jagla Model of Anomalous Liquids
• Thermodynamic and dynamic anomalies for a three dimensional isotropic core-softened potential
• Phase diagram of the Gaussian-core model
• Structural Order for One-Scale and Two-Scale Potentials
• Thermodynamics predicts how confinement modifies hard-sphere dynamics
• Water-like hierarchy of anomalies in a continuous spherical shouldered potential
• Structure of the First and Second Neighbor Shells of Water: Quantitative Relation with Translational and Orientational Order
• Structural anomalies for a three dimensional isotropic core-softened potential
• A Family of Tunable Spherically-Symmetric Potentials that Span the Range from Hard Spheres to Water-like Behavior
• Static and Dynamic Anomalies in a Repulsive Spherical Ramp Liquid: Theory and Simulation
• Relationship between thermodynamics and dynamics of supercooled liquids
• Does confining the hard-sphere fluid between hard walls change its average properties?
• Tuning density profiles and mobility of inhomogeneous fluids
• How short-range attractions impact the structural order, self-diffusivity, and viscosity of a fluid
• Structural anomalies of fluids: Origins in second and higher coordination shells
• Interplay between structure and density anomaly for an isotropic core-softened ramp-like potential
• Entropy-based measure of structural order in water
• Thermodynamic and Dynamic Anomalies for Dumbbell Molecules Interacting with a Repulsive Ramp-Like Potential
• Gaussian core model phase diagram and pair correlations in high Euclidean dimensions
• Cofinement, entropy, and single-particle dynamics of equilibrium hard-sphere mixtures
• Diffusion Anomaly in an Associating Lattice Gas Model
• Long-time self-diffusion of Brownian Gaussian-core particles

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• Long Distance Correlations in Molecular Orientations of Liquid Water and Shape Dependant Hydrophobic Force
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• Testing the isomorph invariance of the bridge functions of Yukawa one-component plasmas. I. Intermediate and long range
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• Thermodynamics and Structural Properties of the High Density Gaussian Core Model
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