Mixture-like behavior near a liquid-liquid phase transition in simulations of supercooled water

Abstract

In simulations of a water-like model (ST2) that exhibits a liquid-liquid phase transition, we test for the occurrence of a thermodynamic region in which the liquid can be modelled as a two-component mixture. We assign each molecule to one of two species based on the distance to its fifth-nearest neighbor, and evaluate the concentration of each species over a wide range of temperature and density. Our concentration data compare well with mixture-model predictions in a region between the liquid-liquid critical temperature and the temperature of maximum density. Fits of the model to the data in this region yield accurate estimates for the location of the critical point. We also show that the liquid outside the region of density anomalies is poorly modelled as a simple mixture.

5 pages, 4 figures; Phys. Rev. Lett., in press (2011)

References in corpus (5)

• Relation Between the Widom line and the Strong-Fragile Dynamic Crossover in Systems with a Liquid-Liquid Phase Transition
• Computer simulations of liquid silica: equation of state and liquid-liquid phase transition
• Observation of the Density Minimum in Deeply Supercooled Confined Water
• Density minimum and liquid-liquid phase transition
• Hierarchies of networked phases induced by multiple liquid-liquid critical points

Cited by in corpus (46)

• Understanding water's anomalies with locally favored structures
• Bond orientational ordering in liquids: Towards a unified description of water-like anomalies, liquid-liquid transition, glass transition, and crystallization
• Two-State Thermodynamics and the Possibility of a Liquid-Liquid Phase Transition in Supercooled TIP4P/2005 Water
• Nature of the anomalies in the supercooled liquid state of the mW model of water
• Free energy surface of ST2 water near the liquid-liquid phase transition
• Reversible structural transformations in supercooled water from 135 to 245 K
• Two-state thermodynamics of the ST2 model for supercooled water
• Crystal nucleation as the ordering of multiple order parameters
• Tuning the liquid-liquid transition by modulating the hydrogen bond angular flexibility in a model for water
• Distinct signature of two local structural motifs of liquid water in the scattering function
• Dynamical Behavior Near a Liquid-Liquid Phase Transition in Simulations of Supercooled Water
• Water-like anomalies as a function of tetrahedrality
• Mass Density Fluctuations in Quantum and Classical descriptions of Liquid Water
• X-ray Diffraction and Molecular Dynamics Study of Medium-range Order in Ambient and Hot Water
• Unravelling the contribution of local structures to the anomalies of water: the synergistic action of several factors
• Thermodynamics of Fluid Polyamorphism
• Thermal Conductivity of Supercooled Water
• The physics of Empty Liquids: from Patchy particles to Water
• Phase diagram of a two-dimensional system with anomalous liquid properties
• Potential Energy Landscape of the Apparent First-Order Phase Transition between Low-Density and High-Density Amorphous Ice
• Phase diagram of the ST2 model of water
• Roles of liquid structural ordering in glass transition, crystallization, and water's anomalies
• Glass Polymorphism in TIP4P/2005 Water: A Description Based on the Potential Energy Landscape Formalism
• Do Machine-Learning Atomic Descriptors and Order Parameters Tell the Same Story? The Case of Liquid Water
• Beyond Local Structures In Critical Supercooled Water Through Unsupervised Learning
• GCIceNet: A Graph Convolutional Network for Accurate Classification of Water Phases
• Diffusion dynamics of supercooled water modeled with the cage-jump motion and hydrogen-bond rearrangement
• Free energy of formation of small ice nuclei near the Widom line in simulations of supercooled water
• Towards a microscopic description of the free-energy landscape of water
• Influence of sample preparation on the transformation of low-density to high-density amorphous ice: An explanation based on the Potential Energy Landscape
• High-density liquid (HDL) adsorption at the supercooled water/vapor interface and its possible relation to the second surface tension inflection point
• A water structure indicator suitable for generic contexts: two-liquid behavior at hydration and nanoconfinement conditions and a molecular approach to hydrophobicity and wetting
• Insight into liquid polymorphism from the complex phase behaviour of a simple model
• Residual entropy and waterlike anomalies in the repulsive one dimensional lattice gas
• Identification of local structures in water from supercooled to ambient conditions
• Thermodynamic metric geometry of the two-state ST2 model for supercooled water
• Topological data analysis for revealing structural origin of density anomalies in silica glass
• Microsecond long atomistic simulation of supercooled water
• The structural order of protein hydration water
• Manifestations of the structural origin of supercooled water's anomalies in the heterogeneous relaxation on the potential energy landscape
• A data driven approach to classify descriptors based on their efficiency in translating noisy trajectories into physically-relevant information
• Hydrogen Bond Topology Reveals Layering of LDL-like and HDL-like Water at its Liquid/Vapor Interface
• Statistical mechanical theory of liquid water
• Low, high and very-high density forms of liquid water revealed by a medium-range order descriptor
• Machine learning evaluation of structural descriptors for supercooled water
• Liquid-Liquid Crossover in Water Model: Local Structure vs. Kinetics of Hydrogen Bonds