相关论文: The Free Energy Surface of Supercooled Water

We review the available experimental information on the thermodynamic properties of supercooled ordinary and heavy water and demonstrate the possibility of modeling these thermodynamic properties on a theoretical basis. We show that by…

We use numerical simulation to examine the possibility of a reversible liquid-liquid transition in supercooled water and related systems. In particular, for two atomistic models of water, we have computed free energies as functions of…

Starting for the Stillinger and Weber expression for the free energy of supercooled liquids, we extend the free energy to the case in which two time scales separate and the system is in quasi-equilibrium. The concept of an effective…

This paper extends our earlier studies of free energy functions of density and crystalline order parameters for models of supercooled water, which allows us to examine the possibility of two distinct metastable liquid phases [J. Chem. Phys.…

We carry out umbrella sampling Monte Carlo simulations to evaluate the free energy surface of the ST2 model of water as a function two order parameters, the density and a bond-orientational order parameter. We approximate the long-range…

We have developed a scaled parametric equation of state to describe and predict thermodynamic properties of supercooled water. The equation of state, built on the growing evidence that the critical point of supercooled liquid-liquid water…

We evaluate the free energy of the fluid and crystal phases for the ST2 potential [F.H. Stillinger and A. Rahman, J. Chem. Phys. 60, 1545 (1974)] with reaction field corrections for the long-range interactions. We estimate the phase…

The existence of a first-order phase transition between a low-density liquid (LDL) and a high-density liquid (HDL) forms of supercooled water has been a central and highly debated issue of physics and chemistry in the last three decades. We…

Twenty years ago Poole et al. (Nature 360, 324, 1992) suggested that the anomalous properties of supercooled water may be caused by a critical point that terminates a line of liquid-liquid separation of lower-density and higher-density…

Relations between the thermodynamics and dynamics of supercooled liquids approaching a glass transition have been proposed over many years. The potential energy surface of model liquids has been increasingly studied since it provides a…

A novel liquid-liquid phase transition has been proposed and investigated in a wide variety of pure substances recently, including water, silica and silicon. From computer simulations using the Stillinger-Weber classical empirical…

The existence of a phase transition between two distinct liquid phases in single-component network-forming liquids (e.g., water, silica, silicon) has elicited considerable scientific interest. The challenge, both for experiments and…

We introduce a model of water contemplating true supercooled-liquid states that, as such, are metastable with respect to the crystalline-solid ones. Its numerical solutions reproduce from Speedy-Angell's stability-limit picture to Poole et…

Liquid-liquid and liquid-vapor coexistence regions of various water models were determined by MC simulations of isotherms of density fluctuation restricted systems and by Gibbs ensemble MC simulations. All studied water models show multiple…

To study the possibility of a fluid-fluid phase transition, we analyze a three-dimensional soft-core isotropic potential for a one-component system. We utilize two independent numerical approaches, (i) integral equation in the…

We study the kinetics of crystallization in deeply supercooled liquid silicon employing computer simulations and the Stillinger-Weber three body potential. The free energy barriers to crystallisation are computed using umbrella sampling…

We present a review on the study of metastable silicon, primarily focusing mainly on the aspects of liquid-liquid transition, critical point and phase behaviour, structural and dynamic properties of liquid phase as well as crystal…

Achieving a coherent understanding of the many thermodynamic and dynamic anomalies of water is among the most important unsolved puzzles in physics, chemistry, and biology. One hypothesized explanation imagines the existence of a line of…

The thermodynamic and kinetic anomalies of supercooled liquids are analyzed from the perspective of energy landscapes. A mean field model, a generalized random energy model of liquids is developed, which exhibits a dynamical transition of…

In equilibrium and supercooled liquids, polymorphism is manifested by thermodynamic regions defined in the phase diagram, which are predominantly of different short- and medium-range order (local structure). It is found that on the phase…