Related papers: Thermodynamics and kinetics of crystallisation in …
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…
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…
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.…
In recent decades, computer simulations have found increasingly widespread use as powerful tools of studying phase transitions in wide variety of systems. In the particular and very important case of aqueous systems, the commonly used…
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…
We investigate the kinetics and the free energy landscape of the crystallization of hard spheres from a supersaturated metastable liquid though direct simulations and forward flux sampling. In this first paper, we describe and test two…
It was recently demonstrated that the Stillinger-Weber silicon undergoes a liquid-liquid first-order phase transition deep into the supercooled region (Sastry and Angell, Nature Materials 2, 739 (2003)). Here we study the effects of…
In this work a method is proposed for computing step free energies for faceted solid-liquid interfaces based on atomistic simulations. The method is demonstrated in an application to (111) interfaces in elemental Si, modeled with the…
A vast array of phenomena, ranging from chemical reactions to phase transformations, are analysed in terms of a free energy surface defined with respect to a single or multiple order parameters. Enhanced sampling methods are typically used,…
In this paper, we report dynamic Monte Carlo simulations of melting and crystallization in a single-chain system. Their free energy barriers are calculated by the umbrella sampling method and can be described well by a simple expression…
We report Monte Carlo simulations of the melting of a single-polymer crystallite. We find that, unlike most atomic and molecular crystals, such crystallites can be heated appreciably above their melting temperature before they transform to…
The ST2 interaction potential has been used in a large number of simulation studies to explore the possibility of a liquid-liquid phase transition (LLPT) in supercooled water. Using umbrella sampling Monte Carlo simulations of ST2 water, we…
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…
Multicanonical ensemble simulations for the simulation of first-order phase transitions suffer from exponential slowing down. Monte Carlo autocorrelation times diverge exponentially with free energy barriers $\Delta F$, which in $L^d$ boxes…
We investigate the phase behavior of a single-component system in 3 dimensions with spherically-symmetric, pairwise-additive, soft-core interactions with an attractive well at a long distance, a repulsive soft-core shoulder at an…
First principles molecular dynamics simulations reveal a liquid-liquid phase transition in supercooled elemental silicon. Two phases coexist below $T_c\approx 1232K$. The low density phase is nearly tetra-coordinated, with a pseudogap at…
The existence of a 'crossover region' in glass-forming liquids has long been considered as a general phenomenon that is as important as the glass transition. One potential origin for the crossover behavior is a liquid-to-liquid phase…
We present a detailed analysis of the free energy surface of a well characterized rigid model for water in supercooled states. We propose a functional form for the liquid free energy, supported by recent theoretical predictions [Y.…
The crystallisation of entangled polymers from their melt is investigated using computer simulation with a coarse-grained model. Using hybrid Monte Carlo simulations enables us to probe the behaviour of long polymer chains. We identify…
When we lower the temperature of a liquid, at some point we meet a first order phase transition to the crystal. Yet, under certain conditions it is possible to keep the system in its metastable phase and to avoid crystallization. In this…