Related papers: From Liquid Structure to Configurational Entropy: …
In molecular liquids such as water, time-delayed influences between microscopic or mesoscopic variables are typically probed using time-correlation functions, which are symmetric under detailed balance and therefore blind to dynamical…
The overlap, or similarity, between liquid configurations is at the core of the mean-field description of the glass transition, and remains a useful concept when studying three-dimensional glass-forming liquids. In liquids, however, the…
Despite the use of glasses for thousands of years, the nature of the glass transition is still mysterious. On approaching the glass transition, the growth of dynamic heterogeneity has long been thought to play a key role in explaining the…
Calculations of the thermodynamical properties of a supercooled liquid confined in a matrix are performed with an inherent structure analysis. The liquid entropy is computed by means of a thermodynamical integration procedure. The…
A new connection between structure and dynamics in glass-forming liquids is presented. We show how the origin of spatially localized excitations, as defined by dynamical facilitation (DF) theory, can be understood from a structure-based…
Volume and enthalpy relaxation of glasses after a sudden temperature change has been extensively studied since Kovacs seminal work. One observes an asymmetric approach to equilibrium upon cooling versus heating and, more…
We report a molecular dynamics simulation study of the properties of the potential energy landscape sampled by a system of water molecules during the process of generating a glass by cooling, and during the process of regenerating the…
The dynamical properties and mechanical functions of amorphous materials are governed by their microscopic structures, particularly the elasticity of the interaction networks, which is generally complicated by structural heterogeneity. This…
We study dynamics of a locally conserved energy in ergodic, local many-body quantum systems on a lattice with no additional symmetry. The resulting dynamics is well approximated by a coarse grained, classical linear functional diffusion…
The transition of a fluid to a rigid glass upon cooling is a common route of transformation from liquid to solid that embodies the most poorly understood features of both phases1,2,3. From the liquid perspective, the puzzle is to understand…
The theory developed in our previous papers is applied in this paper to investigate the dependence of slowing down of dynamics of glass-forming liquids on the attractive and repulsive parts of intermolecular interactions. Through an…
The random first order transition theory of the dynamics of supercooled liquids is extended to treat aging phenomena in nonequilibrium structural glasses. A reformulation of the idea of ``entropic droplets'' in terms of libraries of local…
According to excess-entropy scaling, dynamic properties of liquids like viscosity and diffusion coefficient are determined by the entropy. This link between dynamics and thermodynamics is increasingly studied and of interest also for…
Recent simulation and model system studies suggest that local structural excitations play an important role in the dynamics of liquids and glasses. Here, for the first time, we quantify excitation populations in real liquids, showing that…
Within the framework of density functional theory, the inclusion of exact exchange and non-local van der Waals/dispersion (vdW) interactions is crucial for predicting a microscopic structure of ambient liquid water that quantitatively…
A popular Adam--Gibbs scenario has suggested that the excess entropy of glass and liquid over crystal dominates the dynamical arrest at the glass transition with exclusive contribution from configurational entropy over vibrational entropy.…
We study the dynamics of entropy in a time dependent potential and explore how disorder influences this entropy flow. We show that disorder can trap entropy at the edge of the atomic cloud enabling a novel cooling method. We demonstrate the…
The structure of a simple liquid may be characterised in terms of ground state clusters of small numbers of atoms of that same liquid. Here we use this sensitive structural probe to consider the effect of a liquid-vapour interface upon the…
This paper summarizes the properties of strongly correlating liquids, i.e., liquids with strong correlations between virial and potential energy equilibrium fluctuations at constant volume. We proceed to focus on the experimental…
We describe a model for the thermodynamics and dynamics of glass-forming liquids in terms of excitations from an ideal glass state to a Gaussian manifold of configurationally excited states. The quantitative fit of this three parameter…