Related papers: Numerical method for computing the free energy of …
The free energy of glasses cannot be estimated using thermodynamic integration, as glasses are intrinsically not in equilibrium. We present numerical simulations showing that, in contrast, plausible free-energy estimates of a Kob-Andersen…
Using a recently developed technique to estimate the equilibrium free energy of glassy materials, we explore if equilibrium simulation methods can be used to estimate the solubility of amorphous solids. As an illustration, we compute the…
The scaling properties of the soft-sphere potential allow the derivation of an exact expression for the pressure of a frozen liquid, i.e., the pressure corresponding to configurations which are local minima in its multidimensional potential…
We propose a new method to compute the free energy or enthalpy of fluids or disordered solids by computer simulation . The main idea is to construct a reference system by freezing one representative configuration, and then carry out a…
We devise automated workflows for the calculation of Helmholtz and Gibbs free energies and their temperature and pressure dependence and provide the corresponding computational tools. We employ non-equilibrium thermodynamics for evaluating…
Glass is an under-cooled liquid that very slowly relaxes towards the equilibrium crystalline state. Its energy balance is ill understood, since it is widely believed that the glassy state cannot be described thermodynamically. However, the…
Using a novel thermodynamic integration scheme, we compute the excess free energy, $\gamma$, of a glass-forming, binary Lennard-Jones liquid in contact with a frozen amorphous wall, formed by particles frozen into a similar structure as the…
We develop a free energy framework to describe the response of glasses to applied stress. Unlike crystals, for which the free energy increases quadratically with strain due to affine displacements, for glasses, the nonequilibrium free…
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…
An analysis of the dynamics is performed, of exactly solvable models for fragile and strong glasses, exploiting the partitioning of the free energy landscape in inherent structures. The results are compared with the exact solution of the…
At low temperatures the configurational phase space of a macroscopic complex system (e.g., a spin-glass) of $N\sim 10^{23}$ interacting particles may split into an exponential number $\Omega_s \sim \exp({\rm const} \times N)$ of ergodic…
It is possible to formulate the thermodynamics of a glass forming system in terms of the properties of inherent structures, which correspond to the minima of the potential energy and build up the potential energy landscape in the…
The nature of the glass transition is one of the most important unsolved problems in condensed matter physics. The difference between glasses and liquids is believed to be caused by very large free energy barriers for particle…
Glass materials, as quintessential non-equilibrium systems, exhibit properties such as energy dissipation that are highly sensitive to their preparation histories. A key challenge has been identifying a unified order parameter to…
Despite the critical importance of the elastic properties of modern materials, there is not a singular model that can predict the modulus to an accuracy needed for industrial glass design. To address this problem, we propose an approach to…
This paper gives an introduction and brief overview of some of our recent work on the equilibrium thermodynamics of glasses. We have focused onto first principle computations in simple fragile glasses, starting from the two body interatomic…
Recent developments in statistical mechanics have allowed the estimation of equilibrium free energies from the statistics of work measurements during processes that drive the system out of equilibrium. Here a different class of processes is…
By means of a systematic expansion around the infinite-dimensional solution, we obtain an approximation scheme to compute properties of glasses in low dimensions. The resulting equations take as input the thermodynamic and structural…
The configurational entropy is among the key observables to characterize experimentally the formation of a glass. Physically, it quantifies the multiplicity of metastable states in which an amorphous material can be found at a given…
We describe a self-contained procedure to evaluate the free energy of liquid and solid phases of an alloy system. The free energy of a single-element solid phase is calculated with thermodynamic integration using the Einstein crystal as the…