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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…

Materials Science · Physics 2021-10-13 Sarath Menon , Yury Lysogorskiy , Jutta Rogal , Ralf Drautz

Comparison of free energies between different phases and different compositions underlies the prediction of alloy phase diagrams. To allow direct comparison, consistent reference points for the energies or enthalpies are required, and the…

Materials Science · Physics 2021-05-19 Yang Huang , Michael Widom , Michael C. Gao

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…

Computational Physics · Physics 2011-03-16 Friederike Schmid , Tanja Schilling

The recently proposed Einstein molecule approach is extended to compute the free energy of molecular solids. This method is a variant of the Einstein crystal method of Frenkel and Ladd[J. Chem. Phys. 81,3188 (1984)]. In order to show its…

Statistical Mechanics · Physics 2009-01-14 E. G. Noya , M. M. Conde , C. Vega

In this review we focus on the determination of phase diagrams by computer simulation with particular attention to the fluid-solid and solid-solid equilibria. The calculation of the free energy of solid phases using the Einstein crystal and…

Statistical Mechanics · Physics 2009-01-14 C. Vega , E. Sanz , J. L. F. Abascal , E. G. Noya

We develop a new approach to determining LJ-EAM potentials for alloys and use these to determine the solid-liquid phase diagrams for binary metallic alloys using Kofke's Gibbs-Duhem integration technique combined with semigrand canonical…

Materials Science · Physics 2013-05-29 H. -S. Nam , M. I. Mendelev , D. J. Srolovitz

We describe a first-principles statistical mechanics method to calculate the free energies of crystalline alloys that depend on temperature, composition, and strain. The approach relies on an extension of the alloy cluster expansion to…

Materials Science · Physics 2023-11-01 Sesha Sai Behara , John C. Thomas , Brian Puchala , Anton Van der Ven

In this work the free energy of solid phases is computed for the Lennard-Jones potential and for a model of NaCl. The free energy is evaluated through the Einstein crystal/molecule methodologies using the Molecular Dynamics programs:…

Soft Condensed Matter · Physics 2012-10-16 J. L. Aragones , C. Valeriani , C. Vega

For classical discrete systems under constant composition typically refferred to substitutional alloys, we propose calculation method of Helmholtz free energy based on a set of special microscopic states. The advantage of the method is that…

Statistical Mechanics · Physics 2021-10-22 Ryogo Miyake , Subaru Sugie , Koretaka Yuge

Taking advantage of the advances in generative deep learning, particularly normalizing flow, a framework, called Boltzmann Generator, has recently been proposed for the purpose of generating equilibrium atomic configurations from the…

Statistical Mechanics · Physics 2022-07-27 Rasool Ahmad , Wei Cai

The free energy of mixing and the entropy of mixing for Cu$_{x}$Al$_{1-x}$ liquid binary alloys have been systematically investigated by using the electronic theory of metals along with the perturbation approach at a thermodynamic state…

Materials Science · Physics 2016-07-21 Fysol Ibna Abbas , G. M. Bhuiyan , A. Z. Ziauddin Ahmed

Using the entropy $S$ as a reaction coordinate, we determine the free energy barrier associated with the formation of a liquid droplet from a supersaturated vapor for atomic and molecular fluids. For this purpose, we develop the $\mu VT-S$…

Statistical Mechanics · Physics 2021-08-25 Caroline Desgranges , Jerome Delhommelle

Sets of free energy differences are useful for finding the equilibria of chemical reactions, while absolute free energies have little physical meaning. However finding the relative free energy between two macrostates by subtraction of their…

Statistical Mechanics · Physics 2012-11-26 Joshua T. Berryman , Tanja Schilling

This article describes nonequilibrium techniques for the calculation of free energies of solids using molecular dynamics (MD) simulations. These methods provide an alternative to standard equilibrium thermodynamic integration methods and…

Materials Science · Physics 2022-01-13 Rodrigo Freitas , Mark Asta , Maurice de Koning

We propose a numerical technique to compute the equilibrium free energy of glasses that cannot be prepared quasi-reversibly. For such systems, standard techniques for estimating the free energy by extrapolation, cannot be used. Instead, we…

Statistical Mechanics · Physics 2021-01-04 H. A. Vinutha , Daan Frenkel

The Gibbs free energy is the fundamental thermodynamic potential underlying the relative stability of different states of matter under constant-pressure conditions. However, computing this quantity from atomic-scale simulations is far from…

Materials Science · Physics 2018-02-14 Bingqing Cheng , Michele Ceriotti

The vastness of the space of possible multicomponent metal alloys is hoped to provide improved structural materials but also challenges traditional, low-throughput materials design efforts. Computational screening could narrow this search…

Atomistic simulations are employed to demonstrate the existence of a well-defined thermodynamic phase transformation between grain boundary (GB) phases with different atomic structures. The free energy of different interface structures for…

Materials Science · Physics 2018-09-19 Rodrigo Freitas , Robert E. Rudd , Mark Asta , Timofey Frolov

The calculation of the interfacial free energy between two thermodynamic phases is crucial across various fields, including materials science, chemistry, and condensed matter physics. In this study, we apply an existing thermodynamic…

Soft Condensed Matter · Physics 2024-11-26 Ignacio Sanchez-Burgos , Pablo Montero de Hijes , Eduardo Sanz , Carlos Vega , Jorge R. Espinosa

A melting transition for a system of hard spheres interacting by a repulsive Yukawa potential of DLVO form is studied. To find the location of the phase boundary, we propose a simple theory to calculate the free energies for the coexisting…

Condensed Matter · Physics 2015-06-25 P. S. Kuhn , A. Diehl , Y. Levin , M. C. Barbosa
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