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Accurate free-energy calculations are essential for predicting thermodynamic properties and phase stability, but existing methods are limited: phonon-based approaches neglect anharmonicity and liquids, while molecular dynamics (MD) is…

Materials Science · Physics 2025-11-19 Ekaterina Spirande , Timofei Miryashkin , Andrei Kolmakov , Alexander Shapeev

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

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

Free energies of molecules can be calculated by quantum computations or by normal mode classical calculations. However, the first can be computationally impractical for large molecules and the second is based on the assumption of harmonic…

Chemical Physics · Physics 2016-03-23 Asaf Farhi

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

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

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

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…

Statistical Mechanics · Physics 2021-02-05 Lin Yang , Yang Sun , Zhuo Ye , Feng Zhang , Mikhail I. Mendelev , Cai-Zhuang Wang , Kai-Ming Ho

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

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

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 present a fast and accurate method to calculate vibrational properties for mechanically unstable high temperature phases that suffer from imaginary frequencies at zero temperature. The method is based on standard finite-difference…

Materials Science · Physics 2015-06-03 Nikolas Antolin , Oscar D. Restrepo , Wolfgang Windl

We develop a method to fit high-temperature Gibbs free energy data for the development of interatomic potentials for atomic systems. The approach is based on Hamiltonian thermodynamic integration, enabling the identification of suitable…

Materials Science · Physics 2026-03-04 Liangrui Wei , Yang Sun

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

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

The computational modelling of reactions is simple in theory but can be quite tricky in practice. This article aims at the purpose of providing an assistance to a proper way of describing reactions theoretically and provides rough…

Chemical Physics · Physics 2017-02-14 Arnim Hellweg , Frank Eckert

Alchemical free energy calculations are a useful tool for predicting free energy differences associated with the transfer of molecules from one environment to another. The hallmark of these methods is the use of "bridging" potential energy…

We present an implementation of alchemical free energy simulations at the quantum mechanical level by directly interpolating the electronic Hamiltonian. The method is compatible with any level of electronic structure theory and requires…

Chemical Physics · Physics 2024-09-02 Chenghan Li , Xing Zhang , Garnet Kin-Lic Chan

Free energy calculations in molecular simulations have a variety of applications including determining the strength of molecular processes such as solvation and binding. It has been recently shown that when removing the VDW and Coulomb…

Chemical Physics · Physics 2015-07-15 Asaf Farhi , Bipin Singh

A novel thermodynamic integration (TI) scheme is presented that allows computing the free energy of grain boundaries (GBs) in crystals from atomistic computer simulation. Unlike previous approaches, the method can be applied at arbitrary…

Statistical Mechanics · Physics 2018-09-12 Saswati Ganguly , Jürgen Horbach
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