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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

Ensuring a satisfactory statistical convergence of anharmonic thermodynamic properties requires sampling of many atomic configurations, however the methods to obtain those necessarily produce correlated samples, thereby reducing the…

Statistical Mechanics · Physics 2022-06-07 Erki Metsanurk

Quantitative evaluations of the free energy of materials must take into account thermal and zero-point energy fluctuations. While these effects can easily be estimated within a harmonic approximation, corrections arising from the anharmonic…

Materials Science · Physics 2019-06-18 Venkat Kapil , Edgar Engel , Mariana Rossi , Michele Ceriotti

Within the framework of density functional theory (DFT), the total energy of crystal structures is calculated at zero temperature. Herein, we briefly discuss the DFT-based lattice-dynamics approach for computing crystal free energy, the…

Materials Science · Physics 2015-07-01 Tran Doan Huan

Phonon frequency moments and thermodynamic functions (electrostatic and vibrational parts of the free energy, internal energy, and heat capacity) are calculated for bcc and fcc Coulomb crystals in the harmonic approximation with a…

Plasma Physics · Physics 2009-11-07 D. A. Baiko , A. Y. Potekhin , D. G. Yakovlev

We present a theoretical first-principles method to calculate the free energy of a magnetic system in its high-temperature paramagnetic phase, including vibrational, electronic, and magnetic contributions. The method for calculating free…

We have developed a thorough and accurate method of determining anharmonic free energies, the temperature dependent effective potential technique (TDEP). It is based on \emph{ab initio} molecular dynamics followed by a mapping onto a model…

Statistical Mechanics · Physics 2013-10-14 Olle Hellman , Peter Steneteg , Igor A. Abrikosov , Sergei I. Simak

The anharmonicity resulted from the intrinsic phonon interaction is neglected by quasiharmonic approximation. Although the intensive researches about anharmonicity have been done, up to now the free energy contributed by the anharmonicity…

Statistical Mechanics · Physics 2007-05-23 Zhongqing Wu , Renata M. Wentzcovitch

The efficient and accurate calculation of how ionic quantum and thermal fluctuations impact the free energy of a crystal, its atomic structure, and phonon spectrum is one of the main challenges of solid state physics, especially when strong…

A density-functional-theory based approach to efficiently compute numerically exact vibrational free energies - including anharmonicity - for chemically complex multicomponent alloys is developed. It is based on a combination of…

In the framework of density functional theory (DFT) simulations of molecules and materials, anharmonic terms of the potential energy surface are commonly computed numerically, with an associated cost that rapidly increases with the size of…

Materials Science · Physics 2025-03-17 Davide Mitoli , Jefferson Maul , Alessandro Erba

A methodology for calculating the contribution of charged defects to the configurational free energy of an ionic crystal is introduced. The temperature-independent Wang-Landau Monte Carlo technique is applied to a simple model of a solid…

Materials Science · Physics 2015-06-16 Robert M. Horton , Andrew J. Haslam , Amparo Galindo , George Jackson , Michael W. Finnis

We have developed a method to accurately and efficiently determine the vibrational free energy as a function of temperature and volume for substitutional alloys from first principles. Taking Ti$_{1-x}$Al$_x$N alloy as a model system, we…

The features for the unsteady process of thermal equilibration ("the fast motions") in a one-dimensional harmonic crystal lying in a viscous environment (e.g., a gas) are under investigation. It is assumed that initially the displacements…

Statistical Mechanics · Physics 2021-02-16 Serge N. Gavrilov , Anton M. Krivtsov

Analytic expressions for the energy eigenvalues and eigenfunctions of a one-dimensional harmonic crystal are obtained. The average energy and density profiles are obtained numerically as a function of temperature. A surprisingly large…

Quantum Physics · Physics 2021-08-30 Phil Attard

The phase diagram of numerous materials of technological importance features high-symmetry high-temperature phases that exhibit phonon instabilities. Leading examples include shape-memory alloys, as well as ferroelectric, refractory, and…

Materials Science · Physics 2017-02-06 Sara Kadkhodaei , Qi-Jun Hong , Axel van de Walle

Harmonic calculations based on density-functional theory are generally the method of choice for the description of phonon spectra of metals and insulators. The inclusion of anharmonic effects is, however, delicate as it relies on…

Materials Science · Physics 2015-06-17 Ion Errea , Matteo Calandra , Francesco Mauri

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

The phase field crystal (PFC) method has emerged as a promising technique for modeling materials with atomistic resolution on mesoscopic time scales. The approach is numerically much more efficient than classical density functional theory…

Materials Science · Physics 2015-05-18 Michael Greenwood , Nikolas Provatas , Jörg Rottler

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
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