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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

Ab initio molecular dynamics (AIMD) based on density functional theory (DFT) has become a workhorse for studying the structure, dynamics, and reactions in condensed matter systems. Currently, AIMD simulations are primarily carried out at…

Chemical Physics · Physics 2025-06-10 Ritama Kar , Sagarmoy Mandal , Vaishali Thakkur , Bernd Meyer , Nisanth N. Nair

We introduce a lattice dynamics package which calculates elastic, thermodynamic and thermal transport properties of crystalline materials from data on their force and potential energy as a function of atomic positions. The data can come…

The calculation of free energies from first principles in materials is a formidable task which enables the prediction of phase stability with high accuracy; these calculations are complicated in magnetic materials by the interplay of…

Materials Science · Physics 2023-01-18 Davide Gambino , Johan Klarbring , Björn Alling

Ab initio molecular dynamics (AIMD) is a powerful tool to predict properties of molecular and condensed matter systems. The quality of this procedure is based on accurate electronic structure calculations. The development of quantum…

Using conceptually and procedurally consistent density functional theory (DFT) calculations with an advanced meta-GGA exchange-correlation functional in ab initio molecular dynamics simulations, we determine the insulator-metal transition…

Standard harmonic-to-anharmonic thermodynamic integration (TI) is known to develop a near singularity in the integrand for solids exhibiting diffusive degrees of freedom, such as rotating functional groups or migrating defects. This…

Chemical Physics · Physics 2026-02-13 Venkat Kapil

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

Centroid molecular dynamics (CMD) incorporates nuclear quantum statistics into the calculation of vibrational spectra. However, when performed in Cartesian coordinates, CMD shows unphysical artifacts in certain vibrational bands, known as…

Chemical Physics · Physics 2025-11-04 Jorge Castro , George Trenins , Venkat Kapil , Mariana Rossi

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

In studying solidification process by simulations on the atomic scale, the modeling of crystal nucleation or amorphisation requires the construction of interatomic interactions that are able to reproduce the properties of both the solid and…

Precise prediction of phase diagrams in molecular dynamics (MD) simulations is challenging due to the simultaneous need for long time scales, large length scales and accurate interatomic potentials. We show that thermodynamic integration…

Materials Science · Physics 2023-06-06 Tanooj Shah , Kamron Fazel , Jie Lian , Liping Huang , Yunfeng Shi , Ravishankar Sundararaman

Phonons, quantized vibrations of the atomic lattice, are fundamental to understanding thermal transport, structural stability, and phase behavior in crystalline solids. Despite advances in computational materials science, most predictions…

Materials Science · Physics 2026-01-15 Huiju Lee , Zhi Li , Jiangang he , Yi Xia

Predicting solid-solid phase transitions remains a long-standing challenge in materials science. Solid-solid transformations underpin a wide range of functional properties critical to energy conversion, information storage, and thermal…

Materials Science · Physics 2025-06-03 Cibrán López , Joshua Ojih , Ming Hu , Josep Lluis Tamarit , Edgardo Saucedo , Claudio Cazorla

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

In this paper, a hybrid quasi-static atomistic simulation method at finite temperature is developed, which combines the advantages of MD for thermal equilibrium and atomic-scale finite element method (AFEM) for efficient equilibration. Some…

Atomic Physics · Physics 2015-06-17 Ran Xu , Bin Liu

Thermodynamic Integration (TI) is the state-of-the-art computational technique for accurate Gibbs free energy predictions of solids. Conventional TI schemes start from an NVT harmonic reference and require three successive corrections to…

While the vibrational thermodynamics of materials with small anharmonicity at low temperatures has been understood well based on the harmonic phonons approximation; at high temperatures, this understanding must accommodate how phonons…

Materials Science · Physics 2015-10-20 Tian Lan

A general set of methods is presented for calculating chemical potentials in solid and liquid mixtures using {\em ab initio} techniques based on density functional theory (DFT). The methods are designed to give an {\em ab initio} approach…

Materials Science · Physics 2009-11-07 D. Alfe` , M. J. Gillan , G. D. Price

Phase diagrams serve as a highly informative tool for materials design, encapsulating information about the phases that a material can manifest under specific conditions. In this work, we develop a method in which Bayesian inference is…

Materials Science · Physics 2023-09-06 Timofei Miryashkin , Olga Klimanova , Vladimir Ladygin , Alexander Shapeev
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