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We demonstrate an efficient and accurate, general-purpose first-principles blueprint for calculating anharmonic vibrational free energy and predicting structural phase transition temperatures of solids. Thermodynamic integration is…

Materials Science · Physics 2024-03-14 Junsoo Park , Zhigang Wu , John W. Lawson

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…

Thermodynamic integration (TI) offers a rigorous method for estimating free-energy differences by integrating over a sequence of interpolating conformational ensembles. However, TI calculations are computationally expensive and typically…

Statistical Mechanics · Physics 2024-12-04 Bálint Máté , François Fleuret , Tristan Bereau

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

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

A theory for thermodynamic induction (TI) under isothermal conditions is presented. This includes a treatment of the Helmholtz free energy budget available for a gate variable to utilize towards aiding another variable's approach towards…

Mesoscale and Nanoscale Physics · Physics 2021-10-07 S. N. Patitsas

The anharmonicity of atomic motion limits the thermal conductivity in crystalline solids. However, a microscopic understanding of the mechanisms active in strong thermal insulators is lacking. In this letter, we classify 465 experimentally…

Materials Science · Physics 2023-06-14 Florian Knoop , Thomas A. R. Purcell , Matthias Scheffler , Christian Carbogno

Using normalizing flows and reweighting, Boltzmann Generators enable equilibrium sampling from a Boltzmann distribution, defined by an energy function and thermodynamic state. In this work, we introduce Thermodynamic Interpolation (TI),…

Chemical Physics · Physics 2024-11-18 Selma Moqvist , Weilong Chen , Mathias Schreiner , Feliks Nüske , Simon Olsson

A first-principles approach called the {\it{self-consistent quasiharmonic approximation}} (SC-QHA) method is formulated to calculate the thermal expansion, thermomechanics, and thermodynamic functions of solids at finite temperatures with…

Materials Science · Physics 2016-04-28 Liang-Feng Huang , Xue-Zeng Lu , Emrys Tennessen , James M. Rondinelli

A novel thermodynamic integration (TI) scheme is presented to compute the crystal-liquid interfacial free energy ($\gamma_{\rm cl}$) from molecular dynamics simulation. The scheme is applied to a Lennard-Jones system. By using extremely…

Soft Condensed Matter · Physics 2015-06-19 Ronald Benjamin , Jürgen Horbach

Moving grids are of interest in the numerical solution of hydrodynamical problems and in numerical relativity. We show that conventional integration methods for the simple wave equation in one and more than one dimension exhibit a number of…

Computational Physics · Physics 2009-11-06 Miguel Alcubierre , Bernard F. Schutz

Thermal instability (TI) is a trigger mechanism, which can explain formation of condensations through some regions of the interstellar clouds. Our goal here is to investigate some conditions for occurrence of TI and formation of…

Astrophysics of Galaxies · Physics 2019-08-14 Mohsen Nejad-Asghar

We develop an asymptotically exact renormalization group (RG) approach that treats electron-electron and electron-phonon interactions on equal footing. The approach allows an unbiased study of the instabilities of Fermi liquids without the…

Superconductivity · Physics 2007-05-23 S. -W. Tsai , A. H. Castro Neto , R. Shankar , D. K. Campbell

This paper formulates variational integrators for finite element discretizations of deformable bodies with heat conduction in the form of finite speed thermal waves. The cornerstone of the construction consists in taking advantage of the…

Mathematical Physics · Physics 2014-03-18 Pablo Mata A , Adrian J Lew

Theoretical frameworks used to qualitatively and quantitatively describe nuclear dynamics in solids are often based on the harmonic approximation. However, this approximation is known to become inaccurate or to break down completely in many…

Materials Science · Physics 2020-09-02 Florian Knoop , Thomas A. R. Purcell , Matthias Scheffler , Christian Carbogno

A thermodynamic integration (TI) protocol incorporating dummy atoms is introduced to calculate free energy differences for disulfide bond formation in proteins. This method successfully reproduces experimental redox potentials for multiple…

Biological Physics · Physics 2025-09-24 Daniel Mejia-Rodriguez , Suman Samantray , Margaret S. Cheung , Hoshin Kim

We develop a first-principles approach for the treatment of vibronic interactions in solids that overcomes the main limitations of state-of-the-art electron-phonon coupling formalisms. In particular, anharmonic effects in the nuclear…

Materials Science · Physics 2020-07-29 Marios Zacharias , Matthias Scheffler , Christian Carbogno

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

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…

Disordered solids exhibit unusual properties of their vibrational states and thermal conductivities. Recent progresses have well established the concept of "elastic heterogeneity", i.e., disordered materials show spatially inhomogeneous…

Disordered Systems and Neural Networks · Physics 2014-01-09 Hideyuki Mizuno , Stefano Mossa , Jean-Louis Barrat
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