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We generalize a previously established ab initio approach-originally developed for hexagonal close-packed (hcp) metals-to accommodate solids with both internal and external degrees of freedom. This extension enables the thermodynamic and…

Materials Science · Physics 2026-03-06 Xuejun Gong , Andrea Dal Corso

The Helmholtz energy is a key thermodynamic quantity representing available energy to do work at a constant temperature and volume. Despite a well-established methodology from first-principles calculations, a comprehensive tool and database…

Materials Science · Physics 2025-04-25 Nigel Lee En Hew , Luke Allen Myers , Axel van de Walle , Shun-Li Shang , Zi-Kui Liu

An innovative method is developed for accurate determination of thermodynamic properties as a function of temperature by revisiting the density functional theory (DFT) based quasiharmonic approach (QHA). The present methodology individually…

Materials Science · Physics 2024-05-16 Shun-Li Shang , Rushi Gong , Michael C. Gao , Darren C. Pagan , Zi-Kui Liu

Thermal properties of solid-state materials are a fundamental topic of study with important practical implications. For example, anisotropic displacement parameters (ADPs) are routinely used in physics, chemistry, and crystallography to…

Materials Science · Physics 2016-12-28 Janine George , Volker L. Deringer , Ai Wang , Paul Müller , Ulli Englert , Richard Dronskowski

In the realm of thermal expansion determination, the quasiharmonic approximation (QHA) stands as a widely embraced method for discerning minima of free energies across diverse temperatures such that the temperature dependence of lattice…

Materials Science · Physics 2024-07-12 Samare Rostami , Xavier Gonze

A density functional theory (DFT) framework is presented that links functional derivatives of free-energy functionals to non-linear static density response functions in quantum many-body systems. Within this framework, explicit expressions…

Predictions of the anisotropic coefficients of thermal expansion are needed to not only compare to experimental measurement, but also as input for macroscopic modeling of devices which operate over a large temperature range. While most…

Materials Science · Physics 2019-03-08 Nicholas A. Pike , Ole M. Løvvik

We apply the pseudopotential density functional perturbation theory approach along with the quasiharmonic approximation to calculate the thermal expansion of tungsten and two important metallic alloys, NiAl and PdTi. We derive the theory…

Materials Science · Physics 2009-11-10 Graeme J. Ackland , Xiangyang Huang , Karin M. Rabe

This study investigates the thermal expansion coefficient of two-dimensional (2D) functionalized boron nitride (f-BN) materials using first-principles density functional theory (DFT). Two-dimensional materials, particularly hexagonal boron…

Materials Science · Physics 2025-04-30 Sk Mujaffar Hossain , Dobin Kim , Jaehyun Park , Seung-Cheol Lee , Satadeep Bhattacharjee

"Quasi-harmonic" (QH) theory should not be considered a low-order theory of anharmonic effects in crystals, but should be recognized as an important effect separate from "true" anharmonicity. The original and widely used meaning of QH…

Materials Science · Physics 2022-12-06 Philip B. Allen

This chapter introduces thermal density functional theory, starting from the ground-state theory and assuming a background in quantum mechanics and statistical mechanics. We review the foundations of density functional theory (DFT) by…

Chemical Physics · Physics 2014-06-02 Aurora Pribram-Jones , Stefano Pittalis , E. K. U. Gross , Kieron Burke

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

This article is part-I of a review of density-functional theory (DFT) that is the most widely used method for calculating electronic structure of materials. The accuracy and ease of numerical implementation of DFT methods has resulted in…

Materials Science · Physics 2023-05-25 Prashant Singh , Manoj K Harbola

The structural, dynamical, and thermodynamical properties of diamond, graphite and layered derivatives (graphene, rhombohedral graphite) are computed using a combination of density-functional theory (DFT) total-energy calculations and…

Materials Science · Physics 2009-11-10 Nicolas Mounet , Nicola Marzari

Some anisotropy in both mechanical and thermodynamical properties of bismuth is expected. A combination of density functional theory total energy calculations and density functional perturbation theory in the local density approximation is…

Materials Science · Physics 2016-04-20 B. Arnaud , S. Lebègue , G. Raffy

Density Functional Theory (DFT) has become the quasi-standard for ab-initio simulations for a wide range of applications. While the intrinsic cubic scaling of DFT was for a long time limiting the accessible system size to some hundred…

Materials Science · Physics 2018-02-23 Stephan Mohr , Marc Eixarch , Maximilian Amsler , Mervi J. Mantsinen , Luigi Genovese

This paper gives a short overview of the calculation of thermal properties of materials from first principles, using the Quasi-Harmonic Approximation (QHA). We first introduce some of the thermal properties of interest and describe how they…

Materials Science · Physics 2011-12-22 Stefano Baroni , Paolo Giannozzi , Eyvaz Isaev

The thermal properties of materials are critically important to various technologies and are increasingly the target of materials design efforts. However, it is only relatively recent advances in first-principles computational techniques…

Materials Science · Physics 2021-12-08 Ethan T. Ritz , Nicole A. Benedek

The microscopic origin of the large negative thermal expansion of cubic scandium trifluorides (ScF3) is investigated by performing a set of anharmonic free-energy calculations based on density functional theory. We demonstrate that the…

Materials Science · Physics 2019-03-13 Yusuke Oba , Terumasa Tadano , Ryosuke Akashi , Shinji Tsuneyuki

We coupled first principles calculations and the quasiharmonic approximation combined with experiments (X-Ray diffraction and dilatometry measurements) to determine the thermal properties of NiTiSn (half-Heusler) and Ni2TiSn (Heusler)…

Materials Science · Physics 2015-04-08 P. Hermet , R. M. Ayral , E. Theron , P. G. Yot , F. Salles , M. Tillard , P. Jund
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