Michele Simoncelli^1*, Francesco Mauri^2*, Nicola Marzari^3*

1 Theory of Condensed Matter Group of the Cavendish Laboratory, University of Cambridge (UK)

2 Dipartimento di Fisica, Università di Roma La Sapienza, Piazzale Aldo Moro 5, I-00185 Roma, Italy

3 Theory and Simulation of Materials (THEOS) and National Centre for Computational Design and Discovery of Novel Materials (MARVEL), École Polytechnique Fédérale de Lausanne, Lausanne, Switzerland.

* Corresponding authors emails: ms2855@cam.ac.uk, francesco.mauri@uniroma1.it, nicola.marzari@epfl.ch

DOI10.24435/materialscloud:jz-tf [version v2]

Publication date: May 22, 2023

How to cite this record

Michele Simoncelli, Francesco Mauri, Nicola Marzari, Thermal conductivity of glasses: first-principles theory and applications, Materials Cloud Archive 2023.76 (2023), https://doi.org/10.24435/materialscloud:jz-tf

Description

Predicting the thermal conductivity of glasses from first principles has hitherto been a very complex problem. The established Allen-Feldman and Green-Kubo approaches employ approximations with limited validity--the former neglects anharmonicity, the latter misses the quantum Bose-Einstein statistics of vibrations--and require atomistic models that are very challenging for first principles methods. Here, we present a protocol to determine from first-principles the thermal conductivity k(T) of glasses above the plateau (i.e., above the temperature-independent region appearing almost without exceptions in the k(T) of all glasses at cryogenic temperatures). The protocol combines the Wigner formulation of thermal transport with convergence-acceleration techniques, and accounts comprehensively for the effects of structural disorder, anharmonicity, and Bose-Einstein statistics. We validate this approach in vitreous silica, showing that models containing less than 200 atoms can already reproduce k(T) in the macroscopic limit. We discuss the effects of anharmonicity and the mechanisms determining the trend of k(T) at high temperature, reproducing experiments at temperatures where radiative effects remain negligible.

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data.zip MD5md5:71313c5458f0ad0a6ab3cc796c9fbe68	921.9 KiB	atomistic structures of all the v-SiO2 models studied

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Keywords

vitreous silica first principles thermal transport atomic vibrations