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:rw-rs [version v1]

Publication date: Sep 22, 2022

How to cite this record

Michele Simoncelli, Francesco Mauri, Nicola Marzari, Thermal conductivity of glasses above the plateau: first-principles theory and applications, Materials Cloud Archive 2022.119 (2022), https://doi.org/10.24435/materialscloud:rw-rs

Description

Predicting the thermal conductivity of glasses from first principles has hitherto been a prohibitively complex problem. In fact, past works have highlighted challenges in achieving computational convergence with respect to length and/or time scales using either the established Allen-Feldman or Green-Kubo formulations, endorsing the concept that atomistic models containing thousands of atoms — thus beyond the capabilities of first-principles calculations — are needed to describe the thermal conductivity of glasses. In addition, these established formulations either neglect anharmonicity (Allen-Feldman) or miss the Bose-Einstein statistics of atomic vibrations (Green Kubo), thus leaving open the question on the relevance of these effects. Here, we present a first-principles formulation to address the thermal conductivity of glasses above the plateau, which can account comprehensively for the effects of structural disorder, anharmonicity, and quantum Bose-Einstein statistics. The protocol combines the Wigner formulation of thermal transport with convergence-acceleration techniques, and is validated in vitreous silica using both first-principles calculations and a quantum-accurate machine-learned interatomic potential. We show that models of vitreous silica containing less than 200 atoms can already reproduce the thermal conductivity in the macroscopic limit and that anharmonicity negligibly affects heat transport in vitreous silica. We discuss the microscopic quantities that determine the trend of the conductivity at high temperature, highlighting the agreement of the calculations with experiments in the temperature range above the plateau where radiative effects remain negligible (50<∼T <∼450 K).

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File name	Size	Description
data.zip MD5md5:a2316f43d4ac47af0208c0cfdb7abd92	872.8 KiB	atomistic models of vitreous silica studied in the paper "Thermal conductivity of glasses above the plateau: first-principles theory and applications" by M. Simoncelli, F. Mauri, N. Marzari

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Keywords

vitreous silica first principles thermal transport atomic vibrations