Understanding Phonon Transport Properties Using Classical Molecular Dynamics Simulations

TL;DR

This paper reviews how classical Molecular Dynamics simulations can be used to predict phonon and thermal transport properties of materials, discussing their capabilities, limitations, and strategies for improvement.

Contribution

It provides a comprehensive overview of MD-based methods for thermal transport, highlighting recent developments, challenges, and future directions for more accurate predictions.

Findings

MD simulations can estimate thermal conductivity and interfacial conductance.

Coupling MD with lattice dynamics offers vibrational mode insights.

Developing accurate interatomic potentials and quantum corrections is crucial.

Abstract

Predictive modeling of the phonon/thermal transport properties of materials is vital to rational design for a diverse spectrum of engineering applications. Classical Molecular Dynamics (MD) simulations serve as a tool to simulate the time evolution of the atomic level system dynamics and enable calculation of thermal transport properties for a wide range of materials, from perfect periodic crystals to systems with strong structural and compositional disorder, as well as their interfaces. Although MD does not intrinsically rely on a plane wave-like phonon description, when coupled with lattice dynamics calculations, it can give insights to the vibrational mode level contributions to thermal transport, which includes plane-wave like modes as well as others, rendering the approach versatile and powerful. On the other hand, several deficiencies including the lack of vibrationally accurate interatomic potentials and the inability to rigorously include the quantum nature of phonons prohibit the widespread applicability and reliability of Molecular Dynamics simulations. This article provides a comprehensive review of classical Molecular Dynamics based formalisms for extracting thermal transport properties: thermal conductivity and thermal interfacial conductance and the effects of various structural, compositional, and chemical parameters on these properties. Here, we highlight unusual property predictions, and emphasize on the needs and strategies for developing accurate interatomic potentials and rigorous quantum correction schemes.