Perspective on <i>ab initio</i> phonon thermal transport

Abstract

Coupling of the Peierls-Boltzmann equation with density functional theory paved the way for predictive thermal materials discovery and a variety of new physical insights into vibrational transport behaviors. Rapid theoretical and numerical developments have generated a wealth of thermal conductivity data and understanding of a wide variety of materials—1D, 2D, and bulk—for thermoelectric and thermal management applications. Nonetheless, modern ab initio descriptions of phonon thermal transport face challenges regarding the effects of defects, disorder, structural complexity, strong anharmonicity, quasiparticle couplings, and time and spatially varying perturbations. Highlighting recent research on these issues, this perspective explores opportunities to expand current ab initio phonon transport techniques beyond the paradigm of weakly perturbed crystals, to the wider variety of materials possible. Recent developments in phonon-defect interactions, complexity, disorder and anharmonicity, hydrodynamic transport, and the rising roles of molecular dynamics simulations, high throughput, and machine learning tools are included in this perspective. As more sophisticated theoretical and computational methods continue to advance thermal transport predictions, novel vibrational physics and thermally functional materials will be discovered for improved energy technologies.