First-principles Modeling of Thermal Transport in Materials: Achievements, Opportunities, and Challenges

Thermal transport properties have attracted extensive research attentions over the past decades. First-principles-based approaches have proved to be very useful for predicting the thermal transport properties of materials and revealing the phonon and electron scattering or propagation mechanisms in materials and devices. In this review, we provide a concise but inclusive discussion on state-of-the-art first-principles thermal modeling methods and notable achievements by these methods over the last decade. A wide range of materials are covered in this review, including two-dimensional materials, superhard materials, metamaterials, and polymers. We also cover the very recent important findings on heat transfer mechanisms informed from first principles, including phonon–electron scattering, higher-order phonon–phonon scattering, and the effect of external electric field on thermal transport. Finally, we discuss the challenges and limitations of state-of-the-art approaches and provide an outlook toward future developments in this area.