Phonon band structure and thermal transport correlation in a layered diatomic crystal

To elucidate the three-way relationship among a crystal’s structure, its phonon dispersion characteristics, and its thermal conductivity, an analysis is conducted on layered diatomic Lennard-Jones crystals with various mass ratios. Lattice dynamics theory and molecular dynamics simulations are used to predict the phonon dispersion curves and the thermal conductivity. The layered structure generates directionally dependent thermal conductivities lower than those predicted by density trends alone. The dispersion characteristics are quantified using a set of band diagram metrics, which are used to assess the contributions of acoustic phonons and optical phonons to the thermal conductivity. The thermal conductivity increases as the extent of the acoustic modes increases, and it decreases as the extent of the stop bands increases. The sensitivity of the thermal conductivity to the band diagram metrics is highest at low temperatures, where there is less anharmonic scattering, indicating that dispersion plays a more prominent role in thermal transport in that regime. We propose that the dispersion metrics i provide an indirect measure of the relative contributions of dispersion and anharmonic scattering to the thermal transport, and ii uncouple the standard thermal conductivity structure-property relation to that of structure-dispersion and dispersion-property relations, providing opportunities for better understanding of the underlying physical mechanisms and a potential tool for material design.