Thermal Transport in MoS$_2$ from Molecular Dynamics using Different Empirical Potentials

Abstract: Thermal properties of molybdenum disulfide (MoS$_2$) have recently attracted attention related to fundamentals of heat propagation in strongly anisotropic materials, and in the context of potential applications to optoelectronics and thermoelectrics. Multiple empirical potentials have been developed for classical molecular dynamics (MD) simulations of this material, but it has been unclear which provides the most realistic results. Here, we calculate lattice thermal conductivity of single- and multi-layer pristine MoS$_2$ by employing three different thermal transport MD methods: equilibrium, nonequilibrium, and homogeneous nonequilibrium ones. These methods allow us to verify the consistency of our results and also facilitate comparisons with previous works, where different schemes have been adopted. Our results using variants of the Stillinger-Weber potential are at odds with some previous ones and we analyze the possible origins of the discrepancies in detail. We show that, among the potentials considered here, the reactive empirical bond order (REBO) potential gives the most reasonable predictions of thermal transport properties as compared to experimental data. With the REBO potential, we further find that isotope scattering has only a small effect on thermal conduction in MoS$_2$ and the in-plane thermal conductivity decreases with increasing layer number and saturates beyond about three layers. We identify the REBO potential as a transferable empirical potential for MD simulations of MoS$_2$ which can be used to study thermal transport properties in more complicated situations such as in systems containing defects or engineered nanoscale features. This work establishes a firm foundation for understanding heat transport properties of MoS$_2$ using MD simulations.