Molecular Dynamics Simulation on In-Plane Thermal Conductivity of Graphene/Hexagonal Boron Nitride van der Waals Heterostructures

Graphene, hexagonal boron nitride (h-BN), and their heterostructures are promising thermal interface materials due to the outstanding thermal properties of graphene and h-BN. For the heterostructures, extensive work has mainly focused on the thermal transport of two-dimensional (2D) graphene/h-BN (GBN) in-plane heterostructures in which graphene and h-BN are bonded at the interface. In this study, we investigate the thermal conductivity of three-dimensional (3D) GBN van der Waals (vdW) heterostructures by means of nonequilibrium molecular dynamics (NEMD) simulations. Unlike the 2D GBN in-plane heterostructure, the 3D GBN vdW heterostructure consists of three layers where graphene is sandwiched by two h-BN sheets via vdW forces. Various techniques, including hydrogen-functionalization, vacancy defects, tensile strain, interlayer coupling strength, layer numbers of h-BN, size effect, and temperature, are extensively explored to find an effective route for the modulation of the thermal conductivity. It is found that the thermal conductivity of the triple-layer GBN vdW heterostructure is very sensitive to these extrinsic factors. Of these, hydrogen-functionalization is the most effective method. A low hydrogen coverage of 1% in the sandwiched graphene can lead to 55% reduction in the thermal conductivity of the vdW heterostructure. Vacancy defects on graphene exert a more significant effect on the thermal conductivity reduction for the vdW heterostructure than B or N vacancies in the outer h-BN layers. This work reveals the physical mechanism for manipulating the thermal transport along the GBN vdW heterostructures via structural modification and provides a useful guideline for designing novel thermal management devices based on the GBN vdW heterostructures.