Phonon Thermal Transport at Interfaces of a Graphene/Vertically Aligned Carbon Nanotubes/Hexagonal Boron Nitride Sandwiched Heterostructure

Molecular dynamics simulation is used to calculate the interfacial thermal resistance of a graphene/carbon nanotubes/hexagonal boron nitride (Gr/CNTs/hBN) sandwiched heterostructure, in which vertically aligned carbon nanotube (VACNT) arrays are covalently bonded to graphene and hexagonal boron nitride layers. We find that the interfacial thermal resistance (ITR) of the Gr/VACNT/hBN sandwiched heterostructure is one to two orders of magnitude smaller than the ITR of a Gr/hBN van der Waals heterostructure with the same plane size. It is observed that covalent bonding effectively enhances the phonon coupling between Gr and hBN layers, resulting in an increase in the overlap factor of phonon density of states between Gr and hBN, thus reducing the ITR of Gr and hBN. In addition, the chirality, size (diameter and length), and packing density of sandwich-layer VACNTs have an important influence on the ITR of the heterostructure. Under the same CNT diameter and length, the ITR of the sandwiched heterostructure with armchair-shaped VACNTs is higher than that of the sandwiched heterostructure with zigzag-shaped VACNTs due to the different chemical bonding of chiral CNTs with Gr and hBN. When the armchair-shaped CNT diameter increases or the length decreases, the ITR of the sandwiched heterostructure tends to decrease. Moreover, the increase in the VACNT packing density also leads to a continuous decrease in the ITR of the sandwiched heterostructure, attributed to the extremely high intrinsic thermal conductivity of CNTs and the increase of out-of-plane heat transfer channels. This work may be helpful for understanding the mechanism for ITR in multilayer vertical heterostructures, and provides theoretical guidance for a new strategy to regulate the interlayer thermal resistance of heterostructures by optimizing the design of sandwich layer thermal interface materials.