Role of Carbon Interstitials in Transition Metal Substrates on Controllable Synthesis of High-Quality Large-Area Two-Dimensional Hexagonal Boron Nitride Layers

Reliable and controllable synthesis of two-dimensional (2D) hexagonal boron nitride (h-BN) layers is highly desirable for their applications as 2D dielectric and wide bandgap semiconductors. In this work, we demonstrate that the dissolution of carbon into cobalt (Co) and nickel (Ni) substrates can facilitate the growth of h-BN and attain large-area 2D homogeneity. The morphology of the h-BN film can be controlled from 2D layer-plus-3D islands to homogeneous 2D few-layers by tuning the carbon interstitial concentration in the Co substrate through a carburization process prior to the h-BN growth step. Comprehensive characterizations were performed to evaluate structural, electrical, optical, and dielectric properties of these samples. Single-crystal h-BN flakes with an edge length of ∼600 μm were demonstrated on carburized Ni. An average breakdown electric field of 9 MV/cm was achieved for an as-grown continuous 3-layer h-BN on carburized Co. Density functional theory calculations reveal that the interstitial carbon atoms can increase the adsorption energy of B and N atoms on the Co(111) surface and decrease the diffusion activation energy and, in turn, promote the nucleation and growth of 2D h-BN.