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It is extremely difficult to control the growth orientation of the graphene layer in comparison to Si or III-V semiconductors. Here we report a direct observation of graphene growth and domain boundary formation in a scanning transmission electron microscope, with residual hydrocarbon in the microscope chamber being used as the carbon source for in-plane graphene growth at the step-edge of bilayer graphene substrate. We show that the orientation of the growth is strongly influenced by the step-edge structure and areas grown from a reconstructed 5-7 edge are rotated by 30° with respect to the mother layer. Furthermore, single heteroatoms like Si may act as catalytic active sites for the step-edge growth. The findings provide an insight into the mechanism of graphene growth and defect reconstruction that can be used to tailor carbon nanostructures with desired properties.

In situ observation of step-edge in-plane growth of graphene in a STEM