Synthesis of well-aligned millimeter-sized tetragon-shaped graphene domains by tuning the copper substrate orientation

We present a simple processing method for synthesizing well-aligned millimeter-sized tetragon-shaped graphene domains on a polycrystalline copper substrate via low-pressure chemical vapor deposition. The tetragonal shape is achieved simply by wet loading the copper substrate with processing conditions previously used for the growth of millimeter-sized hexagon-shaped graphene domains. Electron backscatter diffraction (EBSD) shows that the wet loaded copper substrate is uniformly textured with a surface plane between Cu (1 0 0) and Cu (1 1 0). The in-plane rotation of the crystalline orientation across the Cu grains is very small. However, the EBSD showed that the surface orientation of the dry loaded substrate is close to the (1 1 1) crystal plane. The different surface orientation of the wet and dry loaded samples is attributed to the different surface oxygen concentration, which changes the relative stability of the (0 0 1), (1 1 0), and (1 1 1) plane during copper sublimation and recrystallization. These results provide an approach to tune the surface crystal orientation and thus the shape and orientation of the graphene domains.