Repeated growth-etching-regrowth for large-area defect-free single-crystal graphene by chemical vapor deposition

Reducing nucleation density and healing structural defects are two challenges for fabricating large-area high-quality single-crystal graphene, which is essential for its electronic and optoelectronic applications. We have developed a method involving chemical vapor deposition (CVD) growth followed by repeated etching-regrowth, to solve both problems at once. Using this method, we can obtain single-crystal graphene domains with a size much larger than that allowed by the nucleation density in the initial growth and efficiently heal structural defects similar to graphitization but at a much lower temperature, both of which are impossible to realize by conventional CVD. Using this method with Pt as a growth substrate, we have grown ∼3 mm defect-free single-crystal graphene domains with a carrier mobility up to 13,000 cm2 V(-1) s(-1) under ambient conditions.