The Role of Surface Oxygen in the Growth of Large Single-Crystal Graphene on Copper

• Published in: Science (American Association for the Advancement of Science) Vol. 342; no. 6159; pp. 720 - 723
• Main Authors: Hao, Yufeng, Bharathi, M. S., Wang, Lei, Liu, Yuanyue, Chen, Hua, Nie, Shu, Wang, Xiaohan, Chou, Harry, Tan, Cheng, Fallahazad, Babak, Ramanarayan, H., Magnuson, Carl W., Tutuc, Emanuel, Yakobson, Boris I., McCarty, Kevin F., Zhang, Yong-Wei, Kim, Philip, Hone, James, Colombo, Luigi, Ruoff, Rodney S.
• Format: Journal Article
• Language: English
• Published: Washington, DC American Association for the Advancement of Science 08.11.2013; The American Association for the Advancement of Science
• Subjects: Chemical vapor deposition (including plasma-enhanced cvd, mocvd, etc.); Copper; Cross-disciplinary physics: materials science; rheology; Crystallography; Crystals; DIFFUSION; ELECTRICAL CONDUCTIVITY; Electrical resistivity; Exact sciences and technology; Grants; Graphene; Kinetics; Material films; Materials science; Mathematical functions; METHANE; Methods of deposition of films and coatings; film growth and epitaxy; NUCLEATION; OXYGEN; Physics; Resistivity; Species; Scanning electron microscopy; Oxygen; Domain growth; CVD; Monocrystals; Graphene; Residual impurity; Transition elements; Growth mechanism; Kinetics; Nucleation density; Copper; Microstructure; Passivation
• ISSN: 0036-8075; 1095-9203
• DOI: 10.1126/science.1243879

The growth of high-quality single crystals of graphene by chemical vapor deposition on copper (Cu) has not always achieved control over domain size and morphology, and the results vary from lab to lab under presumably similar growth conditions. We discovered that oxygen (O) on the Cu surface substantially decreased the graphene nucleation density by passivating Cu surface active sites. Control of surface O enabled repeatable growth of centimeter-scale single-crystal graphene domains. Oxygen also accelerated graphene domain growth and shifted the growth kinetics from edge-attachment-limited to diffusion-limited. Correspondingly, the compact graphene domain shapes became dendritic. The electrical quality of the graphene films was equivalent to that of mechanically exfoliated graphene, in spite of being grown in the presence of O.