AVS 60th International Symposium and Exhibition
    Graphene and Other 2D Materials Focus Topic Thursday Sessions
       Session GR+AS+BI+PS+SS-ThA

Invited Paper GR+AS+BI+PS+SS-ThA10
Epitaxial Graphene Oxide

Thursday, October 31, 2013, 5:00 pm, Room 104 B

Session: Plasma Processing, Surface Chemistry, Functionalization, and Sensor Applications of 2D Materials
Presenter: E. Riedo, Georgia Institute of Technology
Authors: E. Riedo, Georgia Institute of Technology
A. Bongiorno, Georgia Institute of Technology
Y.J. Chabal, University of Texas at Dallas
C. Berger, Georgia Institute of Technology
C. Aruta, CNR
Correspondent: Click to Email

Graphene and graphene-based materials hold great promise for the next generation of nanodevices. One of the most pressing issues for the technological use of graphene is the possibility to control physical and chemical properties by means of ad hoc functionalization. Thermal, chemical and optical reduction of graphene oxide have been explored as a route to produce graphene-based materials with the desired electron transport, mechanical and optical properties. Here, we demonstrate the ability to reduce graphene oxide at the nanoscale by using hot AFM tips (thermochemical nanolithography, TCNL). The resulting nanostructures have a conductivity that can be tune over 4 orders of magnitude [1]. Graphene oxide is indeed a material of great interest for its potential applications in nanoelectronics, nanoelectromechanical system, sensors, polymer composites, catalysis, energy storage devices and optics. However, the chemistry of graphene oxide and its response to external stimuli such as temperature and light are not well understood and only approximately controlled. This understanding is crucial to enable future applications of this material. We have carried over a combined experimental and density functional theory study [2] which shows that multilayer graphene oxide produced by oxidizing epitaxial graphene through the Hummers method is a metastable material whose structure and chemistry evolve at room temperature with a characteristic relaxation time of about one month. At the quasi-equilibrium, graphene oxide reaches a nearly stable reduced O/C ratio, and exhibits a structure deprived of epoxide groups and enriched in hydroxyl groups. This study shows that the structural and chemical changes are driven by the availability of hydrogen in the oxidized graphitic sheets, which favors the reduction of epoxide groups and the formation of water molecules. Furthermore, we have discovered that a mild chemical oxidation of multilayer epitaxial graphene produces uniform oxidized films showing no propensity to exfoliate. XRD measurements show that the epitaxial graphene oxide films are extremely well ordered with an interlayer distance of 10 Å [3].

[1] Z. Q. Wei, D. Wang, S. Kim, Y. Hu, M. K. Yakes, A. Laracuente, Z. Dai, S. Marder, C. Berger, W. P. King, W. A. de Heer, P. E. Sheehan, and E. Riedo, "Nanoscale Tunable Reduction of Graphene Oxide for Graphene Electronics," Science, 328, 1373-1376, (2010).

[2] S. Kim, S. Zhou, Y. Hu, M. Acik, Y. J. Chabal, C. Berger, W. de Heer, A. Bongiorno, and E. Riedo “ Room Temperature Metastability of Multilayer Epitaxial Graphene Oxide”, Nature Materials, 11, 544, (2012).

[3] L. Aruta, Y. Chabal, E. Riedo, A. Bongiorno, (2013).