Effect of oxygen and nitrogen functionalization on the physical and electronic structure of graphene
graphene, functionalization, chemical vapor deposition, density functional theory
Covalent functionalization of graphene offers opportunities for tailoring its properties and is an unavoidable consequence of some graphene synthesis techniques. However, the changes induced by the functionalization are not well understood. By using atomic sources to control the extent of the oxygen and nitrogen functionalization, we studied the evolution in the structure and properties at the atomic scale. Atomic oxygen reversibly introduces epoxide groups whilst, under similar conditions, atomic nitrogen irreversibly creates diverse functionalities including substitutional, pyridinic, and pyrrolic nitrogen. Atomic oxygen leaves the Fermi energy at the Dirac point (i.e., undoped), whilst atomic nitrogen results in a net n-doping; however, the experimental results are consistent with the dominant electronic effect for both being a transition from delocalized to localized states, and hence the loss of the signature electronic structure of graphene.
Tsinghua University Press
Alexander J. Marsden,Peter Brommer,James J. Mudd,M. Adam Dyson,Robert Cook,María Asensio,Jose Avila,Ana Levy,Jeremy Sloan,David Quigley,Gavin R. Bell,Neil R. Wilson, Effect of oxygen and nitrogen functionalization on the physical and electronic structure of graphene. NanoRes.2015, 8(8): 2620–2635