Highly conductive, monolayer and large-area reduced graphene oxide films fabricated by electrical connection at the two-dimensional boundaries between the tiled graphene oxide flakes

• Graphene oxide flakes were tiled on an insulating substrates and reduced.
• Highly conductive, continuous reduced-Graphene-Oxide films were fabricated.
• Restoration of entire conductivity relies on formation of continuous films.
• Factors for the restoration of entire conductivity of the films are proposed.

The demand to fabricate graphene film in large wafer-scale with minimum cost is crucial for device applications, and one of the promising techniques is the reduction of graphene oxide (GO) films. We have investigated morphological changes of large-area, monolayer GO films during methane (CH4)-assisted thermal annealing process and the role of CH4 in the restoration of their electrical conductivity. We have discovered that long reduction process in high CH4 flow rates can contribute to the partial reparation of lattice defects and formation of new multilayer graphene that are stacked at the boundary areas between the reduced GO (rGO) flakes. These multilayer graphene layers with graphitic domains operate as the electrical connection between the separated rGO flakes and create new conduction pathways across the entire films. This phenomenon is more important than the sole reduction process (elimination of oxygen functional groups) in the restoration of electrical conductivity of the continuous rGO films. We have achieved in the fabrication of highly conductive rGO films with a minimum sheet resistance value of 1.01 kΩ/sq. This study exhibits a promising reduction method for the mass production of large-area, continuous rGO films for thin film device applications.