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Graphene oxide (GO) monolayer sheets, transferred onto Si by the Langmuir-Blodgett technique, were subjected to ammonia plasma treatment at room temperature with the objective of simultaneous reduction and doping. Scanning electron microscopy and atomic force microscopy studies show that plasma treatment at a relatively low power (∼10 W) for up to 15 min does not affect the morphological stability and monolayer character of GO sheets. X-ray photoelectron spectroscopy has been used to study de-oxygenation of GO monolayers and the incorporation of nitrogen in graphitic-N, pyrrolic-N and pyridinic-N forms due to the plasma treatment. The corresponding changes in the valence band electronic structure, density of states at the Fermi level and work function have been investigated by ultraviolet photoelectron spectroscopy. These studies, supported by Raman spectroscopy and electrical conductivity measurements, have shown that a short duration plasma treatment of up to 5 min results in an increase of sp²-C content along with a substantial incorporation of the graphitic-N form, leading to the formation of n-type reduced GO. Prolonged plasma treatment for longer durations results in a decrease of electrical conductivity, which is accompanied by a substantial decrease of sp²-C and an increase in defects and disorder, primarily attributed to the increase in pyridinic-N content.

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Langmuir-Blodgett monolayer sheets of graphene oxide (GO) were transferred onto Si and SiO2/Si, and subjected to hydrogen plasma treatment near room temperature. GO monolayers were morphologically stable at low power (15 W) plasma treatment, for durations up to 2 min and temperatures up to 120 °C. GO monolayers reduced under optimized plasma treatment conditions (30 s duration at 50 °C) exhibit a sheet thickness of (0.5-0.6) nm, high sp(2)-C content (75%), a low O/C ratio (0.16) and a significant red-shift of Raman G-mode to 1588 cm(-1), indicating efficient de-oxygenation and a substantial decrease of defects. A study of the valence band electronic structure of hydrogen plasma reduced GO monolayers shows an increase of DOS in the vicinity of the Fermi level, due to the increase of C 2p-π states, and a substantial decrease of work function. These results, along with conductivity measurements and transfer characteristics, reveal the p-type nature of hydrogen plasma reduced GO monolayers, displaying a conductivity of (0.2-31) S cm(-1) and a field effect mobility of (0.1-6) cm(2) V(-1) s(-1). Plasma treatment at higher temperatures results in a substantial increase in sp(3)-C/damaged alternant hydrocarbon content and incorporation of defects related to the hydrogenation of the graphitic network, as evidenced by multiple Raman features, including a large red-shift of D-mode to 1331 cm(-1) and a high I(D)/I(G) ratio, and supported by the appearance of mid-gap states in the vicinity of the Fermi level.