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Abstract:
We report on experimental and theoretical investigations of nitrogen-doped graphene. The incorporation of nitrogen was achieved during chemical-vapor deposition on Ni(111) using pyridine as a precursor. The obtained graphene layers were investigated using photoelectron spectroscopy. By studying C 1s and N 1s core levels, we show that the nitrogen content is influenced by the growth temperature and determine the atomic arrangement of the nitrogen atoms. Valence-band photoelectron spectra show that the incorporation of nitrogen leads to a broadening of the photoemission lines and a shift of the π band. Density functional calculations for two possible geometric arrangements, the substitution of carbon atoms by nitrogen and vacancies in the graphene sheet with pyridinic nitrogen at the edges, reveal that the two arrangements have opposite effects on the band structure. For the present experimental approach, vacancies with pyridinic nitrogen are dominant. In the latter case the vacancies generated by the nitrogen doping, not the nitrogen itself, have the main effect on the band structure. By intercalating gold between the doped graphene layer and the Ni(111) substrate electronic decoupling is achieved. After intercalation the doping remains.
