▎ 摘 要
By means of Scanning Tunneling Microscopy (STM) experiments and first-principles calculations, we demonstrate the synergetic effect of the combination of two different strategies to modify the properties of graphene supported on a strongly interacting substrate like Rh. A complete control of the corrugation and doping level is achieved combining the introduction of nitrogen defects and oxygen intercalation. Firstly, we show how to use ion bombardment to obtain purely-substitutional N-doped graphene on Rh(111) with tunable dopant concentration. In a second step, the interaction with the substrate is controlled by the amount of intercalated oxygen atoms. Unlike weakly interacting substrates, the highly corrugated structure of G/Rh(111) leads to remarkable variations of the electronic properties associated with nitrogen defects created in the high and low areas of the moire. After oxygen intercalation, the N-doped graphene layer decouples from the substrate preserving the incorporated nitrogen atoms, which display a subtle dependence of the STM contrast. First-principles calculations confirm the identification of substitutional N-defects and the recovery of the Dirac cone with a tunable shift governed by the nitrogen concentration. Our results support the combination of different modification techniques to tailor structural and electronic properties of graphene and other 2D materials. (c) 2018 Elsevier Ltd. All rights reserved.