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ACS Nano ; 9(7): 7314-22, 2015 Jul 28.
Artigo em Inglês | MEDLINE | ID: mdl-26121999


Embedding foreign atoms or molecules in graphene has become the key approach in its functionalization and is intensively used for tuning its structural and electronic properties. Here, we present an efficient method based on chemical vapor deposition for large scale growth of boron-doped graphene (B-graphene) on Ni(111) and Co(0001) substrates using carborane molecules as the precursor. It is shown that up to 19 at. % of boron can be embedded in the graphene matrix and that a planar C-B sp(2) network is formed. It is resistant to air exposure and widely retains the electronic structure of graphene on metals. The large-scale and local structure of this material has been explored depending on boron content and substrate. By resolving individual impurities with scanning tunneling microscopy we have demonstrated the possibility for preferential substitution of carbon with boron in one of the graphene sublattices (unbalanced sublattice doping) at low doping level on the Ni(111) substrate. At high boron content the honeycomb lattice of B-graphene is strongly distorted, and therefore, it demonstrates no unballanced sublattice doping.

Nano Lett ; 14(9): 4982-8, 2014 Sep 10.
Artigo em Inglês | MEDLINE | ID: mdl-25136909


Many propositions have been already put forth for the practical use of N-graphene in various devices, such as batteries, sensors, ultracapacitors, and next generation electronics. However, the chemistry of nitrogen imperfections in this material still remains an enigma. Here we demonstrate a method to handle N-impurities in graphene, which allows efficient conversion of pyridinic N to graphitic N and therefore precise tuning of the charge carrier concentration. By applying photoemission spectroscopy and density functional calculations, we show that the electron doping effect of graphitic N is strongly suppressed by pyridinic N. As the latter is converted into the graphitic configuration, the efficiency of doping rises up to half of electron charge per N atom.

ACS Nano ; 6(12): 10590-7, 2012 Dec 21.
Artigo em Inglês | MEDLINE | ID: mdl-23157662


We report high-resolution scanning tunneling microscopy and spectroscopy of hydrogenated, quasi-free-standing graphene. For this material, theory has predicted the appearance of a midgap state at the Fermi level, and first angle-resolved photoemission spectroscopy (ARPES) studies have provided evidence for the existence of this state in the long-range electronic structure. However, the spatial extension of H defects, their preferential adsorption patterns on graphene, or local electronic structure are experimentally still largely unexplored. Here, we investigate the shapes and local electronic structure of H impurities that go with the aforementioned midgap state observed in ARPES. Our measurements of the local density of states at hydrogenated patches of graphene reveal a hydrogen impurity state near the Fermi level whose shape depends on the tip position with respect to the center of a patch. In the low H concentration regime, we further observe predominantly single hydrogenation sites as well as extended multiple C-H sites in parallel orientation to the lattice vectors, indicating an adsorption at the same graphene sublattice. This is corroborated by ARPES measurements showing the formation of a dispersionless hydrogen impurity state which is extended over the whole Brillouin zone.

J Phys Condens Matter ; 24(23): 235304, 2012 Jun 13.
Artigo em Inglês | MEDLINE | ID: mdl-22581023


Hydrogen adsorption on graphene in commensurate periodic arrangements leads to bandgap opening at the Dirac point and the emergence of dispersionless midgap bands. We study these bandgap effects and their dependence on periodicity for a single hydrogen adsorbate on periodic graphene supercells using spin-polarized density-functional theory calculations. Our results show that for certain periodicities, marked by a scale factor of three, the bandgap is suppressed to a great extent, and has a special level structure around the neutrality point. We present explanations for the origin of the changes to the band structure in terms of the ab initio Hamiltonian matrix. This method may be used to obtain a more accurate tight-binding description of single hydrogen adsorption on graphene.