Long-range interactions between substitutional nitrogen dopants in graphene: Electronic properties calculations

Philippe Lambin, Hakim Amara, Francois Ducastelle, L. Henrard

Résultats de recherche: Contribution à un journal/une revueArticle

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Résumé

Being a true two-dimensional crystal, graphene has special properties. In particular, a pointlike defect in graphene may induce perturbations in the long range. This characteristic questions the validity of using a supercell geometry in an attempt to explore the properties of an isolated defect. Still, this approach is often used in ab initio electronic structure calculations, for instance. How does this approach converge with the size of the supercell is generally not tackled for the obvious reason of keeping the computational load to an affordable level. The present paper addresses the problem of substitutional nitrogen doping of graphene. DFT calculations have been performed for 9×9 and 10×10 supercells. Although these calculations correspond to N concentrations that differ by ∼10%, the local densities of states on and around the defects are found to depend significantly on the supercell size. Fitting the DFT results by a tight-binding Hamiltonian makes it possible to explore the effects of a random distribution of the substitutional N atoms, in the case of finite concentrations, and to approach the case of an isolated impurity when the concentration vanishes. The tight-binding Hamiltonian is used to calculate the STM image of graphene around an isolated N atom. STM images are also calculated for graphene doped with 0.5 at% concentration of nitrogen. The results are discussed in the light of recent experimental data and the conclusions of the calculations are extended to other point defects in graphene.
langue originaleAnglais
Numéro d'article045448
Nombre de pages10
journalPhys. Rev. B
Volume86
Numéro de publication4
Les DOIs
étatPublié - 27 juil. 2012

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Graphite
Electronic properties
Graphene
graphene
Nitrogen
Doping (additives)
nitrogen
electronics
Hamiltonians
interactions
Discrete Fourier transforms
Defects
defects
Atoms
Point defects
statistical distributions
point defects
Electronic structure
atoms
Impurities

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abstract = "Being a true two-dimensional crystal, graphene has special properties. In particular, a pointlike defect in graphene may induce perturbations in the long range. This characteristic questions the validity of using a supercell geometry in an attempt to explore the properties of an isolated defect. Still, this approach is often used in ab initio electronic structure calculations, for instance. How does this approach converge with the size of the supercell is generally not tackled for the obvious reason of keeping the computational load to an affordable level. The present paper addresses the problem of substitutional nitrogen doping of graphene. DFT calculations have been performed for 9×9 and 10×10 supercells. Although these calculations correspond to N concentrations that differ by ∼10{\%}, the local densities of states on and around the defects are found to depend significantly on the supercell size. Fitting the DFT results by a tight-binding Hamiltonian makes it possible to explore the effects of a random distribution of the substitutional N atoms, in the case of finite concentrations, and to approach the case of an isolated impurity when the concentration vanishes. The tight-binding Hamiltonian is used to calculate the STM image of graphene around an isolated N atom. STM images are also calculated for graphene doped with 0.5 at{\%} concentration of nitrogen. The results are discussed in the light of recent experimental data and the conclusions of the calculations are extended to other point defects in graphene.",
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Long-range interactions between substitutional nitrogen dopants in graphene: Electronic properties calculations. / Lambin, Philippe; Amara, Hakim; Ducastelle, Francois; Henrard, L.

Dans: Phys. Rev. B, Vol 86, Numéro 4, 045448, 27.07.2012.

Résultats de recherche: Contribution à un journal/une revueArticle

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