Understanding adsorption of hydrogen atoms on graphene

Abstract

Adsorption of hydrogen atoms on a single graphite sheet (graphene) has been investigated by first-principles electronic structure means, employing plane-wave based, periodic density functional theory. A reasonably large 5x5 surface unit cell has been employed to study single and multiple adsorption of H atoms. Binding and barrier energies for sequential sticking have been computed for a number of configurations involving adsorption on top of carbon atoms. We find that binding energies per atom range from ~0.8 eV to ~1.9 eV, with barriers to sticking in the range 0.0-0.2 eV. In addition, depending on the number and location of adsorbed hydrogen atoms, we find that magnetic structures may form in which spin density localizes on a $\sqrt{3}x\sqrt{3}R30^{\circ }$ sublattice, and that binding (barrier) energies for sequential adsorption increase (decrease) linearly with the site-integrated magnetization. These results can be rationalized with the help of the valence-bond resonance theory of planar $\pi$ conjugated systems, and suggest that preferential sticking due to barrierless adsorption is limited to formation of hydrogen pairs.

arXiv comment12 pages, 8 figures and 4 tables

References in corpus (18)

• Electric Field Effect in Atomically Thin Carbon Films
• The electronic properties of graphene
• Two-Dimensional Gas of Massless Dirac Fermions in Graphene
• Experimental Observation of Quantum Hall Effect and Berry's Phase in Graphene
• Interstellar Dust Grains
• Magnetism in Graphene Induced by Single-Atom Defects
• Hydrogen on graphene: Electronic structure, total energy, structural distortions, and magnetism from first-principles calculations
• Magnetic Correlations at Graphene Edges
• Disorder Induced Localized States in Graphene
• Magnetic nanographite
• Vacancy induced magnetism in graphene and graphene ribbons
• Magnetism in Disordered Graphene and Irradiated Graphite
• Modeling disorder in graphene
• Charge Transport in Disordered Graphene-Based Low Dimensional Materials
• First principles study of magnetism in nanographenes
• A Defective Graphene Phase Predicted to be a Room Temperature Ferromagnetic Semiconductor
• Hidden multiferroic order in graphene zigzag ribbons
• Kinetic Monte Carlo Studies of Hydrogen Abstraction from Graphite

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