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.

12 pages, 8 figures and 4 tables

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• Ab initio simulations of the kinetic properties of the hydrogen monomer on graphene
• Hydrogenation-induced ferromagnetism on graphite surfaces
• Adsorption of Hydrogen in Graphene without Band Gap Opening at the Dirac Point
• A theoretical study of the dynamics of atomic hydrogen on graphene bilayers
• Nearly Free Electron States in Graphane Nanoribbon Superlattice
• A kinetic Monte Carlo study of desorption of H2 from graphite (0001)
• First-principles study of bandgap effects in graphene due to hydrogen adsorption
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• Spin-Polarized Semiconductor Induced by Magnetic Impurities in Graphene