Direct Observation of Ordered Configurations of Hydrogen Adatoms on Graphene

Ordered configurations of hydrogen adatoms on graphene have long been proposed, calculated, and searched for. Here, we report direct observation of several ordered configurations of H adatoms on graphene by scanning tunneling microscopy. On the top side of the graphene plane, H atoms in the configurations appear to stick to carbon atoms in the same sublattice. Scanning tunneling spectroscopy measurements revealed a substantial gap in the local density of states in H-contained regions as well as in-gap states below the conduction band due to the incompleteness of H ordering. These findings can be well explained by density functional theory calculations based on double-sided H configurations. In addition, factors that may influence H ordering are discussed.