A Systematic Study of Electronic Structure from Graphene to Graphane

TL;DR

This study investigates how hydrogenation transforms graphene's electronic properties into graphane using density functional theory, revealing inhomogeneous metallic and insulating phases and potential for electronic patterning.

Contribution

It provides a detailed analysis of electronic structure changes across various hydrogen concentrations, highlighting the formation of metallic islands and insulating regions, and demonstrates tunable electronic properties through hydrogen patterning.

Findings

Hydrogenation favors clustered configurations forming compact islands.

Graphene transitions from semi-metal to metal to insulator with increasing hydrogen coverage.

Patterning hydrogen removal can induce a band gap of 1.4 eV.

Abstract

While graphene is a semi-metal, a recently synthesized hydrogenated graphene called graphane, is an insulator. We have probed the transformation of graphene upon hydrogenation to graphane within the framework of density functional theory. By analyzing the electronic structure for eighteen different hydrogen concentrations, we bring out some novel features of this transition. Our results show that the hydrogenation favors clustered configurations leading to the formation of compact islands. The analysis of the charge density and electron localization function (ELF) indicates that as hydrogen coverage increases the semi-metal turns into a metal showing a delocalized charge density, then transforms into an insulator. The metallic phase is spatially inhomogeneous in the sense, it contains the islands of insulating regions formed by hydrogenated carbon atoms and the metallic channels formed by contiguous bare carbon atoms. It turns out that it is possible to pattern the graphene sheet to tune the electronic structure. For example removal of hydrogen atoms along the diagonal of the unit cell yielding an armchair pattern at the edge gives rise to a band gap of 1.4 eV. We also show that a weak ferromagnetic state exists even for a large hydrogen coverage whenever there is a sub-lattice imbalance in presence of odd number of hydrogen atoms.