Graphene on the carbon face of SiC: electronic structure modification by hydrogen intercalation

TL;DR

This study uses density functional theory to explore how native interface defects and hydrogen intercalation affect the electronic structure of graphene on the C face of SiC, revealing defect-driven doping mechanisms.

Contribution

It provides new insights into how native interface defects and hydrogen intercalation modify the electronic properties of graphene on SiC, highlighting the importance of interface defect management.

Findings

Hydrogen intercalation dopes graphene with electrons from the substrate.

Native interface defects influence doping mechanisms on C-terminated SiC.

Complete removal of reconstruction is needed for effective passivation with hydrogen.

Abstract

It has been shown that the first C layer on the SiC(0001)(2{\times}2)C surface already exhibits graphene-like electronic structure, with linear pi bands near the Dirac point. Indeed, the (2{\times}2)C reconstruction, with a Si adatom and C restatom structure, efficiently passivates the SiC(0001) surface thanks to an adatom/restatom charge transfer mechanism. Here, we study the effects of interface modifications on the graphene layer using density functional theory calculations. The modifications we consider are inspired from native interface defects observed by scanning tunneling microscopy. One H atom per 4 {\times} 4 SiC cell (5 {\times} 5 graphene cell) is introduced in order to saturate a restatom dangling bond and hinder the adatom/restatom charge transfer. As a consequence, the graphene layer is doped with electrons from the substrate and the interaction with the adatom states slightly increases. Native interface defects are therefore likely to play an important role in the doping mechanism on the C terminated SiC substrates. We also conclude that an efficient passivation of the C face of SiC by H requires a complete removal of the reconstruction. Otherwise, at variance with the Si terminated SiC substrates, the presence of H at the interface would increase the graphene/substrate interaction.