Resolving the Controversial Existence of Silicene and Germanene Nanosheets Grown on Graphite

The highly oriented pyrolytic graphite (HOPG) surface, consisting of a dangling bond-free lattice, is regarded as a potential substrate for van der Waals heteroepitaxy of two-dimensional layered materials. In this work, the growth of silicon and germanium on HOPG is investigated with scanning tunneling microscopy by using typical synthesis conditions for silicene and germanene on metal surfaces. At low coverages, the deposition of Si and Ge gives rise to tiny and sparse clusters that are surrounded by a honeycomb superstructure. From the detailed analysis of the superstructure, its comparison with the one encountered on the bare and clean HOPG surface, and simulations of the electron density, we conclude that the superstructure is caused by charge density modulations in the HOPG surface. At high coverages, we find the formation of clusters, assembled in filamentary patterns, which indicates a Volmer-Weber growth mode instead of a layer-by-layer growth mode. This coverage-dependent study sets the stage for revisiting recent results alleging the synthesis of silicene and germanene on the HOPG surface.