Graphene meets gallenene -- A straightforward approach to developing large-area heterostacks by gallium self-propagation

Gallenene is an atomically thin two-dimensional metallene that to be considered as a potential candidate for accessing new ways of developing ultra-thin gallium-based semiconductor devices. Using the solidmelt exfoliation technique, we demonstrate the feasibility of fabricating a gallenene film on epitaxial graphene substrates with lateral sizes approaching the centimeter scale. The stepwise self-propagation of gallenene across the epitaxial graphene surface on the macroscopic scale was observed by optical microscopy at room temperature shortly after initial processing without any further physical or chemical treatment of the sample. On the other hand, evidence for the occurrence of epitaxial graphene intercalation through the gallenene propagation leading to a transformation into quasi-freestanding bilayer graphene (QFBLG) has been observed by confocal micro-Raman spectroscopy. The results reveal a new pathway for a controlled fabrication of two-dimensional heterostructures and stacks based on interaction between a liquid metal and epitaxial graphene.