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Two-dimensional layered and atomically thin elemental superconductors may bekey ingredients in next-generation quantum technologies, if they can bestabilized and integrated into heterostructured devices under ambientconditions. However, atomically thin elemental superconductors are largelyunexplored outside ultra-high vacuum due to rapid oxidation, and even 2Dlayered superconductors require complex encapsulation strategies to maintainmaterial quality. Here we demonstrate environmentally stable, single-crystal,few-atom-thick superconducting gallium, 2D-Ga, produced by confinementheteroepitaxy (CHet) at the interface of epitaxial graphene (EG) and siliconcarbide (SiC). 2D-Ga becomes superconducting at 4 K; this elevation over bulkalpha-Ga (Tc~1 K) is primarily attributed to an increased density of states atthe Fermi level as the incipient Ga-Ga dimerization seen in alpha-Ga issuppressed by epitaxy to SiC. We also demonstrate the importance of controllingSiC surface morphology (i.e. step height) and defect-engineering in graphenelayers prior to intercalation to achieve large-area uniform 2D-Ga layers withisotropic transport properties. This work demonstrates that unique 2D forms of3D materials can be stabilized at the EG/SiC interface, which represents ascalable route towards air-stable crystalline 2D superconductors as a potentialfoundation for next-generation quantum technologies.

An Air-Stable and Atomically Thin Graphene/Gallium Superconducting Heterostructure