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The synthesis of new graphene‐based quantum materials by intercalation is an auspicious approach. However, an accompanying proximity coupling depends crucially on the structural details of the new heterostructure. It is studied in detail the Pb monolayer structure after intercalation into the graphene buffer layer on the SiC(0001) interface by means of photoelectron spectroscopy, x‐ray standing waves, and scanning tunneling microscopy. A coherent fraction close to unity proves the formation of a flat Pb monolayer on the SiC surface. An interlayer distance of 3.67 Å to the suspended graphene underlines the formation of a truly van der Waals heterostructure. The 2D Pb layer reveals a quasi ten‐fold periodicity due to the formation of a grain boundary network, ensuring the saturation of the Si surface bonds. Moreover, the densely‐packed Pb layer also efficiently minimizes the doping influence by the SiC substrate, both from the surface dangling bonds and the SiC surface polarization, giving rise to charge‐neutral monolayer graphene. The observation of a long‐ranged (3×3$\sqrt {3}\times \sqrt {3}$) reconstruction on the graphene lattice at tunneling conditions close to Fermi energy is most likely a result of a nesting condition to be perfectly fulfilled. [ABSTRACT FROM AUTHOR]

Abstract The synthesis of new graphene‐based quantum materials by intercalation is an auspicious approach. However, an accompanying proximity coupling depends crucially on the structural details of the new heterostructure. It is studied in detail the Pb monolayer structure after intercalation into the graphene buffer layer on the SiC(0001) interface by means of photoelectron spectroscopy, x‐ray standing waves, and scanning tunneling microscopy. A coherent fraction close to unity proves the formation of a flat Pb monolayer on the SiC surface. An interlayer distance of 3.67 Å to the suspended graphene underlines the formation of a truly van der Waals heterostructure. The 2D Pb layer reveals a quasi ten‐fold periodicity due to the formation of a grain boundary network, ensuring the saturation of the Si surface bonds. Moreover, the densely‐packed Pb layer also efficiently minimizes the doping influence by the SiC substrate, both from the surface dangling bonds and the SiC surface polarization, giving rise to charge‐neutral monolayer graphene. The observation of a long‐ranged (3×3) reconstruction on the graphene lattice at tunneling conditions close to Fermi energy is most likely a result of a nesting condition to be perfectly fulfilled.