The stacking of different two-dimensional (2D) materials provides a promising approach to realize new states of quantum matter. In this combined scanning tunneling microscopy (STM) and density functional theory (DFT) study we show that the structure in weakly bound, purely van der Waals (vdW) interacting systems is strongly influenced by screening and relaxation. We studied in detail the physisorption of lead phthalocyanine (PbPc) molecules on epitaxial monolayer graphene on SiC(0001) as well as on highly ordered pyrolytic graphite (HOPG), resembling truly 2D and anisotropic, semi-infinite three-dimensional (3D) supports. Our analysis demonstrates that the different deformation ability of the vdW coupled systems, i.e., their actual thickness and buckling, triggers the molecular morphology and exhibits a proximity coupled band structure. It thus provides important implications for future 2D design concepts.

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• Graphene
• Band structure methods
• Density functional theory
• Scanning tunneling microscopy