We report a direct observation of the electronic structure of monolayer SnTe on graphene by angle-resolved photoemission spectroscopy. By combining low-energy electron diffraction, momentum microscopy, core-level spectroscopy, and first-principles calculations, we show that the observed monolayer-limit electronic structure is consistent with a puckered even-layer biatomic-layer building block rather than a nonpuckered square-flat structure. The observed band dispersion and its polarization dependence are reproduced by a puckered structure with a substrate-renormalized buckling amplitude. We further show that graphene actively interacts with ultrathin SnTe by selecting its in-plane orientational texture, renormalizing the buckling amplitude, and modifying the local interfacial electrostatic environment in the monolayer limit. In comparison, multilayer SnTe exhibits a more ringlike momentum-space distribution, interlayer-split valence bands, and a stronger $p$-type character, revealing the onset of thickness evolution from an interface-stabilized puckered ultrathin limit toward a more bulklike state.

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• Ferroelectricity
• Spin-orbit coupling
• 2-dimensional systems
• Interfaces
• Angle-resolved photoemission spectroscopy
• Low-energy electron diffraction