A van der Waals Heterostructure with an Electronically Textured Moiré Pattern: PtSe 2 /PtTe 2 .

The interlayer interaction in Pt-dichalcogenides strongly affects their electronic structures. The modulations of the interlayer atom-coordination in vertical heterostructures based on these materials are expected to laterally modify these interlayer interactions and thus provide an opportunity to texture the electronic structure. To determine the effects of local variation of the interlayer atom coordination on the electronic structure of PtSe 2 , van der Waals heterostructures of PtSe 2 and PtTe 2 have been synthesized by molecular beam epitaxy. The heterostructure forms a coincidence lattice with 13 unit cells of PtSe 2 matching 12 unit cells of PtTe 2 , forming a moiré superstructure. The interaction with PtTe 2 reduces the band gap of PtSe 2 monolayers from 1.8 eV to 0.5 eV. While the band gap is uniform across the moiré unit cell, scanning tunneling spectroscopy and d I /d V mapping identify gap states that are localized within certain regions of the moiré unit cell. Deep states associated with chalcogen p z -orbitals at binding energies of ∼ -2 eV also exhibit lateral variation within the moiré unit cell, indicative of varying interlayer chalcogen interactions. Density functional theory calculations indicate that local variations in atom coordination in the moiré unit cell cause variations in the charge transfer from PtTe 2 to PtSe 2 , thus affecting the value of the interface dipole. Experimentally this is confirmed by measuring the local work function by field emission resonance spectroscopy, which reveals a large work function modulation of ∼0.5 eV within the moiré structure. These results show that the local coordination variation of the chalcogen atoms in the PtSe 2 /PtTe 2 van der Waals heterostructure induces a nanoscale electronic structure texture in PtSe 2 .