Alternative Structure Model of Correlated Charge Density Wave in Monolayer 1T-Nb(Ta)Se₂

The putative Mott charge density wave (CDW) phases of monolayer 1T-NbSe2 and 1T-TaSe2 have attracted a lot of recent interest due to the unexpected orbital texture of their Mott-Hubbard states and the superstructure related to an exotic possibility of a quantum spin liquid with a spinon Fermi surface. The origins of the orbital texture and the superstructure have been, however, elusive. We find by using density functional theory calculations that these CDW phases can have an alternative metastable structure, an anion (Se) centered cluster, in contrast to the prevailing model of a cation (Nb or Ta) centered David star cluster. This structure can be stabilized by the charge transfer from the bilayer graphene/SiC substrate used commonly in the experiments. The anion-centered structure has a similar electronic band structure of a charge transfer insulator to that of DS clusters but naturally explains the orbital texture of the upper Hubbard band from simply its atomic structure. Moreover, this band structure exhibits a Fermi surface nesting to possibly break the symmetry spontaneously into a 3×3-R30° superstructure observed experimentally. The resulting ground state of the superstructure is shown to be a trivial band insulator, in contrast to exotic proposals. This result emphasizes the huge structural flexibility of these heteroexpitaxial monolayers, for which careful studies on atomic structures and interactions with substrates are highly requested.