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Thinning crystalline materials to two dimensions (2D) creates a rich playground for electronic phases, including charge, spin, superconducting and topological order. Bulk materials hosting charge density waves (CDWs), when reduced to ultrathin films, have shown CDW enhancement and tunability. However, charge order confined to only 2D remains elusive. Here we report a distinct charge ordered state emerging in the monolayer limit of 1T-VSe$_2$. Systematic scanning tunneling microscopy experiments reveal that bilayer VSe$_2$ largely retains the bulk electronic structure, hosting a tri-directional CDW. However, monolayer VSe$_2$ exhibits a dimensional crossover, hosting two CDWs with distinct wavelengths. Electronic structure calculations reveal that while one CDW is bulk-like and arises from the well-known Peierls mechanism, the other is decidedly unconventional. The observed CDW-lattice decoupling and the emergence of a flat band suggest that the new CDW arises from enhanced electron-electron interactions in the 2D limit. These findings establish monolayer-VSe$_2$ as the first host of coexisting charge orders with distinct origins, opening the door to tailoring electronic phenomena via emergent interactions in 2D materials.
We have investigated the chiral charge-density wave (CDW) in $1T$-VSe$_2$ using scanning tunneling microscopy (STM) measurements and optical polarimetry measurements. With the STM mesurements, we revealed that the CDW intensities along each triple-$q
Using the Lanczos exact-diagonalization and density-matrix renormalization group methods, we study the extended Hubbard model at quarter filling defined on the anisotropic triangular lattice. We focus on charge ordering (CO) phenomena induced by onsi
To gain insight into the mechanism of charge-ordering transitions, which conventionally are pictured as a disproportionation of an ion M as 2M$^{n+}$ $rightarrow$ M$^{(n+1)+}$ + M$^{(n-1)+}$, we (1) review and reconsider the charge state (or oxidatio
The capability to isolate one to few unit-cell thin layers from the bulk matrix of layered compounds opens fascinating prospects to engineer novel electronic phases. However, a comprehensive study of the thickness dependence and of potential extrinsi
We present a detailed study of the bulk electronic structure of high quality VSe$_{2}$ single crystals using optical spectroscopy. Upon entering the charge density wave phase below the critical temperature of 112 K, the optical conductivity of VSe$_2