Vanadium dichalcogenides have attracted increasing interests for the charge density wave phenomena and possible ferromagnetism. Here, we report on the multiphase behavior and gap opening in monolayer VTe2 grown by molecular beam epitaxy. Scanning tunneling microscopy (STM) and spectroscopy study revealed the (4×4) metallic and gapped (2√3×2√3) charge-density wave (CDW) phases with an energy gap of ~40 meV. Through the in-plane condensation of vanadium atoms, the typical star-of-David clusters and truncated triangle-shaped clusters are formed in the (4×4) and (2√3×2√3) phases respectively, resulting in different surface morphologies and electronic structures as confirmed by density functional theory (DFT) calculations with on-site Coulomb repulsion. The CDW-driven reorganization of the atomic structure weakens the ferromagnetic superexchange coupling and strengthens the antiferromagnetic exchange coupling on the contrary, suppressing the long-range magnetic order in monolayer VTe2.The electron correlation is found to be important to explain the gap opening in the (2√3×2√3) phase.
/ 18Two-dimensional (2D) transition-metal dichalcogenides (TMDs) are recently attracting great attention for their diverse physical properties such as ferromagnetism 1,2 , Mott-insulator phase 3,4 , quantum Hall effect 5-7 , superconductivity and charge density wave (CDW) [8][9][10][11] . CDW is a periodic symmetry-lowering redistribution of charge in a material, accompanied with periodic modulation of the atomic lattice and electronic densities. The CDW transition in the group VB dichalcogenides, such as VS2, VSe2, NbSe2, TaS2, TaSe2 and TaTe2, has been extensively studied [12][13][14][15][16][17][18][19][20] . The phase transition exhibits a layer-dependent behavior, for instance, VSe2 and NbSe2 have increased CDW transition temperatures as the thicknesses reduce down to a few monolayers. In monolayer VSe2 and NbSe2, the TCDW can be enhanced to 140 K and 145 K compared to 110 K and 33 K of the bulk TCDW respectively [21][22][23][24] . The intricate interplay between CDW and other collective electronic states such as superconductivity has also been explored in NbSe2 and TaS2 25,26 . While the driving mechanisms of CDW in twodimensional TMDs consisting of Fermi surface nesting 27,28 , saddle point singularities 29,30 and electron-phonon coupling [31][32][33][34] have been proposed, a consistent picture on the CDW formation is still to emerge.As for VTe2, CDW phase transition has been observed in VTe2 thin films as the change of resistance at 240 K and 135 K, which can be driven by an electric field due to local Joule heating 35 . When the thickness reduces from multilayer to single layer, the absence of interlayer interaction result in the structural transition from a monoclinic distorted 1Tʹ structure to a hexagonal 1T structure 36 . The 1Tʹ structure has a (3×1) double zigzag chain-like modulation of V atoms, which arise from the in-plane metal coordination through d orbital hybridization. As the temperature is cooled below TCDW, the mo...