Multiple charge density wave phases of monolayer VSe2manifested by graphene substrates.

A combined study of scanning tunneling microscopy (STM) and angle-resolved photoemission spectroscopy (ARPES) is conducted to understand the multiple charge density wave (CDW) phases of monolayer (ML) VSe2films manifested by graphene substrates. Submonolayer (∼0.8 ML) VSe2films are prepared on two different substrates of single-layer graphene (SLG) and bi-layer graphene (BLG) on a 6H-SiC(0001). We find that ML VSe2films are less coupled to the SLG substrate compared to that of ML VSe2/BLG. Then, ML VSe2grown on SLG and BLG substrates reveals a very different topography in STM. While ML VSe2/BLG shows one unidirectional modulation of √3 × 2 and √3 × âˆš7 CDW in topography, ML VSe2/SLG presents a clear modulation of 4 × 1 CDW interfering with √3 × 2 and √3 × âˆš7 CDW which has not been previously observed. We explicitly show that the reciprocal vector of 4 × 1 CDW fits perfectly into the long parallel sections of cigar-shaped Fermi surfaces near the M point in ML VSe2, satisfying Fermi surface nesting. Since bulk VSe2is also well-known for the 4 × 4 × 3 CDW formed by Fermi surface nesting, the 4 × 1 CDW in ML VSe2/SLG is attributed to the planar projection of 4 × 4 × 3 CDW in bulk. Our result clarifies the nature of the 4 × 1 CDW in ML VSe2system and is a good example demonstrating the essential role of substrates in two-dimensional transition metal dichalcogenides.

Emergence of a Metal-Insulator Transition and High-Temperature Charge-Density Waves in VSe2 at the Monolayer Limit.

Emergent phenomena driven by electronic reconstructions in oxide heterostructures have been intensively discussed. However, the role of these phenomena in shaping the electronic properties in van der Waals heterointerfaces has hitherto not been established. By reducing the material thickness and forming a heterointerface, we find two types of charge-ordering transitions in monolayer VSe2 on graphene substrates. Angle-resolved photoemission spectroscopy (ARPES) uncovers that Fermi-surface nesting becomes perfect in ML VSe2. Renormalization-group analysis confirms that imperfect nesting in three dimensions universally flows into perfect nesting in two dimensions. As a result, the charge-density wave-transition temperature is dramatically enhanced to a value of 350 K compared to the 105 K in bulk VSe2. More interestingly, ARPES and scanning tunneling microscopy measurements confirm an unexpected metal-insulator transition at 135 K that is driven by lattice distortions. The heterointerface plays an important role in driving this novel metal-insulator transition in the family of monolayer transition-metal dichalcogenides.