Van der Waals Epitaxial Growth of 2D Metallic Vanadium Diselenide Single Crystals and their Extra‐High Electrical Conductivity

2D metallic transition-metal dichalcogenides (MTMDs) have recently emerged as a new class of materials for the engineering of novel electronic phases, 2D superconductors, magnets, as well as novel electronic applications. However, the mechanical exfoliation route is predominantly used to obtain such metallic 2D flakes, but the batch production remains challenging. Herein, the van der Waals epitaxial growth of monocrystalline, 1T-phase, few-layer metallic VSe₂ nanosheets on an atomically flat mica substrate via a "one-step" chemical vapor deposition method is reported. The thickness of the VSe₂ nanosheets is precisely tuned from several nanometers to several tenths of nanometers. More significantly, the 2D VSe₂ single crystals are found to present an excellent metallic feature, as evidenced by the extra-high electrical conductivity of up to 10⁶ S m⁻¹ , 1-4 orders of magnitude higher than that of various conductive 2D materials. The thickness-dependent charge-density-wave phase transitions are also examined through low-temperature transport measurements, which reveal that the synthesized 2D metallic 1T-VSe₂ nanosheets should serve as good research platforms for the detecting novel many-body states. These results open a new path for the synthesis and property investigations of nanoscale-thickness 2D MTMDs crystals.