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A superstructure can elicit versatile new properties of materials by breakingtheir original geometrical symmetries. It is an important topic in the layeredgraphene-like two-dimensional transition-metal dichalcogenides (TMDs), but itsorigin remains unclear. Using diamond-anvil cell techniques, synchrotron x-raydiffraction, x-ray absorption, and the first-principles calculations, we showthat the evolution from the weak Van der Waals bonding to the Heisenbergcovalent bonding between layers induces an isostructural transition inquasi-two-dimensional 1$\textit{T}$-type VSe$_2$ at high pressure. Furthermore,our results show that high-pressure induce a novel superstructure at 15.5 GPa,rather than suppress as it would normally, which is unexpected. It is driven bythe Fermi surface nesting, enhanced by the pressure-induced distortion. Theresults suggest that the superstructure not only appears in the two-dimensionalstructure but also can emerge in the pressure-tuned three-dimensional structurewith new symmetry and develop superconductivity.

Novel Superstructure-Phase Two-Dimensional Material 1$\textit{T}$-VSe$_2$ at High Pressure