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Through ${in~situ}$ photoemission spectroscopy, we investigated the change inthe electronic and crystal structures of dimensionality-controlled VO$_2$ filmscoherently grown on TiO$_2$(001) substrates. In the nanostructured films, thebalance between the instabilities of a bandlike Peierls transition and a Motttransition is controlled as a function of thickness. The characteristicspectral change associated with temperature-driven metal-insulator transitionin VO$_2$ thick films holds down to 1.5 nm (roughly corresponding to five Vatoms along the [001] direction), whereas VO$_2$ films of less than 1.0 nmexhibit insulating nature without V-V dimerization. These results suggest thatthe delicate balance between a Mott instability and a bandlike Peierlsinstability is modulated at a scale of a few nanometers by the dimensionalcrossover effects and confinement effects, which consequently induce thecomplicated electronic phase diagram of ultrathin VO$_2$ films.

Thickness dependence of electronic and crystal structures in VO$_2$ ultrathin films: suppression of the collaborative Mott-Peierls transition