We report the growth of ultrathin VO2 films on rutile TiO2 (001) substrates via reactive molecular-beam epitaxy. The films were formed by the cyclical deposition of amorphous vanadium and its subsequent oxidation and transformation to VO2 via solid-phase epitaxy. Significant metal-insulator transitions were observed in films as thin as 2.3 nm, where a resistance change ΔR/R of 25 was measured. Low angle annular dark field scanning transmission electron microscopy was used in conjunction with electron energy loss spectroscopy to study the film/substrate interface and revealed the vanadium to be tetravalent and the titanium interdiffusion to be limited to 1.6 nm.
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