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The thickness-dependent epitaxial strains and phase transformations of (001)-VO2/TiO2 thin films are investigated systematically in a wide thickness range (from 9 to 150 nm). Under a thickness of 18 nm, the tensile in-plane strain is maintained, owing to the good lattice and the symmetry matching between the VO2 thin film and the TiO2 substrate, but the compressive out-of-plane epitaxial strain is gradually relaxed. The epitaxial strains co-stabilize the rutile phase (R phase) in this thickness range. Beyond a thickness of 18 nm, the out-of-plane lattice c exhibits a sudden elongation and reaches the bulk level of 2.8528 Å at a thickness of 20 nm, which indicates a structural phase transition (SPT). A further increase of the film thickness results in another new phase (tetragonal-like or T-like) with lattice distortion, which maintains the tetragonal symmetry in the thickness range of 20 to 55 nm. From a thickness of 60 nm, the monoclinic phase (M1 phase) appears, which indicates another SPT from T-like to the monoclinic M1 phase. This SPT is more favorable energetically, owing to the assistance of the strain relaxation in the thicker films. Additionally, the metal-insulator transition temperature positively increases as a function of the out-of-plane strain. This result is consistent with the fact that the tensile strain along the cR axis (V-V atom chain) is conducive for the stabilized insulating phase. This work highlights strain engineering as a crucial avenue for manipulating the phase transformations and properties in the correlated electron system.

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