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Epitaxial films of vanadium dioxide (VO 2 ) on rutile TiO 2 substrates provide a means of strain-engineering the transition pathways and stabilizing of the intermediate phases between monoclinic (insulating) M1 and rutile (metal) R end phases. In this work, we investigate structural behavior of epitaxial VO 2 thin films deposited on isostructural MgF 2 (001) and (110) substrates via temperature-dependent Raman microscopy analysis. The choice of MgF 2 substrate clearly reveals how elongation of V–V dimers accompanied by the shortening of V–O bonds triggers the intermediate M2 phase in the temperature range between 70–80 °C upon the heating–cooling cycles. Consistent with earlier claims of strain-induced electron correlation enhancement destabilizing the M2 phase our temperature-dependent Raman study supports a small temperature window for this phase. The similarity of the hysteretic behavior of structural and electronic transitions suggests that the structural transitions play key roles in the switching properties of epitaxial VO 2 thin films. 

Straining the vanadium dimers along the rutilec‐axis can be used to tune the metal‐to‐insulator transition (MIT) of VO₂but has thus far been limited to TiO₂substrates. In this work VO₂/MgF₂epitaxial films are grown via molecular beam epitaxy (MBE) to strain engineer the transition temperature (T_MIT). First, growth parameters are optimized by varying the synthesis temperature of the MgF₂(001) substrate (T_S) using a combination of X‐ray diffraction techniques, temperature dependent transport, and soft X‐ray photoelectron spectroscopy. It is determined thatT_Svalues greater than 350 °C induce Mg and F interdiffusion and ultimately the relaxation of the VO₂layer. Using the optimized growth temperature, VO₂/MgF₂(101) and (110) films are then synthesized. The three film orientations display MITs with transition temperatures in the range of 15–60 °C through precise strain engineering.