Epitaxial VO2 thin films grown on (1120) sapphire (α-Al2O3) substrates by MOCVD at 600 °C have been characterized by conventional electron microscopy and high resolution electron microscopy (HREM). Three different epitaxial relationships between the monoclinic VO2 films and sapphire substrates have been found at room temperature: I. (200)  monoclinic VO2 ‖ (1120)  sapphire, II. (002)  monoclinic VO2 ‖ (1120)  sapphire, and III. (020)  monoclinic VO2 ‖ (1120)  sapphire. Expitaxial relationships II and III are equivalent to each other when the film possesses tetragonal structure at the deposition temperature; i.e., they can be described as (010)  tetragonal VO2 ‖ (1120)  sapphire and (100)  tetragonal VO2 ‖ (1120)  sapphire. HREM image shows that the initial nucleation of the film was dominated by the first orientation relationship, but the film then grew into the grains of the second and the third (equivalent to each other at the deposition temperature) epitaxial relationships. Successive 90°transformation rotational twins around the a-axis are commonly observed in the monoclinic films.
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