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We have systematically studied a variety of vanadium dioxide (VO2)crystalline forms, including bulk single crystals and oriented thin films,using infrared (IR) near-field spectroscopic imaging techniques. By measuringthe IR spectroscopic responses of electrons and phonons in VO2 withsub-grain-size spatial resolution (~20 nm), we show that epitaxial strain inVO2 thin films not only triggers spontaneous local phase separations but alsoleads to intermediate electronic and lattice states that are intrinsicallydifferent from those found in bulk. Generalized rules of strain and symmetrydependent mesoscopic phase inhomogeneity are also discussed. These results setthe stage for a comprehensive understanding of complex energy landscapes thatmay not be readily determined by macroscopic approaches.

Phase transition in bulk single crystals and thin films of VO2 by nano-infrared spectroscopy and imaging