Nano-optical Investigations of the Metal-Insulator Phase Behavior of Individual VO2 Microcrystals

Despite the relatively simple stoichiometry and structure of VO2, many questions regarding the nature of its famous metal insulator transition (MIT) remain unresolved, This is in part due to the prevailing use of polycrystalline film samples and the limited spatial resolution in most studies, hindering access to and control of the complex phase behavior and its inevitable spatial inhomogeneities. Here, we investigate the MIT and associated nanodomain formation in individual VO2 microcrystals subject to substrate stress. We employ symmetry-selective polarization Raman spectroscopy to identify crystals that are strain-stabilized in either the monoclinic M1 or M2 insulating phase at room-temperature. Raman measurements are further used to characterize the phase dependence on temperature, identifying the appearance of the M2 phase during the MIT. The associated formation and spatial evolution of rutile (R) metallic domains is studied with nanometer-scale spatial resolution using infrared scattering-scanning near-held optical microscopy (s-SNOM). We deduce that even for small crystals of VO2, the MIT is influenced by the competition between the R, M1, and M2 crystal phases with their different lattice constants subjected to the external substrate-induced stress. The results have important implications for the interpretation of the investigations of conventional polycrystalline thin Films where the mutual interaction of constituent crystallites may affect the nature of the MIT in VO2.