Excited state dynamics of nanocrystalline VO2 with white light continuum time resolved spectroscopy

Abstract

In an attempt to use ultrafast pump probe spectroscopy technique with white light continuum to reveal wavelength dependent dynamics of VO2, bandgap needs to be opened. Therefore, nanostructured amorphous and crystalline VO2 thin films were prepared with pulsed DC magnetron reactive sputtering. The mean diameters of grains were measured as 22 +/- 0.1 nm and 44 +/- 0.1 nm for amorphous and crystalline VO2 thin films, respectively. Temperature dependent resistance measurements show that nanocrystalline VO2 thin film exhibit metal insulator phase transition. The films exhibited dual band gaps (2.3 eV, < 0.6 eV for amorphous films and 13 eV, 1.8 eV for crystalline film). Increased band gaps made it possible to perform time resolved transmission and reflection experiments with white light continuum at fluences above and below photo induced phase transition threshold. Although transmission chance due to photo induced phase transition of VO2 in the literature usually takes places at infrared region of the spectrum, transmission chance was observed in visible as low as 630 nm in broadband probe spectra. It was observed that measured time scales depend on not only pump fluence but also probe wavelength. Experiments gave the evidence of the long-lived lower energy non-equilibrium state related to the photo induced phase