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Abstract: Laser-induced ultrafast nonlinear optical (NLO) response was observed in transient absorption, reflection and NLO measurements in VO2 thin films. The films were prepared using pulsed laser deposition technique with metallic vanadium and V2O5 powder employed as target material. The obtained thin films exhibit a thermal, as well as a laser-induced phase transition (PT) from semiconductor state at room temperature to metallic state. A typical hysterisis was observed for electric resistivity and optical reflectance verses temperature T. For the laser-induced PT in femtosecond pump–probe experiment, the PT was found to be ultrafast, immediately upon laser excitation. Kinetics study suggests that the PT is realized via an intermediate state, presumably a Wannier–Mott exciton (WME) state, followed by a resonant transition to the metallic phase state. The presence of the intermediate state is responsible for an extremely large third-order susceptibility observed in a nonlinear holographic experiment. In a 80nm thick VO2 thin amorphous film, the value of χ (3) was measured to be 1.3×10−8 esu which is four orders of magnitude greater than a standard reference sample of CS2. In addition, the nonlinear response was further enhanced with diffraction signal increased by a factor of 4 after the laser excitation. A signal dip at ∼1.2ns was repeatedly observed, which is presumably due to the excitation process associated with the intermediate state. Finally, the resonant transition from the intermediate state to the metallic state, giving rise to a maximum diffraction signal intensity from the formed transient grating. [Copyright &y& Elsevier]

Abstract: As a kind of phase transition functional material, Vanadium dioxide (VO2) thin films deposited on fused quartz substrate were fabricated using pulsed laser deposition (PLD) technique. Europium was introduced for structure study. By laser excitation at 526nm, VO2 thin film undergoes a reversible and ultrafast phase transition from semiconductor to metallic state, which results in a change of optical properties. In fluorescence measurement, Eu emission was found severely quenched in all as-grown thin films. After annealing the sample in air, a red Eu-emission appeared. The emission spectrum is characterized by a pronounced twin peak, centered at 617nm (5D0–7F2), surrounded by a set of broad, but relatively weaker bands (emission from 5D0 to 7F j manifold). The emission lifetime increased when the sample annealed at higher temperature for longer time. Each spectral component is actually a doublet which is the spectral overlap of emissions from Eu3+ situated in two sites with different configurations. One is a linear h-Eu3+-h, where h stands for holes. Another is a right-angle configuration of h-Eu3+-h with Eu3+ in the corner. In as-grown VO2 film, Eu3+ ions can either substitute V4+, leaving a negative charge around (Eu3+–O)–, or substitute V5+, leaving two negative charges around (Eu3+–O)−−. Due to trapped electrons in a large radius state, it covers Eu3+V4+–V5+ complexes. It suggests that the screening by degenerate electronic gas may result in switching off the Eu-related optical response for a wide spectral region, causing emission quenching in VO2 films. [Copyright &y& Elsevier]