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Emission of terahertz pulses from vanadium dioxide films undergoing metal–insulator phase transition

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Abstract

This paper describes research on the optics of functional materials, which can change their dielectric properties according to their function. Vanadium dioxide is a good example of such a material where the insulator-to-metal phase transition offers the possibility to control dielectric properties and to use them as a triggering element for photonic applications in the wide spectral range from optical to terahertz frequencies. We observed emission of terahertz (THz) radiation from VO2 films in insulating and conductive phase states under femtosecond pulse irradiation. We found that the efficiency of THz emission increases up to 30 times after the insulator-to-metal phase transition. This process occurs in thin films while it is fundamentally forbidden in the bulk material, and polarization analysis of the emitted radiation reveals the crucial importance of interface contributions. The properties of the THz radiation emitted by VO2 are determined by displacement photocurrents at the VO2–air and VO2–substrate interfaces induced by the incident laser light. In each phase state the contributions of the two boundaries are different. Properties of the effective dielectric susceptibility χ(2) tensor for the insulating phase were defined. In demonstrating the conversion of optical into THz radiation in VO2 films, we found that fundamental symmetry restrictions are not applicable to problems of nonlinear optics of thin films.

© 2015 Optical Society of America

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Figures (7)

Fig. 1.
Fig. 1. Scheme of the experimental setup. BS, beamsplitter; DL, motorized delay line; ZnTe, 4-mm-thick ZnTe electro-optical crystal; λ/2, λ/4, waveplates; OAP, off-axis parabolic mirror; WP, Wollaston prism; PD1, PD2, balanced photodiodes.
Fig. 2.
Fig. 2. Result of XRD analysis of VO2/R-Al2O3 film: (a) 2θ-scan, (b) pole figure for reflection at 2θ=37.14°, (c) φ-scan for (0006)Al2O3, and (d) mutual directions of R-cut Al2O3 substrate axes and VO2(200) film axes in its two phase states. For low-temperature phase, both possible VO2 film orientations are shown.
Fig. 3.
Fig. 3. (a) Temperature dependence of maximum transmitted THz amplitude for 100 nm PLD film. (b) Spectra of THz radiation transmitted through the sample in the conductive and insulating phase state. The black curve represents the reference spectrum with no sample in the THz beam.
Fig. 4.
Fig. 4. Typical waveform and spectrum of a THz pulse generated in VO2 film on sapphire substrate in conductive (red) and insulating (blue) phase.
Fig. 5.
Fig. 5. Detected THz amplitude versus laser pulse fluence for semiconductor (red) and conductive (black) states.
Fig. 6.
Fig. 6. Polarization of the THz radiation generated in the VO2 film grown by MOCVD in (a) insulating and (b) conductive states for different angles between pump polarization and film orientation.
Fig. 7.
Fig. 7. (a) THz amplitude (black) and polarization direction β (red) of THz radiation versus direction of optical polarization α (a) for insulating phase of the film and (b) for conductive phase. Solid lines show the dependences for the effective χ(2) tensor introduced in Section 5. Squares and circles represent results for two different samples.

Tables (1)

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Table 1. Contrast in THz Absorption and THz Emission upon Phase Transition

Equations (1)

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χxxx(2)=1,χxyy(2)=0.02,χyyx(2)=χyxy(2)=0.12,χyyy(2)=χyxx(2)=χxxy(2)=χxyx(2)=0,
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