March 19, 2008
The optical/infrared properties of films of vanadium dioxide (VO2) and vanadium sesquioxide (V2O3) have been investigated via ellipsometry and near-normal incidence reflectance measurements from far infrared to ultraviolet frequencies. Significant changes occur in the optical conductivity of both VO2 and V2O3 across the metal-insulator transitions at least up to (and possibly beyond) 6 eV. We argue that such changes in optical conductivity and electronic spectral weight over a broad frequency range is evidence of the important role of electronic correlations to the metal-insulator transitions in both of these vanadium oxides. We observe a sharp optical transition with possible final state (exciton) effects in the insulating phase of VO2. This sharp optical transition occurs between narrow a1g bands that arise from the quasi-one-dimensional chains of vanadium dimers. Electronic correlations in the metallic phases of both VO2 and V2O3 lead to reduction of the kinetic energy of the charge carriers compared to band theory values, with paramagnetic metallic V2O3 showing evidence of stronger correlations compared to rutile metallic VO2.
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November 28, 2006
The metal-insulator transition and unconventional metallic transport in vanadium dioxide (VO$_2$) are investigated with a combination of spectroscopic ellipsometry and reflectance measurements. The data indicates that electronic correlations, not electron-phonon interactions, govern charge dynamics in the metallic state of VO$_2$. This study focuses on the frequency and temperature dependence of the conductivity in the regime of extremely short mean free path violating the Io...
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In the pursuit of advanced photoelectric devices, researchers have uncovered near room-temperature metal-insulator transitions (MIT) in non-volatile VO2. Although theoretical investigations propose that polaron dynamics mediate the MIT, direct experimental evidence remains scarce. In this study, we present direct evidence of the polaron state in insulating VO2 through high-resolution spectroscopic ellipsometry measurements and first-principles calculations. We demonstrate tha...
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Thin films of VO$_2$ on different substrates, Al$_2$O$_3$ and SiO$_2$/Si, have been prepared and characterized from room temperature up to 360 K. From the band structure in the rutile metallic phase and in the monoclinic insulating phase the optical properties are calculated and compared with reflection measurements as a function of temperatures. Various interband transitions can be assigned and compared with previous speculations. We extract the parameters of the metallic ch...
July 25, 2008
Materials with strong electronic Coulomb interactions play an increasing role in modern materials applications. "Thermochromic" systems, which exhibit thermally induced changes in their optical response, provide a particularly interesting case. The optical switching associated with the metal-insulator transition of vanadium dioxide (VO2), for example, has been proposed for use in "intelligent" windows, which selectively filter radiative heat in hot weather conditions. In this...
March 13, 2006
We have investigated the charge dynamics of VO2 by optical reflectivity measurements. Optical conductivity clearly shows a metal-insulator transition. In the metallic phase, a broad Drude-like structure is observed. On the other hand, in the insulating phase, a broad peak structure around 1.3 eV is observed. It is found that this broad structure observed in the insulating phase shows a temperature dependence. We attribute this to the electron-phonon interaction as in the phot...
March 26, 2015
We use polarization- and temperature-dependent x-ray absorption spectroscopy, in combination with photoelectron microscopy, x-ray diffraction and electronic transport measurements, to study the driving force behind the insulator-metal transition in VO2. We show that both the collapse of the insulating gap and the concomitant change in crystal symmetry in homogeneously strained single-crystalline VO2 films are preceded by the purely-electronic softening of Coulomb correlations...
January 8, 2019
The insulator-to-metal transition (IMT) in vanadium dioxide (VO2) can enable a variety of optics applications, including switching and modulation, optical limiting, and tuning of optical resonators. Despite the widespread interest in optics, the optical properties of VO2 across its IMT are scattered throughout the literature, and are not available in some wavelength regions. We characterized the complex refractive index of VO2 thin films across the IMT for free-space waveleng...
March 29, 2004
To compare the metal-insulator transitions (MITs) of VO2 and V2O3 we analyze the relations between the structural and electronic properties of the vanadium Magneli phases. These materials set up the homologous series VnO(2n-1) (3 <= n <= 9) and have crystal structures comprising typical dioxide-like and sesquioxide-like regions. As the MITs of the vanadium Magneli phases are accompanied by structural transformations, we are able to discuss the effects of characteristic change...
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We present a detailed infrared study of the insulator-to-metal transition (IMT) in vanadium dioxide (VO2) thin films. Conventional infrared spectroscopy was employed to investigate the IMT in the far-field. Scanning near-field infrared microscopy directly revealed the percolative IMT with increasing temperature. We confirmed that the phase transition is also percolative with cooling across the IMT. We present extensive near-field infrared images of phase coexistence in the IM...
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We combine ultrafast electron diffraction and time-resolved terahertz spectroscopy measurements to unravel the connection between structure and electronic transport properties during the photoinduced insulator-metal transitions in vanadium dioxide. We determine the structure of the metastable monoclinic metal phase, which exhibits anti-ferroelectric charge order arising from a thermally activated, orbital-selective phase transition in the electron system. The relative contrib...