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Register a new userVanadium dioxide : A Peierls-Mott insulator stable against disorder
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Vanadium dioxide undergoes a first order metal-insulator transition at 340 K. In this work, we develop and carry out state of the art linear scaling DFT calculations refined with non-local dynamical mean-field theory. We identify a complex mechanism, a Peierls-assisted orbital selection Mott instability, which is responsible for the insulating M$_1$ phase, and furthermore survives a moderate degree of disorder.
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Vanadium dioxide(VO$_2$) is a paradigmatic example of a strongly correlated system that undergoes a metal-insulator transition at a structural phase transition. To date, this transition has necessitated significant post-hoc adjustments to theory in order to be described properly. Here we report standard state-of-the-art first principles quantum Monte Carlo (QMC) calculations of the structural dependence of the properties of VO$_2$. Using this technique, we simulate the interactions between electrons explicitly, which allows for the metal-insulator transition to naturally emerge, importantly without ad-hoc adjustments. The QMC calculations show that the structural transition directly causes the metal-insulator transition and a change in the coupling of vanadium spins. This change in the spin coupling results in a prediction of a momentum-independent magnetic excitation in the insulating state. While two-body correlations are important to set the stage for this transition, they do not change significantly when VO$_2$ becomes an insulator. These results show that it is now possible to account for electron correlations in a quantitatively accurate way that is also specific to materials.
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 Ioffe-Regel-Mott limit of metallic transport. The standard quasiparticle picture of charge conduction is found to be untenable in metallic VO$_2$.
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 IMT regime in VO2. We find that the coexisting insulating and metallic regions at a fixed temperature are static on the time scale of our measurements. A novel approach for analyzing the far-field and near-field infrared data within the Bruggeman effective medium theory was employed to extract the optical constants of the incipient metallic puddles at the onset of the IMT. We found divergent effective carrier mass in the metallic puddles that demonstrates the importance of electronic correlations to the IMT in VO2. We employ the extended dipole model for a quantitative analysis of the observed near-field infrared amplitude contrast and compare the results with those obtained with the basic dipole model.
The thermal radiative near field transport between vanadium dioxide and silicon oxide at submicron distances is expected to exhibit a strong dependence on the state of vanadium dioxide which undergoes a metal-insulator transition near room temperature. We report the measurement of near field thermal transport between a heated silicon oxide micro-sphere and a vanadium dioxide thin film on a titanium oxide (rutile) substrate. The temperatures of the 15 nm vanadium dioxide thin film varied to be below and above the metal-insulator-transition, the sphere temperatures were varied in a range between 100 and 200 Celsius. The measurements were performed using a vacuum-based scanning thermal microscope with a cantilevered resistive thermal sensor. We observe a thermal conductivity per unit area between the sphere and the film with a distance dependence following a power law trend and a conductance contrast larger than 2 for the two different phase states of the film.
We present the first comprehensive broadband optical spectroscopy data on two insulating phases of vanadium dioxide (VO2): monoclinic M2 and triclinic. The main result of our work is that the energy gap and the electronic structure are essentially unaltered by the first-order structural phase transition between the M2 and triclinic phases. Moreover, the optical interband features in the M2 and triclinic phases are remarkably similar to those observed in the well-studied monoclinic M1 insulating phase of VO2. As the energy gap is insensitive to the different lattice structures of the three insulating phases, we rule out Peierls effects as the dominant contributor to the opening of the gap. Rather, the energy gap arises from intra-atomic Coulomb correlations.
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