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Register a new userReversible modulation of metal-insulator transition in VO2 via chemically-induced oxygen migration
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Metal-insulator transitions (MIT),an intriguing correlated phenomenon induced by the subtle competition of the electrons repulsive Coulomb interaction and kinetic energy, is of great potential use for electronic applications due to the dramatic change in resistivity. Here, we demonstrate a reversible control of MIT in VO2 films via oxygen stoichiometry engineering. By facilely depositing and dissolving a water-soluble yet oxygen-active Sr3Al2O6 capping layer atop the VO2 at room temperature, oxygen ions can reversibly migrate between VO2 and Sr3Al2O6, resulting in a gradual suppression and a complete recovery of MIT in VO2. The migration of the oxygen ions is evidenced in a combination of transport measurement, structural characterization and first-principles calculations. This approach of chemically-induced oxygen migration using a water-dissolvable adjacent layer could be useful for advanced electronic and iontronic devices and studying oxygen stoichiometry effects on the MIT.
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Unusual metallic states involving breakdown of the standard Fermi-liquid picture of long-lived quasiparticles in well-defined band states emerge at low temperatures near correlation-driven Mott transitions. Prominent examples are ill-understood metallic states in $d$- and $f$-band compounds near Mott-like transitions. Finding of superconductivity in solid O$_{2}$ on the border of an insulator-metal transition at high pressures close to 96~GPa is thus truly remarkable. Neither the insulator-metal transition nor superconductivity are understood satisfactorily. Here, we undertake a first step in this direction by focussing on the pressure-driven insulator-metal transition using a combination of first-principles density-functional and many-body calculations. We report a striking result: the finding of an orbital-selective Mott transition in a pure $p$-band elemental system. We apply our theory to understand extant structural and transport data across the transition, and make a specific two-fluid prediction that is open to future test. Based thereupon, we propose a novel scenario where soft multiband modes built from microscopically coexisting itinerant and localized electronic states are natural candidates for the pairing glue in pressurized O$_{2}$.
The Metal-Insulator transition (MIT) in VO2 is characterized by the complex interplay among lattice, electronic and orbital degrees of freedom. In this contribution we investigated the strain-modulation of the orbital hierarchy and the influence over macroscopic properties of the metallic phase of VO2 such as Fermi Level (FL) population and metallicity, i.e., the material ability to screen an electric field, by means of temperature-dependent X-ray Absorption Near Edge Structure (XANES) and Resonant Photoemission spectroscopy (ResPES). We demonstrate that the MIT in strained VO2 is of the Filling Control type, hence it is generated by electron correlation effects. In addition, we show that the MIT in Nanostructured (NS) disordered VO2, where the structural phase transition is quenched, is driven by electron correlation. Therefore a fine tuning of the correlation could lead to a precise control and tuning of the transition features.
Ultrathin freestanding membranes with a pronounced metal-insulator transition (MIT) provides huge potential in future flexible electronic applications as well as a unique aspect of the study of lattice-electron interplay. However, the reduction of the thickness to an ultrathin region (a few nm) is typically detrimental to the MIT in epitaxial films, and even catastrophic for their freestanding form. Here, we report an enhanced MIT in VO2-based freestanding membranes, with a lateral size up to millimetres and VO2 thickness down to 5 nm. The VO2-membranes were detached by dissolving a Sr3Al2O6 sacrificial layer between the VO2 thin film and c-Al2O3(0001) substrate, allowing a transfer onto arbitrary surfaces. Furthermore, the MIT in the VO2-membrane was greatly enhanced by inserting an intermediate Al2O3 buffer layer. In comparison to the best available ultrathin VO2-membranes, the enhancement of MIT is over 400% at 5 nm VO2 thickness and more than one order of magnitude for VO2 above 10 nm. Our study widens the spectrum of functionality in ultrathin and large-scale membranes, and enables the potential integration of MIT into flexible electronics and photonics.
We demonstrate control of the carrier density of single phase anatase TiO2 thin films by nearly two orders of magnitude by modulating the growth kinetics during pulsed laser deposition, under fixed thermodynamic conditions. The resistivity and the intensity of the photoluminescence spectra of these TiO2 samples, both of which correlate with the number of oxygen vacancies, are shown to depend strongly on the growth rate. A quantitative model is used to explain the carrier density changes.
Synchrotron X-ray total scattering studies of structural changes in rutile VO2 at the metal-insulator transition temperature of 340 K reveal that monoclinic and tetragonal phases of VO2 coexist in equilibrium, as expected for a first-order phase transition. No evidence for any distinct intermediate phase is seen. Unbiased local structure studies of the changes in V--V distances through the phase transition, using reverse Monte Carlo methods, support the idea of phase coexistence and point to the high degree of correlation in the dimerized low-temperature structure. No evidence for short range V--V correlations that would be suggestive of local dimers is found in the metallic phase.
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