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Enhanced metal-insulator transition in freestanding VO2 down to 5 nm thickness

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 Added by Kun Han
 Publication date 2021
  fields Physics
and research's language is English




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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.



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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.
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.
149 - E. Radue , E. Crisman , L. Wang 2012
In this paper we used Raman spectroscopy to investigate the optical properties of vanadium dioxide (VO2) thin films during the thermally induced insulating to metallic phase transition. We observed a significant difference in transition temperature in similar VO2 films grown on quartz and sapphire substrates: the film grown on quartz displayed the phase transition at a lower temperature (Tc=50C) compared a film grown on sapphire (Tc=68C). We also investigated differences in the detected Raman signal for different wavelengths and polarizations of the excitation laser. We found that for either substrate, a longer wavelength (in our case 785 nm) yielded the clearest VO2 Raman spectra, with no polarization dependence.
104 - Kun Han , Hanyu Wang , Liang Wu 2021
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.
Vanadium dioxide (VO2) has been widely studied for its rich physics and potential applications, undergoing a prominent insulator-metal transition (IMT) near room temperature. The transition mechanism remains highly debated, and little is known about the IMT at nanoscale dimensions. To shed light on this problem, here we use ~1 nm wide carbon nanotube (CNT) heaters to trigger the IMT in VO2. Single metallic CNTs switch the adjacent VO2 at less than half the voltage and power required by control devices without a CNT, with switching power as low as ~85 ${mu}W$ at 300 nm device lengths. We also obtain potential and temperature maps of devices during operation using Kelvin Probe Microscopy (KPM) and Scanning Thermal Microscopy (SThM). Comparing these with three-dimensional electrothermal simulations, we find that the local heating of the VO2 by the CNT play a key role in the IMT. These results demonstrate the ability to trigger IMT in VO2 using nanoscale heaters, and highlight the significance of thermal engineering to improve device behaviour.
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