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Nanoscale imaging of the electronic and structural transitions in vanadium dioxide

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 Added by Mumtaz Qazilbash
 Publication date 2011
  fields Physics
and research's language is English




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We investigate the electronic and structural changes at the nanoscale in vanadium dioxide (VO2) in the vicinity of its thermally driven phase transition. Both electronic and structural changes exhibit phase coexistence leading to percolation. In addition, we observe a dichotomy between the local electronic and structural transitions. Nanoscale x-ray diffraction reveals local, non-monotonic switching of the lattice structure, a phenomenon that is not seen in the electronic insulator-to-metal transition mapped by near-field infrared microscopy.



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The metal-insulator transition (MIT) in vanadium dioxide (VO2) has the potential to lead to a number of disruptive technologies, including ultra-fast data storage, optical switches, and transistors which move beyond the limitations of silicon. For applications, VO2 films are deposited on crystalline substrates to prevent cracking observed in bulk VO2 crystals across the thermally driven MIT. Near the MIT, VO2 films exhibit nanoscale coexistence between metallic and insulating phases, which opens up further potential applications such as memristors, tunable capacitors, and optically engineered devices such as perfect absorbers. It is generally believed that the formation of phase domains must be affected to some extent by random processes which lead to unreliable performance in nanoscale MIT based devices. Here we show that nanoscale randomness is suppressed in the thermally driven MIT in sputtered VO2 films; the observed domain patterns of metallic and insulating phases in the vicinity of the MIT in these films behave in a strikingly reproducible way. This result opens the door for realizing reliable nanoscale VO2 devices.
We report the simultaneous measurement of the structural and electronic components of the metal-insulator transition of VO$_2$ using electron and photoelectron spectroscopies and microscopies. We show that these evolve over different temperature scales, and are separated by an unusual monoclinic-like metallic phase. Our results provide conclusive evidence that the new monoclinic-like metallic phase, recently identified in high-pressure and nonequilibrium measurements, is accessible in the thermodynamic transition at ambient pressure, and we discuss the implications of these observations on the nature of the MIT in VO$_2$.
Vanadium dioxide, an archetypal correlated-electron material, undergoes an insulator-metal transition near room temperature that exhibits electron-correlation-driven and structurally-driven physics. Using ultrafast optical spectroscopy and x-ray scattering we show that these processes can be disentangled in the time domain. Specifically, following intense sub-picosecond electric-field excitation, a partial collapse of the insulating gap occurs within the first ps. Subsequently, this electronic reconfiguration initiates a change in lattice symmetry taking place on a slower timescale. We identify the kinetic energy increase of electrons tunneling in the strong electric field as the driving force, illustrating a novel method to control electronic interactions in correlated materials on an ultrafast timescale.
Phase competition in correlated oxides offers tantalizing opportunities as many intriguing physical phenomena occur near the phase transitions. Owing to a sharp metal-insulator transition (MIT) near room temperature, correlated vanadium dioxide (VO2) exhibits a strong competition between insulating and metallic phases that is important for practical applications. However, the phase boundary undergoes strong modification when strain is involved, yielding complex phase transitions. Here, we report the emergence of the nanoscale M2 phase domains in VO2 epitaxial films under anisotropic strain relaxation. The phase states of the films are imaged by multi-length-scale probes, detecting the structural and electrical properties in individual local domains. Competing evolution of the M1 and M2 phases indicates a critical role of lattice-strain on both the stability of the M2 Mott phase and the energetics of the MIT in VO2 films. This study demonstrates how strain engineering can be utilized to design phase states, which allow deliberate control of MIT behavior at the nanoscale in epitaxial VO2 films.
The competition between collective quantum phases in materials with strongly correlated electrons depends sensitively on the dimensionality of the electron system, which is difficult to control by standard solid-state chemistry. We have fabricated superlattices of the paramagnetic metal LaNiO3 and the wide-gap insulator LaAlO3 with atomically precise layer sequences. Using optical ellipsometry and low-energy muon spin rotation, superlattices with LaNiO3 as thin as two unit cells are shown to undergo a sequence of collective metalinsulator and antiferromagnetic transitions as a function of decreasing temperature, whereas samples with thicker LaNiO3 layers remain metallic and paramagnetic at all temperatures. Metal-oxide superlattices thus allow control of the dimensionality and collective phase behavior of correlated-electron systems.
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