How optical excitation controls the structure and properties of vanadium dioxide

Abstract

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 contribution of this photoinduced monoclinic metal (which has no equilibrium analog) and the photoinduced rutile metal (known from the equilibrium phase diagram) to the time and pump-fluence dependent multi-phase character of the film is established, as is the respective impact of these two distinct phase transitions on the observed changes in terahertz conductivity. Our results represent an important new example of how light can control the properties of strongly correlated materials and elucidate that multi-modal experiements are essential when seeking a detailed connection between ultrafast changes in optical-electronic properties and lattice structure in complex materials.

9 pages including figures, supplemental material included as ancillary file

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• Uniting the order and disorder dynamics in photoexcited VO2
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• Mott materials: unsuccessful metals with a bright future
• Relativistic ultrafast electron diffraction at high repetition rates
• High-strain-induced local modification of the electronic properties of VO${}_2$ thin films
• Concurrent probing of electron-lattice dephasing induced by photoexcitation in 1T-TaSeTe using ultrafast electron diffraction
• Ultimate bunch length and emittance performance of an MeV ultrafast electron diffraction apparatus with a DC gun and a multi-cavity SRF linac
• Nature of the photo-induced metallic state in monoclinic VO${}_2$
• Excimer Formation in Zinc-phthalocyanine Revealed using Ultrafast Electron Diffraction
• Light-induced phase transitions in vanadium dioxide: a tensor network study
• First-order kinetics bottleneck during photoinduced ultrafast insulator-metal transition in 3D orbitally-driven Peierls insulator CuIr${}_2$S${}_4$
• Band-selective Plasmonic Polaron in Thermoelectric Semimetal Ta${}_2$PdSe${}_6$ with ultra-high power factor
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• INQ, a modern GPU-accelerated computational framework for (time-dependent) density functional theory
• Terahertz-driven ultrafast dynamics of rare-earth nickelates by controlling only the charge degree of freedom
• Temporal dynamics of all-optical switching in hybrid VO2/Si waveguides
• Ultrafast optical melting of trimer superstructure in layered 1T'-TaTe2
• Tuning of Localized Surface Plasmons in Vanadium Dioxide Nanoparticles via Size and Insulator-Metal Transition
• Ultrafast dynamics of atomic correlated disordering in photoinduced VO${}_2$