83 research outputs found
Unified Band Theoretic Description of Electronic and Magnetic Properties of Vanadium Dioxide Phases
The debate about whether the insulating phases of vanadium dioxide (VO2) can
be described by band theory or must be described by a theory of strong electron
correlations remains unresolved even after decades of research. Energy-band
calculations using hybrid exchange functionals or including self-energy
corrections account for the insulating or metallic nature of different phases,
but have not yet successfully accounted for the observed magnetic orderings.
Strongly-correlated theories have had limited quantitative success. Here we
report that, by using hard pseudopotentials and an optimized hybrid exchange
functional, the energy gaps and magnetic orderings of both monoclinic VO2
phases and the metallic nature of the high-temperature rutile phase are
consistent with available experimental data, obviating an explicit role for
strong correlations. We also report a potential candidate for the newly-found
metallic monoclinic phase and present a detailed magnetic structure of the M2
monoclinic phase
Ultrafast Plasmonic Control of Second Harmonic Generation
Efficient frequency conversion techniques are crucial to the development of
plasmonic metasurfaces for information processing and signal modulation. In
principle, nanoscale electric-field confinement in nonlinear materials enables
higher harmonic conversion efficiencies per unit volume than those attainable
in bulk materials. Here we demonstrate efficient second-harmonic generation
(SHG) in a serrated nanogap plasmonic geometry that generates steep electric
field gradients on a dielectric metasurface. An ultrafast pump is used to
control plasmon-induced electric fields in a thin-film material with inversion
symmetry that, without plasmonic enhancement, does not exhibit an an even-order
nonlinear optical response. The temporal evolution of the plasmonic near-field
is characterized with ~100as resolution using a novel nonlinear interferometric
technique. The ability to manipulate nonlinear signals in a metamaterial
geometry as demonstrated here is indispensable both to understanding the
ultrafast nonlinear response of nanoscale materials, and to producing active,
optically reconfigurable plasmonic device
Instantaneous band gap collapse in photoexcited monoclinic VO due to photocarrier doping
Using femtosecond time-resolved photoelectron spectroscopy we demonstrate
that photoexcitation transforms monoclinic VO quasi-instantaneously into a
metal. Thereby, we exclude an 80 femtosecond structural bottleneck for the
photoinduced electronic phase transition of VO. First-principles many-body
perturbation theory calculations reveal a high sensitivity of the VO
bandgap to variations of the dynamically screened Coulomb interaction,
supporting a fully electronically driven isostructral insulator-to-metal
transition. We thus conclude that the ultrafast band structure renormalization
is caused by photoexcitation of carriers from localized V 3d valence states,
strongly changing the screening \emph{before} significant hot-carrier
relaxation or ionic motion has occurred
Control of Plasmonic Nanoantennas by Reversible Metal-insulator Transition
We demonstrate dynamic reversible switching of VO2 insulator-to-metal transition (IMT) locally on the scale of 15 nm or less and control of nanoantennas, observed for the first time in the near-field. Using polarization-selective near-field imaging techniques, we simultaneously monitor the IMT in VO2 and the change of plasmons on gold infrared nanoantennas. Structured nanodomains of the metallic VO2 locally and reversibly transform infrared plasmonic dipole nanoantennas to monopole nanoantennas. Fundamentally, the IMT in VO2 can be triggered on femtosecond timescale to allow ultrafast nanoscale control of optical phenomena. These unique features open up promising novel applications in active nanophotonics
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