Robert E. Marvel

Instantaneous Band Gap Collapse in Photoexcited Monoclinic VO2 due to Photocarrier Doping

Using femtosecond time-resolved photoelectron spectroscopy we demonstrate that photoexcitation transforms monoclinic VO2 quasi-instantaneously into a metal. Thereby, we exclude an 80 fs structural bottleneck for the photoinduced electronic phase transition of VO2. First-principles many-body perturbation theory calculations reveal a high sensitivity of the VO2 band gap to variations of the dynamically screened Coulomb interaction, supporting a fully electronically driven isostructural 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 before significant hot-carrier relaxation or ionic motion has occurred.

Ultra-compact silicon photonic devices reconfigured by an optically induced semiconductor-to-metal transition

Vanadium dioxide (VO(2)) is a promising reconfigurable optical material and has long been a focus of condensed matter research owing to its distinctive semiconductor-to-metal phase transition (SMT), a feature that has stimulated recent development of thermally reconfigurable photonic, plasmonic, and metamaterial structures. Here, we integrate VO(2) onto silicon photonic devices and demonstrate all-optical switching and reconfiguration of ultra-compact broadband Si-VO(2) absorption modulators (L < 1 μm) and ring-resonators (R ~ λ(0)). Optically inducing the SMT in a small, ~0.275 μm(2), active area of polycrystalline VO(2) enables Si-VO(2) structures to achieve record values of absorption modulation, ~4 dB μm(-1), and intracavity phase modulation, ~π/5 rad μm(-1). This in turn yields large, tunable changes to resonant wavelength, |Δλ(SMT)| ~ 3 nm, approximately 60 times larger than Si-only control devices, and enables reconfigurable filtering and optical modulation in excess of 7 dB from modest Q-factor (~10(3)), high-bandwidth ring resonators (>100 GHz). All-optical integrated Si-VO(2) devices thus constitute platforms for reconfigurable photonics, bringing new opportunities to realize dynamic on-chip networks and ultrafast optical shutters and modulators.

Photothermal optical modulation of ultra-compact hybrid Si-VO 2 ring resonators

We demonstrate photothermally induced optical switching of ultra-compact hybrid Si-VO₂ ring resonators. The devices consist of a sub-micron length ~70 nm thick patch of phase-changing VO₂ integrated onto silicon ring resonators as small as 1.5 μm in radius. The semiconductor-to-metal transition (SMT) of VO₂ is triggered using a 532 nm pump laser, while optical transmission is probed using a tunable cw laser near 1550 nm. We observe optical modulation greater than 10dB from modest quality-factor (~10³) resonances, as well as a large -1.26 nm change in resonant wavelength Δλ, resulting from the large change in the dielectric function of VO₂ in the insulator-to-metal transition achieved by optical pumping.

Tunable optical antennas enabled by the phase transition in vanadium dioxide

Optical antennas, subwavelength metallic structures resonating at visible frequencies, are a relatively new branch of antenna technology being applied in science, technology and medicine. Dynamically tuning the resonances of these antennas would increase their range of application and offer potential increases in plasmonic device efficiencies. Silver nanoantenna arrays were fabricated on a thin film of the phase change material vanadium dioxide (VO(2)) and the resonant wavelength of these arrays was modulated by increasing the temperature of the substrate above the critical temperature (approximately 68 °C). Depending on the array, wavelength modulation of up to 110 nm was observed.

Optical switching and photoluminescence in erbium-implanted vanadium dioxide thin films

Vanadium dioxide (VO2) is under intensive consideration for optical switching due to its reversible phase transition, which features a drastic and rapid shift in infrared reflectivity. Classified as an insulator–to–metal transition, the phase transition in VO2 can be induced thermally, electrically, and optically. When induced optically, the transition can occur on sub-picosecond time scales. It is interesting to dope VO2 with erbium ions (Er3+) and observe their combined properties. The first excited-state luminescence of Er3+ lies within the wavelength window of minimal transmission-loss in silicon and has been widely utilized for signal amplification and generation in silicon photonics. The incorporation of Er3+ into VO2 could therefore result in a novel photonic material capable of simultaneous optical switching and amplification. In this work, we investigate the optical switching and photoluminescence in Er-implanted VO2 thin films. Thermally driven optical switching is demonstrated in the Er-implant...

Super-Resolution in Label-Free Photomodulated Reflectivity

We demonstrate a new, label-free, far-field super-resolution method based on an ultrafast pump-probe scheme oriented toward nanomaterial imaging. A focused pump laser excites a diffraction-limited spatial temperature profile, and the nonlinear changes in reflectance are probed. Enhanced spatial resolution is demonstrated with nanofabricated silicon and vanadium dioxide nanostructures. Using an air objective, resolution of 105 nm was achieved, well beyond the diffraction limit for the pump and probe beams and offering a novel kind of dedicated nanoscopy for materials.

Tunneling breakdown of a strongly correlated insulating state in V O 2 induced by intense multiterahertz excitation

We directly trace the near- and mid-infrared transmission change of a VO

Ultrafast Mid-Infrared Nanoscopy of Strained Vanadium Dioxide Nanobeams

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Control of Plasmonic Nanoantennas by Reversible Metal-insulator Transition

thin film during an ultrafast insulator-to-metal transition triggered by high-field multi-terahertz transients. Non-thermal switching into a metastable metallic state is governed solely by the amplitude of the applied terahertz field. In contrast to resonant excitation below the threshold fluence, no signatures of excitonic self-trapping are observed. Our findings are consistent with the generation of spatially separated charge pairs and a cooperative transition into a delocalized metallic state by THz field-induced tunneling. The tunneling process is a condensed-matter analogue of the Schwinger effect in nonlinear quantum electrodynamics. We find good agreement with the pair production formula by replacing the Compton wavelength with an electronic correlation length of 2.1

Tracking the insulator-to-metal phase transition in VO2 with few-femtosecond extreme UV transient absorption spectroscopy

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