Harmonic Generation up to Fifth Order from Al/Au/CuS Nanoparticle Films.

Dual heterostructures integrating noble-metal and copper chalcogenide nanoparticles have attracted a great deal of attention in nonlinear optics, because coupling of their localized surface plasmon resonances (LSPRs) substantially enhances light-matter interactions through local-field effects. Previously, enhanced cascaded third-harmonic generation was demonstrated in Au/CuS heterostructures mediated by harmonically coupled surface plasmon resonances. This suggests a promising approach for extending nonlinear enhancement to higher harmonics by adding an additional nanoparticulate material with higher-frequency harmonic resonances to the hybrid films.

Surface plasmon mediated harmonically resonant effects on third harmonic generation from Au and CuS nanoparticle films.

A growing class of nonlinear materials employ the localized surface plasmonic resonance (LSPR) of nanoparticles to enhance harmonic generation. Material systems containing harmonically coupled metallic and semiconductor plasmonic nanoparticles have been shown to further increase performance. Here, we explore the effect of dual plasmonic interactions in bilayer CuS and Au nanoparticle films on third harmonic generation (THG).

Reconfigurable Multistate Optical Systems Enabled by VO Phase Transitions.

Reconfigurable optical systems are the object of continuing, intensive research activities, as they hold great promise for realizing a new generation of compact, miniaturized, and flexible optical devices. However, current reconfigurable systems often tune only a single state variable triggered by an external stimulus, thus, leaving out many potential applications. Here we demonstrate a reconfigurable multistate optical system enabled by phase transitions in vanadium dioxide (VO).

Optical Limiting Based on Huygens' Metasurfaces.

Optical limiting is desirable or necessary in a variety of applications that employ high-power light sources or sensitive photodetectors. However, the most prevalent methods compromise between on-state transmission and turndown ratio or rely on narrow transmission windows. We demonstrate that a metasurface-based architecture incorporating phase-change materials enables both high and broadband on-state transmission (-4.

Refractive Index-Based Control of Hyperbolic Phonon-Polariton Propagation.

Hyperbolic phonon polaritons (HPhPs) are generated when infrared photons couple to polar optic phonons in anisotropic media, confining long-wavelength light to nanoscale volumes. However, to realize the full potential of HPhPs for infrared optics, it is crucial to understand propagation and loss mechanisms on substrates suitable for applications from waveguiding to infrared sensing. We employ scattering-type scanning near-field optical microscopy (s-SNOM) and nano-Fourier transform infrared (FTIR) spectroscopy, in concert with analytical and numerical calculations, to elucidate HPhP characteristics as a function of the complex substrate dielectric function.

Spatially and spectrally resolved orbital angular momentum interactions in plasmonic vortex generators.

Understanding the near-field electromagnetic interactions that produce optical orbital angular momentum (OAM) is crucial for integrating twisted light into nanotechnology. Here, we examine the cathodoluminescence (CL) of plasmonic vortices carrying OAM generated in spiral nanostructures. The nanospiral geometry defines a photonic local density of states that is sampled by the electron probe in a scanning transmission electron microscope (STEM), thus accessing the optical response of the plasmonic vortex with high spatial and spectral resolution.

Imaging Nanometer Phase Coexistence at Defects During the Insulator-Metal Phase Transformation in VO Thin Films by Resonant Soft X-ray Holography.

We use resonant soft X-ray holography to image the insulator-metal phase transition in vanadium dioxide with element and polarization specificity and nanometer spatial resolution. We observe that nanoscale inhomogeneity in the film results in spatial-dependent transition pathways between the insulating and metallic states. Additional nanoscale phases form in the vicinity of defects which are not apparent in the initial or final states of the system, which would be missed in area-integrated X-ray absorption measurements.

Polarization- and wavelength-resolved near-field imaging of complex plasmonic modes in Archimedean nanospirals.

Asymmetric nanophotonic structures enable a wide range of opportunities in optical nanotechnology because they support efficient optical nonlinearities mediated by multiple plasmon resonances over a broad spectral range. The Archimedean nanospiral is a canonical example of a chiral plasmonic structure because it supports even-order nonlinearities that are not generally accessible in locally symmetric geometries. However, the complex spiral response makes nanoscale experimental characterization of the plasmonic near-field structure highly desirable.

Silicon waveguide optical switch with embedded phase change material.

Phase-change materials (PCMs) have emerged as promising active elements in silicon (Si) photonic systems. In this work, we design, fabricate, and characterize a hybrid Si-PCM optical switch. By integrating vanadium dioxide (a PCM) within a Si photonic waveguide, in a non-resonant geometry, we achieve ~10 dB broadband optical contrast with a PCM length of 500 nm using thermal actuation.

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

Coulomb correlations can manifest in exotic properties in solids, but how these properties can be accessed and ultimately manipulated in real time is not well understood. The insulator-to-metal phase transition in vanadium dioxide (VO) is a canonical example of such correlations. Here, few-femtosecond extreme UV transient absorption spectroscopy (FXTAS) at the vanadium edge is used to track the insulator-to-metal phase transition in VO This technique allows observation of the bulk material in real time, follows the photoexcitation process in both the insulating and metallic phases, probes the subsequent relaxation in the metallic phase, and measures the phase-transition dynamics in the insulating phase.

Dynamically Reconfigurable Metadevice Employing Nanostructured Phase-Change Materials.

Mastering dynamic free-space spectral control and modulation in the near-infrared (NIR) and optical regimes remains a challenging task that is hindered by the available functional materials at high frequencies. In this work, we have realized an efficient metadevice capable of spectral control by minimizing the thermal mass of a vanadium dioxide phase-change material (PCM) and placing the PCM at the feed gap of a bow-tie field antenna. The device has an experimentally measured tuning range of up to 360 nm in the NIR and a modulation depth of 33% at the resonant wavelength.

Geometric constraints on phase coexistence in vanadium dioxide single crystals.

The appearance of stripe phases is a characteristic signature of strongly correlated quantum materials, and its origin in phase-changing materials has only recently been recognized as the result of the delicate balance between atomic and mesoscopic materials properties. A vanadium dioxide (VO) single crystal is one such strongly correlated material with stripe phases. Infrared nano-imaging on low-aspect-ratio, single-crystal VO microbeams decorated with resonant plasmonic nanoantennas reveals a novel herringbone pattern of coexisting metallic and insulating domains intercepted and altered by ferroelastic domains, unlike previous reports on high-aspect-ratio VO crystals where the coexisting metal/insulator domains appear as alternating stripe phases perpendicular to the growth axis.

Heterogeneous nucleation and growth dynamics in the light-induced phase transition in vanadium dioxide.

We report on ultrafast optical investigations of the light-induced insulator-to-metal phase transition in vanadium dioxide with controlled disorder generated by substrate mismatch. These results reveal common dynamics of this optically-induced phase transition that are independent of this disorder. Above the fluence threshold for completing the transition to the rutile crystalline phase, we find a common time scale, independent of sample morphology, of 40.

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.

Hybrid Si-VO(2)-Au optical modulator based on near-field plasmonic coupling.

We present a computational design for an integrated electro-optic modulator based on near-field plasmonic coupling between gold nanodisks and a thin film of vanadium dioxide on a silicon substrate. Active modulation is achieved by applying a time-varying electric field to initiate large changes in the refractive index of vanadium dioxide. Significant decrease in device footprint (200 nm x 560 nm) and increase in extinction ratio per unit length (9 dB/µm) compared to state-of-the-art photonic and plasmonic modulators are predicted.

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.

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.

Polarization selective phase-change nanomodulator.

Manipulating optical signals below the diffraction limit is crucial for next-generation data-storage and telecommunication technologies. Although controlling the flow of light around nanoscale waveguides was achieved over a decade ago, modulating optical signals at terahertz frequencies within nanoscale volumes remains a challenge. Since the physics underlying any modulator relies on changes in dielectric properties, the incorporation of strongly electron-correlated materials (SECMs) has been proposed because they can exhibit orders of magnitude changes in electrical and optical properties with modest thermal, electrical or optical trigger signals.

Ultrafast phase transition via catastrophic phonon collapse driven by plasmonic hot-electron injection.

Ultrafast photoinduced phase transitions could revolutionize data-storage and telecommunications technologies by modulating signals in integrated nanocircuits at terahertz speeds. In quantum phase-changing materials (PCMs), microscopic charge, lattice, and orbital degrees of freedom interact cooperatively to modify macroscopic electrical and optical properties. Although these interactions are well documented for bulk single crystals and thin films, little is known about the ultrafast dynamics of nanostructured PCMs when interfaced to another class of materials as in this case to active plasmonic elements.

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).

Plasmonic probe of the semiconductor to metal phase transition in vanadium dioxide.

An array of 180 nm diameter gold nanoparticles (NPs) embedded in a thin vanadium dioxide film was used as a nanoscale probe of the thermochromic semiconductor-to-metal transition (SMT) in the VO2. The observed 30% reduction in plasmon dephasing time resulted from the interaction between the localized surface plasmon resonance of the NPs with the 1.4 eV electronic transitions in VO2.

Bandgap engineering of strained monolayer and bilayer MoS2.

We report the influence of uniaxial tensile mechanical strain in the range 0-2.2% on the phonon spectra and bandstructures of monolayer and bilayer molybdenum disulfide (MoS2) two-dimensional crystals. First, we employ Raman spectroscopy to observe phonon softening with increased strain, breaking the degeneracy in the E' Raman mode of MoS2, and extract a Grüneisen parameter of ~1.

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.