Gradient High-Q Dielectric Metasurfaces for Broadband Sensing and Control of Vibrational Light-Matter Coupling.

Surface-enhanced infrared absorption spectroscopy (SEIRA) has emerged as a powerful technique for ultrasensitive chemical-specific analysis. SEIRA can be realized by employing metasurfaces that can enhance light-matter interactions in the spectral bands of molecular vibrations. Increasing sample complexity emphasizes the need for metasurfaces that can operate simultaneously at different spectral bands, both accessing rich spectral information over a broad band, and resolving subtle differences in the absorption fingerprints through narrow-band resonances. Here, a novel concept of resonance-gradient metasurfaces is introduced, where the required spectral selectivity is achieved via local high-quality-factor (high-Q) resonances, while the continuous coverage of a broad band is enabled by the gradual adjustment of the unit-cell dimensions along the planar structure. The highly tailorable design of the gradient metasurfaces provides flexibility for shaping the spectral sampling density to match the relevant bands of target analytes while keeping a compact device footprint. The versatility of the gradient metasurfaces is demonstrated through several sensing scenarios, including polymer mixture deconvolution, detecting a multistep bioassay, and identification of the onset of vibrational strong coupling regime. The proposed gradient-resonance platform significantly contributes to the rapidly evolving landscape of nonlocal metasurfaces, enabling applications in molecular detection and analysis of fundamental light-matter interaction phenomena.

Spectral Tuning of High-Harmonic Generation with Resonance-Gradient Metasurfaces.

High-index dielectric subwavelength structures and metasurfaces are capable of enhancing light-matter interaction by orders of magnitude via geometry-dependent optical resonances. This enhancement, however, comes with a fundamental limitation of a narrow spectral range of operation in the vicinity of one or few resonant frequencies. Here, this limitation is tackled by introducing an innovative and practical approach to achieve spectrally tunable enhancement of light-matter interaction with resonant metasurfaces. Resonance-gradient metasurfaces are designed and fabricated with varying geometrical parameters that translate into resonant frequencies dependence on one of the coordinates of the metasurface. The metasurfaces are composed of bone-like nanoresonators, which are made of germanium and support high-quality optical resonances in the mid-IR spectral range. The concept is applied to observe the resonant enhancement of the third and fifth harmonics generated from the gradient metasurfaces being used in conjunction with a tunable excitation laser to provide a wide spectral coverage of resonantly-enhanced tunable generation of multiple optical harmonics.

Coherent Control of Topological States in an Integrated Waveguide Lattice.

Topological photonics holds the promise for enhanced robustness of light localization and propagation enabled by the global symmetries of the system. While traditional designs of topological structures rely on lattice symmetries, there is an alternative strategy based on accidentally degenerate modes of the individual meta-atoms. Using this concept, we experimentally realize topological edge state in an array of silicon nanostructured waveguides, each hosting a pair of degenerate modes at telecom wavelengths. Exploiting the hybrid nature of the topological mode, we implement its coherent control by adjusting the phase between the degenerate modes and demonstrating selective excitation of bulk or edge states. The resulting field distribution is imaged via third harmonic generation showing the localization of topological modes as a function of the relative phase of the excitations. Our results highlight the impact of engineered accidental degeneracies on the formation of topological phases, extending the opportunities stemming from topological nanophotonic systems.

Multifunctional and Transformative Metaphotonics with Emerging Materials.

Future technologies underpinning multifunctional physical and chemical systems and compact biological sensors will rely on densely packed transformative and tunable circuitry employing nanophotonics. For many years, plasmonics was considered as the only available platform for subwavelength optics, but the recently emerged field of resonant metaphotonics may provide a versatile practical platform for nanoscale science by employing resonances in high-index dielectric nanoparticles and metasurfaces. Here, we discuss the recently emerged field of metaphotonics and describe its connection to material science and chemistry. For tunabilty, metaphotonics employs a variety of the recently highlighted materials such as polymers, perovskites, transition metal dichalcogenides, and phase change materials. This allows to achieve diverse functionalities of metasystems and metasurfaces for efficient spatial and temporal control of light by employing multipolar resonances and the physics of bound states in the continuum. We anticipate expanding applications of these concepts in nanolasers, tunable metadevices, metachemistry, as well as a design of a new generation of chemical and biological ultracompact sensing devices.

Observation of Ultrafast Self-Action Effects in Quasi-BIC Resonant Metasurfaces.

High-index dielectric metasurfaces can support sharp optical resonances enabled by the physics of bound states in the continuum (BICs) often manifested in experiments as quasi-BIC resonances. They provide a way to enhance light-matter interaction at the subwavelength scale bringing novel opportunities for nonlinear nanophotonics. Strong narrow-band field enhancement in quasi-BIC metasurfaces leads to an extreme sensitivity to a change of the refractive index that may limit nonlinear functionalities for the pump intensities beyond the perturbative regime. Here we study ultrafast self-action effects observed in quasi-BIC silicon metasurfaces and demonstrate how they alter the power dependence of the third-harmonic generation efficiency. We study experimentally a transition from the subcubic to supercubic regimes for the generated third-harmonic power driven by a blue-shift of the quasi-BIC in the multiphoton absorption regime. Our results suggest a way to implement ultrafast nonlinear dynamics in high-index resonant dielectric metasurfaces for nonlinear meta-optics beyond the perturbative regime.

Experimental observation of topological Z2 exciton-polaritons in transition metal dichalcogenide monolayers.

The rise of quantum science and technologies motivates photonics research to seek new platforms with strong light-matter interactions to facilitate quantum behaviors at moderate light intensities. Topological polaritons (TPs) offer an ideal platform in this context, with unique properties stemming from resilient topological states of light strongly coupled with matter. Here we explore polaritonic metasurfaces based on 2D transition metal dichalcogenides (TMDs) as a promising platform for topological polaritonics. We show that the strong coupling between topological photonic modes of the metasurface and excitons in TMDs yields a topological polaritonic Z2 phase. We experimentally confirm the emergence of one-way spin-polarized edge TPs in metasurfaces integrating MoSe2 and WSe2. Combined with the valley polarization in TMD monolayers, the proposed system enables an approach to engage the photonic angular momentum and valley and spin of excitons, offering a promising platform for photonic/solid-state interfaces for valleytronics and spintronics.

Rewritable and Tunable Laser-Induced Optical Gratings in Phase-Change Material Films.

Laser-induced periodic surface structures (LIPSS) can be fabricated in virtually all types of solid materials and show great promise for efficient and scalable production of surface patterns with applications in various fields from photonics to engineering. While the majority of LIPSS manifest as modifications of the surface relief, in special cases, laser impact can also lead to periodic modulation of the material phase state. Here, we report on the fabrication of high-quality periodic structures in the films of phase-change material Ge2Sb2Te5 (GST). Due to considerable contrast of the refractive index of GST in its crystalline and amorphous states, the fabricated structures provide strong spatial modulation of the optical properties, which facilitates their applications. By changing the excitation laser wavelength, we observe the scaling of the grating period as well as transition between formation of different types of LIPSS. We optimize the laser exposure routine to achieve large-scale high-quality phase-change gratings with controllable period and demonstrate their reversible tunability through intermediate amorphization steps. Our results reveal the prospects of fast and rewritable fabrication of high-quality periodic structures for photonics and can serve as a guideline for further development of phase-change material-based optical elements.

Perovskite-Gallium Phosphide Platform for Reconfigurable Visible-Light Nanophotonic Chip.

Reduction of the wavelength in on-chip light circuitry is critically important not only for the sake of keeping up with Moore's law for photonics but also for reaching toward the spectral ranges of operation of emerging materials, such as atomically thin semiconductors, vacancy-based single-photon emitters, and quantum dots. This requires efficient and tunable light sources as well as compatible waveguide networks. For the first challenge, halide perovskites are prospective materials that enable cost-efficient fabrication of micro- and nanolasers. On the other hand, III-V semiconductor nanowires are optimal for guiding of visible light as they exhibit a high refractive index as well as excellent shape and crystalline quality beneficial for strong light confinement and long-range waveguiding. Here, we develop an integrated platform for visible light that comprises gallium phosphide (GaP) nanowires directly embedded into compact CsPbBr3-based light sources. In our devices, perovskite microcrystals support stable room-temperature lasing and broadband chemical tuning of the emission wavelength in the range of 530-680 nm, whereas GaP nanowaveguides support efficient outcoupling of light, its subwavelength (<200 nm) confinement, and long-range guiding over distances more than 20 µm. As a highlight of our approach, we demonstrate sequential transfer and conversion of light using an intermediate perovskite nanoparticle in a chain of GaP nanowaveguides.

Nonlinear polaritons in a monolayer semiconductor coupled to optical bound states in the continuum.

Optical bound states in the continuum (BICs) provide a way to engineer very narrow resonances in photonic crystals. The extended interaction time in these systems is particularly promising for the enhancement of nonlinear optical processes and the development of the next generation of active optical devices. However, the achievable interaction strength is limited by the purely photonic character of optical BICs. Here, we mix the optical BIC in a photonic crystal slab with excitons in the atomically thin semiconductor MoSe2 to form nonlinear exciton-polaritons with a Rabi splitting of 27 meV, exhibiting large interaction-induced spectral blueshifts. The asymptotic BIC-like suppression of polariton radiation into the far field toward the BIC wavevector, in combination with effective reduction of the excitonic disorder through motional narrowing, results in small polariton linewidths below 3 meV. Together with a strongly wavevector-dependent Q-factor, this provides for the enhancement and control of polariton-polariton interactions and the resulting nonlinear optical effects, paving the way toward tuneable BIC-based polaritonic devices for sensing, lasing, and nonlinear optics.

Mapping plasmonic topological states at the nanoscale.

We report on the first experimental observation of topological edge states in zigzag chains of plasmonic nanodisks. We demonstrate that such edge states can be selectively excited with the linear polarization of the incident light, and visualize them directly by near-field scanning optical microscopy. Our work provides experimental verification of a novel paradigm for manipulating light at the nanoscale in topologically nontrivial structures.

Demonstration of unusual nanoantenna array modes through direct reconstruction of the near-field signal.

We perform complex investigation of the distribution of electromagnetic fields in the vicinity of an array of silver nanoantennas, which can operate as an efficient light trapping structure in the visible spectral range. In theory, this array should support unusual collective modes that possess an advantageous distribution of local electric fields, ensuring both strong field localization beneath nanoantennas and a low level of optical losses inside the metal. Using an aperture-type near-field scanning optical microscope (NSOM), we obtain near-field patterns that show excellent agreement with the NSOM signal, directly reconstructed from rigorous numerical simulations using an approach based on the electromagnetic reciprocity theorem. The agreement between theory and experiment allows us to claim the first-time experimental verification of the existence of collective modes with such properties in an array of silver nanoantennas. The confirmation of this physical phenomenon opens the door to a new class of light-trapping structures for photovoltaics.

Nanoscale patterning of metal nanoparticle distribution in glasses.

: We show that electric field imprinting technique allows for patterning of metal nanoparticles in the glass matrix at the subwavelength scale. The formation of glass-metal nanocomposite strips with a width down to 150 nm is demonstrated. The results of near-field microscopy of imprinted patterns are in good agreement with the performed numerical modeling. Atomic force microscopy reveals that imprinting also results in the formation of nanoscale surface profile with the height going down with the decrease of the strip width. The experiments prove the applicability of this technique for the fabrication of nanoscale plasmonic components.

Mie scattering as a cascade of Fano resonances.

We reveal that the resonant Mie scattering by high-index dielectric nanoparticles can be presented through cascades of Fano resonances. We employ the exact solution of Maxwell's equations and demonstrate that the Lorenz-Mie coefficients of the Mie problem can be expressed generically as infinite series of Fano functions as they describe interference between the background radiation originated from an incident wave and narrow-spectrum Mie scattering modes that lead to Fano resonances.