Continuous spectral and coupling-strength encoding with dual-gradient metasurfaces

Optical metasurfaces excel at enhancing and controlling light-matter interactions, which are primarily dictated by two factors: the spectral overlap of the resonances with target excitations in the material and the coupling-strength between them, where resonance linewidth and localized field enhancement are the governing influences. Current metasurface designs are limited to sampling a few discrete points within this vast 2D interaction parameter space or have varied only a single parameter. Symmetry-protected bound states in the continuum (BICs) allow precise control over the wavelength and linewidth of individual resonances, but rely on large arrangements of identical unit cells, limiting the continuous mapping of the parameter space. Therefore, optical platforms that concurrently probe the spectral and coupling parameters, so far, remained elusive. Here, we introduce the concept of dual-gradient metasurfaces for the continuous and simultaneous encoding of the spectral and coupling-strength of light-matter interactions, enabled by smooth local variations of the unit cell parameters. Contrary to conventional understanding, we demonstrate that BICs can be excited in such non-periodic systems provided the parameter variations are sufficiently small. Our dual-gradient metasurface exhibits an extraordinary resonance density, with each unit cell supporting a unique mode. This results in up to 27,500 distinct modes, all contained within a compact footprint. We apply this technology to surface-enhanced molecular sensing, capturing not only the spectral fingerprint of molecules but also unveiling an additional coupling-based dimension of spectroscopic data. This advancement in metasurface design paves the way for generalized light-matter coupling with metasurfaces, with applications ranging from on-chip spectrometer, to chirality encoding and AI-driven biochemical spectroscopy

Nanoscale mechanical manipulation of ultrathin SiN membranes enabling infrared near-field microscopy of liquid-immersed samples

Scattering scanning near-field optical microscopy (s-SNOM) is a powerful technique for mid-infrared spectroscopy at nanometer length scales. By investigating objects in aqueous environments through ultrathin membranes, s-SNOM has recently been extended towards label-free nanoscopy of the dynamics of living cells and nanoparticles, assessing both the optical and the mechanical interactions between the tip, the membrane and the liquid suspension underneath. Here, we report that the tapping AFM tip induces a reversible nanometric deformation of the membrane manifested as either an indentation or protrusion. This mechanism depends on the driving force of the tapping cantilever, which we exploit to minimize topographical deformations of the membrane to improve optical measurements. Furthermore, we show that the tapping phase, or phase delay between driving signal and tip oscillation, is a highly sensitive observable for quantifying the mechanics of adhering objects, exhibiting highest contrast for low tapping amplitudes where the membrane remains nearly flat. We correlate mechanical responses with simultaneously recorded spectroscopy data to reveal the thickness of nanometric water pockets between membrane and adhering objects. Besides a general applicability of depth profiling, our technique holds great promise for studying mechano-active biopolymers and living cells, biomaterials that exhibit complex behaviors when under a mechanical load

Environmental permittivity-asymmetric BIC metasurfaces with electrical reconfigurability

In the rapidly evolving field of nanophotonics, achieving precise spectral and temporal light manipulation at the nanoscale remains a critical challenge. While photonic bound states in the continuum (BICs) have emerged as a powerful means of controlling light, their common reliance on geometrical symmetry breaking for obtaining tailored resonances makes them highly susceptible to fabrication imperfections and fundamentally limits their maximum resonance quality factor. Here, we introduce the concept of environmental symmetry breaking by embedding identical resonators into a surrounding medium with carefully placed regions of contrasting refractive indexes, activating permittivity-driven quasi-BIC resonances without any alterations of the underlying resonator geometry and unlocking an additional degree of freedom for light manipulation through actively tuning the surrounding refractive index contrast. We demonstrate this concept by integrating polyaniline (PANI), an electro-optically active polymer, to achieve electrically reconfigurable qBICs. This integration not only demonstrates rapid switching speeds, and exceptional durability but also significantly boosts the system's optical response to environmental perturbations. Our strategy significantly expands the capabilities of resonant light manipulation through permittivity modulation, opening avenues for on-chip optical devices, advanced sensing, and beyond

Emergent resonances in a thin film tailored by optically-induced small permittivity asymmetries

Resonances are usually associated with finite systems - the vibrations of clamped strings in a guitar or the optical modes in a cavity defined by mirrors. In optics, resonances may be induced in infinite continuous media via periodic modulations of their optical properties. Here we demonstrate that periodic modulations of the permittivity of a featureless thin film can also act as a symmetry breaking mechanism, allowing the excitation of photonic $\textit{quasi}$-bound states in the continuum ($\textit{q}$BICs). By interfering two ultrashort laser pulses in the unbounded film, transient resonances can be tailored through different parameters of the pump beams. We show that the system offers resonances tunable in wavelength and quality-factor, and spectrally selective enhancement of third harmonic generation. Due to a fast decay of the permittivity asymmetry, we observe ultrafast dynamics, enabling time-selective near-field enhancement with picosecond precision. Optically-induced permittivity asymmetries may be exploited in on-demand weak to ultrastrong light-matter interaction regimes and light manipulation at dynamically chosen wavelengths in lithography-free metasurfaces

Yttrium Hydride Nanoantennas for Active Plasmonics

A key challenge for the development of active plasmonic nanodevices is the lack of materials with fully controllable plasmonic properties. In this work, we demonstrate that a plasmonic resonance in top-down nanofabricated yttrium antennas can be completely and reversibly turned on and off using hydrogen exposure. We fabricate arrays of yttrium nanorods and optically observe, in extinction spectra, the hydrogen-induced phase transition between the metallic yttrium dihydride and the insulating trihydride. Whereas the yttrium dihydride nanostructures exhibit a pronounced particle plasmon resonance, the transition to yttrium trihydride leads to a complete vanishing of the resonant behavior. The plasmonic resonance in the dihydride state can be tuned over a wide wavelength range by simply varying the size of the nanostructures. Furthermore, we develop an analytical diffusion model to explain the temporal behavior of the hydrogen loading and unloading trajectories observed in our experiments and gain information about the thermodynamics of our device. Thus, our nanorod system serves as a versatile basic building block for active plasmonic devices ranging from switchable perfect absorbers to active local heating control elements

Quantitative Angle-Resolved Small-Spot Reflectance Measurements on Plasmonic Perfect Absorbers: Impedance Matching and Disorder Effects

Plasmonic devices with absorbance close to unity have emerged as essential building blocks for a multitude of technological applications ranging from trace gas detection to infrared imaging. A crucial requirement for such elements is the angle independence of the absorptive performance. In this work, we develop theoretically and verify experimentally a quantitative model for the angular behavior of plasmonic perfect absorber structures based on an optical impedance matching picture. To achieve this, we utilize a simple and elegant <i>k</i>-space measurement technique to record quantitative angle-resolved reflectance measurements on various perfect absorber structures. Particularly, this method allows quantitative reflectance measurements on samples where only small areas have been nanostructured, for example, by electron-beam lithography. Combining these results with extensive numerical modeling, we find that matching of both the real and imaginary parts of the optical impedance is crucial to obtain perfect absorption over a large angular range. Furthermore, we successfully apply our model to the angular dispersion of perfect absorber geometries with disordered plasmonic elements as a favorable alternative to current array-based designs

Plasmonic Smart Dust for Probing Local Chemical Reactions

Locally probing chemical reactions or catalytic processes on surfaces under realistic reaction conditions has remained one of the main challenges in materials science and heterogeneous catalysis. Where conventional surface interrogation techniques usually require high-vacuum conditions or ensemble average measurements, plasmonic nanoparticles excel in extreme light focusing and can produce highly confined electromagnetic fields in subwavelength volumes without the need for complex near-field microscopes. Here, we demonstrate an all-optical probing technique based on plasmonic smart dust for monitoring local chemical reactions in real time. The silica shell-isolated gold nanoparticles that form the smart dust can work as strong light concentrators and optically report subtle environmental changes at their pinning sites on the probed surface during reaction processes. As a model system, we investigate the hydrogen dissociation and subsequent uptake trajectory in palladium with both “dust-on-film” and “film-on-dust” platforms. Using time-resolved single particle measurements, we demonstrate that our technique can in situ encode chemical reaction information as optical signals for a variety of surface morphologies. The presented technique offers a unique scheme for real-time, label-free, and high-resolution probing of local reaction kinetics in a plethora of important chemical reactions on surfaces, paving the way toward the development of inexpensive and high-output reaction sensors for real-world applications

Si Metasurface Supporting Multiple Quasi-BICs for Degenerate Four-Wave Mixing

Dielectric metasurfaces supporting quasi-bound states in the continuum (qBICs) enable high field enhancement with narrow-linewidth resonances in the visible and near-infrared ranges. The resonance emerges when distorting the meta-atom's geometry away from a symmetry-protected BIC condition and, usually, a given design can sustain one or two of these states. In this work, we introduce a silicon-on-silica metasurface that simultaneously supports up to four qBIC resonances in the near-infrared region. This is achieved by combining multiple symmetry-breaking distortions on an elliptical cylinder array. By pumping two of these resonances, the nonlinear process of degenerate four-wave mixing is experimentally realized. By comparing the nonlinear response with that of an unpatterned silicon film, the near-field enhancement inside the nanostructured dielectric is revealed. The presented results demonstrate independent geometric control of multiple qBICs and their interaction trough wave mixing processes, opening new research pathways in nanophotonics, with potential applications in information multiplexing, multi-wavelength sensing and nonlinear imaging

Pixelated High‑<i>Q</i> Metasurfaces for in Situ Biospectroscopy and Artificial Intelligence-Enabled Classification of Lipid Membrane Photoswitching Dynamics

Nanophotonic devices excel at confining light into intense hot spots of electromagnetic near fields, creating exceptional opportunities for light–matter coupling and surface-enhanced sensing. Recently, all-dielectric metasurfaces with ultrasharp resonances enabled by photonic bound states in the continuum (BICs) have unlocked additional functionalities for surface-enhanced biospectroscopy by precisely targeting and reading out the molecular absorption signatures of diverse molecular systems. However, BIC-driven molecular spectroscopy has so far focused on end point measurements in dry conditions, neglecting the crucial interaction dynamics of biological systems. Here, we combine the advantages of pixelated all-dielectric metasurfaces with deep learning-enabled feature extraction and prediction to realize an integrated optofluidic platform for time-resolved in situ biospectroscopy. Our approach harnesses high-Q metasurfaces specifically designed for operation in a lossy aqueous environment together with advanced spectral sampling techniques to temporally resolve the dynamic behavior of photoswitchable lipid membranes. Enabled by a software convolutional neural network, we further demonstrate the real-time classification of the characteristic cis and trans membrane conformations with 98% accuracy. Our synergistic sensing platform incorporating metasurfaces, optofluidics, and deep learning reveals exciting possibilities for studying multimolecular biological systems, ranging from the behavior of transmembrane proteins to the dynamic processes associated with cellular communication

Origin of optical nonlinearity in plasmonic semiconductor nanostructures

The development of nanoscale nonlinear elements in photonic integrated circuits is hindered by the physical limits to the nonlinear optical response of dielectrics, which requires that the interacting waves propagate in transparent volumes for distances much longer than their wavelength. Here we present experimental evidence that optical nonlinearities in doped semiconductors are due to free-electron and their efficiency could exceed by several orders of magnitude that of conventional dielectric nonlinearities. Our experimental findings are supported by comprehensive computational results based on the hydrodynamic modeling, which naturally includes nonlocal effects, of the free-electron dynamics in heavily doped semiconductors. By studying third-harmonic generation from plasmonic nanoantenna arrays made out of heavily n-doped InGaAs with increasing levels of free-carrier density, we discriminate between hydrodynamic and dielectric nonlinearities. As a result, the value of maximum nonlinear efficiency as well as its spectral location can now be controlled by tuning the doping level. Having employed the common material platform InGaAs/InP that supports integrated waveguides, our findings pave the way for future exploitation of plasmonic nonlinearities in all-semiconductor photonic integrated circuits