Trends in Nanophotonics-Enabled Optofluidic Biosensors

Optofluidic sensors integrate photonics with micro/nanofluidics to realize compact devices for the label-free detection of molecules and the real-time monitoring of dynamic surface binding events with high specificity, ultrahigh sensitivity, low detection limit, and multiplexing capability. Nanophotonic structures composed of metallic and/or dielectric building blocks excel at focusing light into ultrasmall volumes, creating enhanced electromagnetic near-fields ideal for amplifying the molecular signal readout. Furthermore, fluidic control on small length scales enables precise tailoring of the spatial overlap between the electromagnetic hotspots and the analytes, boosting light-matter interaction, and can be utilized to integrate advanced functionalities for the pre-treatment of samples in real-world-use cases, such as purification, separation, or dilution. In this review, the authors highlight current trends in nanophotonics-enabled optofluidic biosensors for applications in the life sciences while providing a detailed perspective on how these approaches can synergistically amplify the optical signal readout and achieve real-time dynamic monitoring, which is crucial in biomedical assays and clinical diagnostics

Metallic and All‐Dielectric Metasurfaces Sustaining Displacement‐Mediated Bound States in the Continuum

Bound states in the continuum (BICs) are localized electromagnetic modes within the continuous spectrum of radiating waves. Due to their infinite lifetimes without radiation losses, BICs are driving research directions in lasing, non-linear optical processes, and sensing. However, conventional methods for converting BICs into leaky resonances, or quasi-BICs, with high-quality factors typically rely on breaking the in-plane inversion symmetry of the metasurface and often result in resonances that are strongly dependent on the angle of the incident light, making them unsuitable for many practical applications. Here, an emerging class of BIC-driven metasurfaces is numerically analyzed and experimentally demonstrated, where the coupling to the far field is controlled by the displacement of individual resonators. In particular, both all-dielectric and metallic as well as positive and inverse displacement-mediated metasurfaces sustaining angular-robust quasi-BICs are investigated in the mid-infrared spectral region. Their optical behavior with regard to changes in the angle of incidence is investigated and experimentally shows their superior performance compared to two conventional alternatives: silicon-based tilted ellipses and cylindrical nanoholes in gold. These findings are anticipated to open exciting perspectives for bio-sensing, conformal optical devices, and photonic devices using focused light

Metallic and All-Dielectric Metasurfaces Sustaining Displacement-Mediated Bound States in the Continuum

Bound states in the continuum (BICs) are localized electromagnetic modes within the continuous spectrum of radiating waves. Due to their infinite lifetimes without radiation losses, BICs are driving research directions in lasing, non-linear optical processes, and sensing. However, conventional methods for converting BICs into leaky resonances, or quasi-BICs, with high-quality factors typically rely on breaking the in-plane inversion symmetry of the metasurface and often result in resonances that are strongly dependent on the angle of the incident light, making them unsuitable for many practical applications. Here, we numerically analyze and experimentally demonstrate an emerging class of BIC-driven metasurfaces, where the coupling to the far field is controlled by the displacement of individual resonators. In particular, we investigate both all-dielectric and metallic as well as positive and inverse displacement-mediated metasurfaces sustaining angular-robust quasi-BICs in the mid-infrared spectral region. We explore their behavior with changes in the incidence angle of illumination and experimentally show their superior performance compared to two conventional alternatives: silicon-based tilted ellipses and cylindrical nanoholes in gold. We anticipate our findings to open exciting perspectives for bio-sensing, conformal optical devices, and photonic devices using focused light.Comment: 27 pages, 7 figures, 1 tabl

Mirror‐Coupled Plasmonic Bound States in the Continuum for Tunable Perfect Absorption

Tailoring critical light-matter coupling is a fundamental challenge of nanophotonics, impacting fields from higher harmonic generation and energy conversion to surface-enhanced spectroscopy. Plasmonic perfect absorbers (PAs), where resonant antennas couple to their mirror images in adjacent metal films, excel at obtaining different coupling regimes by tuning the antenna-film gap size. However, practical PA applications require constant gap size, making it impossible to maintain critical coupling beyond singular wavelengths. Here, a new approach for plasmonic PAs is introduced by combining mirror-coupled resonances with the unique loss engineering capabilities of plasmonic quasi-bound states in the continuum. This novel combination allows to tailor the light–matter interaction within the under-coupling, over-coupling, and critical coupling regimes using flexible tuning knobs including asymmetry parameter, dielectric gap, and geometrical scaling factor. The study demonstrates a pixelated PA metasurface with optimal absorption over a broad range of mid-infrared wavenumbers (950–2000 cm−1) using only a single gap size and applies it for multispectral surface-enhanced molecular spectroscopy. Moreover, the asymmetry parameter enables convenient adjustment of the quality factor and resonance amplitude. This concept expands the capabilities and flexibility of traditional gap-tuned PAs, opening new perspectives for miniaturized sensing platforms towards on-chip and in situ detection

Multi-band metasurface-driven surface-enhanced infrared absorption spectroscopy for improved characterization of in-situ electrochemical reactions

Surface-enhanced spectroscopy techniques are the method-of-choice to characterize adsorbed intermediates occurring during electrochemical reactions, which are crucial in realizing a green sustainable future. Characterizing species with low coverages or short lifetimes have so far been limited by low signal enhancement. Recently, metasurface-driven surface-enhanced infrared absorption spectroscopy (SEIRAS) has been pioneered as a promising narrowband technology to study single vibrational modes of electrochemical interfaces during CO oxidation. However, many reactions involve several species or configurations of adsorption that need to be monitored simultaneously requiring reproducible and broadband sensing platforms to provide a clear understanding of the underlying electrochemical processes. Here, we experimentally realize multi-band metasurface-driven SEIRAS for the in-situ study of electrochemical CO2 reduction on a Pt surface. We develop an easily reproducible and spectrally-tunable platinum nano-slot metasurface. Two CO adsorption configurations at 2030 cm-1 and 1840 cm-1 are locally enhanced as a proof of concept that can be extended to more vibrational bands. Our platform provides a 41-fold enhancement in the detection of characteristic absorption signals compared to conventional broadband electrochemically roughened platinum films. A straightforward methodology is outlined starting by baselining our system in CO saturated environment and clearly detecting both configurations of adsorption, in particular the hitherto hardly detectable CO bridge configuration. Then, thanks to the signal enhancement provided by our platform, we find that the CO bridge configuration on platinum does not play a significant role during CO2 reduction in an alkaline environment. We anticipate that our technology will guide researchers in developing similar sensing platforms.Comment: 21 pages, 4 figure

Mirror-coupled plasmonic bound states in the continuum for tunable perfect absorption

Tailoring critical light-matter coupling is a fundamental challenge of nanophotonics, impacting diverse fields from higher harmonic generation and energy conversion to surface-enhanced spectroscopy. Plasmonic perfect absorbers (PAs), where resonant antennas couple to their mirror images in adjacent metal films, have been instrumental for obtaining different coupling regimes by tuning the antenna-film distance. However, for on-chip uses, the ideal PA gap size can only match one wavelength, and wide range multispectral approaches remain challenging. Here, we introduce a new paradigm for plasmonic PAs by combining mirror-coupled resonances with the unique loss engineering capabilities of plasmonic bound states in the continuum (BICs). Our BIC-driven PA platform leverages the asymmetry of the constituent meta-atoms as an additional degree of freedom for reaching the critical coupling (CC) condition, delivering resonances with unity absorbance and high quality factors approaching 100 in the mid-infrared. Such a platform holds flexible tuning knobs including asymmetry parameter, dielectric gap, and geometrical scaling factor to precisely control the coupling condition, resonance frequency, and selective enhancement of magnetic and electric fields while maintaining CC. We demonstrate a pixelated PA metasurface with optimal absorption over a broad range of mid-infrared frequencies (950 ~ 2000 1/cm) using only a single spacer layer thickness and apply it for multispectral surface-enhanced molecular spectroscopy in tailored coupling regimes. Our concept greatly expands the capabilities and flexibility of traditional gap-tuned PAs, opening new perspectives for miniaturized sensing platforms towards on-chip and in-situ detection.Comment: Main text and supporting information, 31 pages, 5 Figures manuscript + 11 Supporting Figure

All‐Dielectric Programmable Huygens' Metasurfaces

Low‐loss nanostructured dielectric metasurfaces have emerged as a breakthrough platform for ultrathin optics and cutting‐edge photonic applications, including beam shaping, focusing, and holography. However, the static nature of their constituent materials has traditionally limited them to fixed functionalities. Tunable all‐dielectric infrared Huygens' metasurfaces consisting of multi‐layer Ge disk meta‐units with strategically incorporated non‐volatile phase change material Ge3Sb2Te6 are introduced. Switching the phase‐change material between its amorphous and crystalline structural state enables nearly full dynamic light phase control with high transmittance in the mid‐IR spectrum. The metasurface is realized experimentally, showing post‐fabrication tuning of the light phase within a range of 81% of the full 2π phase shift. Additionally, the versatility of the tunable Huygen's metasurfaces is demonstrated by optically programming the spatial light phase distribution of the metasurface with single meta‐unit precision and retrieving high‐resolution phase‐encoded images using hyperspectral measurements. The programmable metasurface concept overcomes the static limitations of previous dielectric metasurfaces, paving the way for “universal” metasurfaces and highly efficient, ultracompact active optical elements like tunable lenses, dynamic holograms, and spatial light modulators

Double-layer graphene for enhanced tunable infrared plasmonics

Graphene is emerging as a promising material for photonic applications owing to its unique optoelectronic properties. Graphene supports tunable, long-lived and extremely confined plasmons that have great potential for applications such as biosensing and optical communications. However, in order to excite plasmonic resonances in graphene, this material requires a high doping level, which is challenging to achieve without degrading carrier mobility and stability. Here, we demonstrate that the infrared plasmonic response of a graphene multilayer stack is analogous to that of a highly doped single layer of graphene, preserving mobility and supporting plasmonic resonances with higher oscillator strength than previously explored single-layer devices. Particularly, we find that the optically equivalent carrier density in multilayer graphene is larger than the sum of those in the individual layers. Furthermore, electrostatic biasing in multilayer graphene is enhanced with respect to single layer due to the redistribution of carriers over different layers, thus extending the spectral tuning range of the plasmonic structure. The superior effective doping and improved tunability of multilayer graphene stacks should enable a plethora of future infrared plasmonic devices with high optical performance and wide tunability.Peer ReviewedPostprint (published version

Long-term stability of capped and buffered palladium-nickel thin films and nanostructures for plasmonic hydrogen sensing applications

One of the main challenges in optical hydrogen sensing is the stability of the sensor material. We found and studied an optimized material combination for fast and reliable optical palladium-based hydrogen sensing devices. It consists of a palladium-nickel alloy that is buffered by calcium fluoride and capped with a very thin layer of platinum. Our system shows response times below 10 s and almost no short-term aging effects. Furthermore, we successfully incorporated this optimized material system into plasmonic nanostructures, laying the foundation for a stable and sensitive hydrogen detector

Plasmonic Bound States in the Continuum to Tailor Light-Matter Coupling

Plasmon resonances play a pivotal role in enhancing light-matter interactions in nanophotonics, but their low-quality factors have hindered applications demanding high spectral selectivity. Even though symmetry-protected bound states in the continuum with high-quality factors have been realized in dielectric metasurfaces, impinging light is not efficiently coupled to the resonant metasurfaces and is lost in the form of reflection due to low intrinsic losses. Here, we demonstrate a novel design and 3D laser nanoprinting of plasmonic nanofin metasurfaces, which support symmetry-protected bound states in the continuum up to 4th order. By breaking the nanofins out-of-plane symmetry in parameter space, we achieve high-quality factor (up to 180) modes under normal incidence. We reveal that the out-of-plane symmetry breaking can be fine-tuned by the triangle angle of the 3D nanofin meta-atoms, opening a pathway to precisely control the ratio of radiative to intrinsic losses. This enables access to the under-, critical-, and over-coupled regimes, which we exploit for pixelated molecular sensing. Depending on the coupling regime we observe negative, no, or positive modulation induced by the analyte, unveiling the undeniable importance of tailoring light-matter interaction. Our demonstration provides a novel metasurface platform for enhanced light-matter interaction with a wide range of applications in optical sensing, energy conversion, nonlinear photonics, surface-enhanced spectroscopy, and quantum optics.Comment: 33 pages, 4 figures, 9 supplementary figure