Metasurfaces based on quasi-bound states in the continuum (quasi-BICs) constitute an emerging toolkit in nanophotonic sensing as they sustain high quality factor resonances and substantial near-field enhancements. It is demonstrated that silicon metasurfaces composed of crescent shaped meta-atoms provide tailored light-matter interaction controlled by the crescent geometry. Significantly, this metasurface not only exhibits a fundamental quasi-BIC resonance, but also supports a higher-order resonance with tunable electromagnetic field enhancement and advantageous properties for sensing. The higher-order resonance shows twice the sensitivity of the fundamental one for bulk refractive index sensing. It is further demonstrated that both the fundamental and higher-order resonances can be exploited for sensing ultrathin layers of biomolecules in air and buffer solutions. Specifically, when measuring in buffer solution, the figure of merit of the sensor, defined as the change in the spectral position of the resonance normalized to its full width at half maximum, is a factor of 2.5 larger for the higher-order resonance when compared to the fundamental one. Due to its high sensitivity and potential for straightforward microfluidic integration, the silicon crescent metasurface is ideally suited for real-time and in situ biosensing, enabling compact sensing devices for a wide range of diagnostic applications.
Photonic crystals (PhCs) display photonic stop bands (PSBs) and at the edges of these PSBs transport light with reduced velocity, enabling the PhCs to confine and manipulate incident light with enhanced light–matter interaction. Intense research has been devoted to leveraging the optical properties of PhCs for the development of optical sensors for bioassays, diagnosis, and environmental monitoring. These applications have furthermore benefited from the inherently large surface area of PhCs, giving rise to high analyte adsorption and the wide range of options for structural variations of the PhCs leading to enhanced light–matter interaction. Here, we focus on bottom-up assembled PhCs and review the significant advances that have been made in their use as label-free sensors. We describe their potential for point-of-care devices and in the review include their structural design, constituent materials, fabrication strategy, and sensing working principles. We thereby classify them according to five sensing principles: sensing of refractive index variations, sensing by lattice spacing variations, enhanced fluorescence spectroscopy, surface-enhanced Raman spectroscopy, and configuration transitions.
All-dielectric metasurfaces supporting photonic bound states in the continuum (BICs) are an exciting toolkit for achieving resonances with ultranarrow linewidths. However, the transition from theory to experimental realization can significantly reduce the optical performance of BIC-based nanophotonic systems, severely limiting their application potential. Here, we introduce a combined numerical/experimental methodology for predicting how unavoidable tolerances in nanofabrication such as random geometrical variations affect the performance of different BIC metasurface designs. We compare several established all-dielectric BIC unit cell geometries with broken in-plane inversion symmetry including tilted ellipses, asymmetric double rods, and split rings. Significantly, even for low fabrication-induced geometrical changes, both the BIC resonance amplitude and its quality factor (Q-factor) are significantly reduced. We find that the all-dielectric ellipses maintain the highest Q-factors throughout the geometrical variation range, whereas the rod and split ring geometries fall off more quickly. The same behavior is confirmed experimentally, where geometrical variation values are derived from automated processing of sets of scanning electron microscopy (SEM) images. Our methodology provides crucial insights into the performance degradation of BIC metasurfaces when moving from simulations to fabricated samples and will enable the development of robust, high-Q, and easy to manufacture nanophotonic platforms for applications ranging from biomolecular sensing to higher harmonic generation.
The construction of ordered nanoparticle arrays is important for nanophotonics and sensing applications. We report a facile technology for continuous-flow fabrication of particle-laden plasmonic microcapsules (PLPMs) by combining droplet microfluidics, nanoparticle self-assembly and thin film deposition. The metallic hierarchical nanostructures on PLPMs are presented with high-density "hot-spot" scattering sites with the nanoarray pitch and gap distance being controlled by the deposited metal film thickness and nanoparticle size. The noble metal "hot-spots" show high, localized surface plasmon resonance according to the near-field electromagnetic field enhancement. Surface-enhanced Raman scattering (SERS) analytical enhancement factors of >10 can be obtained with good reproducibility using 4-methylbenzenethiol (4-MBT) as a probe molecule and Au or Ag as the metal layer. The droplet microfluidics platform enables continuous generation of homogeneous microcapsules with high frequency. This proposed strategy therefore combines advantages from both top-down (creation of microdroplets and deposition of the metal film) and bottom-up (self-assembly of nanoparticles) processes with flexibility in material selection (nanoparticles and polymer) and structure scaling (metal layer thickness, nanoparticle size and microcapsule size). Therefore, it provides a fast and reliable method of producing plasmonic microsensors.
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. Here, we demonstrate the design and 3D laser nanoprinting of plasmonic nanofin metasurfaces, which support symmetry-protected bound states in the continuum up to the fourth order. By breaking the nanofins’ out-of-plane symmetry in parameter space, we achieve high-quality factor (up to 180) modes under normal incidence. The out-of-plane symmetry breaking can be fine-tuned by the nanofins’ triangle angle, 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. We observe a strong dependence of the sensing performance on the coupling regime, demonstrating the importance of judicious tailoring of light-matter interactions. Our demonstration provides a metasurface platform for enhanced light-matter interaction with a wide range of applications.
Construction of textured bioinspired surfaces with refined structures that exhibit superior wetting properties is of great importance for many applications ranging from self-cleaning, antibiofouling, anti-icing, oil/water separation, smart membrane, and microfluidic devices. Previously, the preparation of artificial surfaces generally relies on the combination of different approaches together, which is a lack of flexibility to control over the individual architecture unit, the surface topology, as well as the complex procedure needed. In this work, we report a method for rapid fabrication of three-tier hierarchical microunits (structures consisting of multiple levels) using a facile droplet microfluidics approach. These units include the first-tier microspheres consisting of the second-tier close-packed polystyrene (PS) nanoparticles decorated with the third-tier elegant polymer nanowrinkles. These nanowrinkles on the PS nanoparticles are formed according to the interfacial instability induced by gradient photopolymerization of N-isopropylacrylamide (NIPAM) monomers. The formation process and topologies of nanowrinkles can be regulated by the photopolymerization process and the fraction of carboxylic groups on the PS nanoparticle surface. Such a hierarchical microsphere mimics individual units of bioinspired surfaces. Therefore, the surfaces from self-assembly of these fabricated two-tier and three-tier hierarchical microunits collectively exhibit "gecko" and "rose petal" wetting states, with the micro-and nanoscale structures amplifying the initial hydrophobicity but still being highly adhesive to water. This approach offers promising advantages of high-yield fabrication, precise control over the size and component of the microspheres, and integration of microfluidic droplet generation, colloidal nanoparticle self-assembly, and interfacial polymerization-induced nanowrinkles in a straightforward manner.
Hierarchical plasmonic–photonic microspheres (PPMs) with high controllability in their structures and optical properties have been explored toward surface-enhanced Raman spectroscopy. The PPMs consist of gold nanocrystal (AuNC) arrays (3rd-tier) anchored on a hexagonal nanopattern (2nd-tier) assembled from silica nanoparticles (SiO 2 NPs) where the uniform microsphere backbone is termed the 1st-tier. The PPMs sustain both photonic stop band (PSB) properties, resulting from periodic SiO 2 NP arrangements of the 2nd-tier, and a surface plasmon resonance (SPR), resulting from AuNC arrays of the 3rd-tier. Thanks to the synergistic effects of the photonic crystal (PC) structure and the AuNC array, the electromagnetic (EM) field in such a multiscale composite structure can tremendously be enhanced at certain wavelengths. These effects are demonstrated by experimentally evaluating the Raman enhancement of benzenethiol (BT) as a probe molecule and are confirmed via numerical simulations. We achieve a maximum SERS enhancement factor of up to ∼10 8 when the resonances are tailored to coincide with the excitation wavelength by suitable structural modifications.
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