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Structural colors of high performance and economically feasible fabrication are desired in various applications. Herein, we demonstrate that reflective full-color filters based on the interference effect can be realized in periodic Fabry-Perot (F-P) nanocavity arrays of the same thickness. Enabled by simply adjusting the nanocavity size and array period, the resonant wavelengths can be successively tuned in the whole visible light range, which is mainly attributed to the varied effective refractive index introduced by the different filling density of the F-P nanocavity. Compared to the plasmonic colors utilizing the similar nanostructures, the proposed interference colors offer unique advantages of higher color contrast, wider gamut, and lower fabrication requirements. Besides, these color filters do not involve modulating the vertical dimensions of the F-P nanocavities, which is conducive to the monolithic integration of multicolor optical cavities and their large-area applications in consumable products combined with replica patterning techniques, such as nanoimprinting and soft lithography.
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Sub-wavelength aperture arrays featuring small gaps have an extraordinary significance in enhancing the interactions of terahertz (THz) waves with matters. But it is difficult to obtain large light-substance interaction enhancement and high optical response signal detection capabilities at the same time. Here, we propose a simple terahertz bow-tie aperture arrays structure with a large electric field enhancement factor and high transmittance at the same time. The field enhancement factor can reach a high value of 1.9×104 and the transmission coefficient of around 0.8 (the corresponding normalized-to-area transmittance is about 14.3) at 0.04 µm feature gap simultaneously. The systematic simulation results show that the designed structure can enhance the intensity of electromagnetic hotspot by continuously reducing the feature gap size without affecting the intensity of the transmittance. We also visually displayed the significant advantages of extremely strong electromagnetic hot spots in local terahertz refractive index detection, which provides a potential platform and simple strategy for enhanced THz spectral detection.
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Plasmonic artificial molecules are promising platforms for linear and nonlinear optical modulation at various regimes including the visible, infrared and terahertz bands. Fano resonances in plasmonic artificial structures are widely used for controlling spectral lineshapes and tailoring of near-field and far-field optical response. Generation of a strong Fano resonance usually relies on strong plasmon coupling in densely packed plasmonic structures. Challenges in reproducible fabrication using conventional lithography significantly hinders the exploration of novel plasmonic nanostructures for strong Fano resonance. In this work, we propose a new class of plasmonic molecules with symmetric structure for Fano resonances, named evenly divided disk, which shows a strong Fano resonance due to the interference between a subradiant anti-bonding mode and a superradiant bonding mode. We successfully fabricated evenly divided disk structures with high reproducibility and with sub-20 nm gaps, using our recently developed sketch and peel lithography technique. The experimental spectra agree well with the calculated response, indicating the robustness of the Fano resonance for the evenly divided disk geometry. Control experiments reveal that the strength of the Fano resonance gradually increases when increasing the number of split parts on the disk from three to eight individual segments. The Fano-resonant plasmonic molecules that can also be reliably defined by our unique fabrication approach open up new avenues for application and provide insight into the design of artificial molecules for controlling light-matter interactions.
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Enhanced near-field and quality factor of resonance are key issues in plasmonic structures. Here, we demonstrate a kind of notched bowtie metamaterials in the terahertz (THz) regime with narrow linewidth and extremely enhanced near field. The notched bowtie is a variation of common bowtie structure created by introducing symmetric notches on the two sides of the triangular metallic structure. Benefiting from the introduction of notches, the modulation depth of transmittance spectra and near-field enhancement of the notched bowtie arrays were strongly enhanced due to the increase of the structure-derived equivalent inductance. The results demonstrated that near-field enhancement can be increased to above 4000. In addition, the designed structure possesses a narrowed resonance linewidth, and thus an improved quality factor, which could be a promising platform for THz sensing and other potential applications of THz metamaterials.
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We demonstrate a configuration to generate transmissive structural colors through triangular-lattice square nanohole arrays in aluminum (Al) film with Al nanodisks on the bottom of the nanoholes. By using a simple nanofabrication process, colors covering the entire visible light with different brightness and saturation are achieved by tuning both the period of arrays and the size of nanoholes. The optical behaviors of the structures are systematically investigated by both experimental and theoretical methods. The results indicate that the localized surface plasmon resonance of nanohole arrays plays the key role in the extraordinary transmission and meanwhile the coupling of disks and holes is also of importance for the enhanced transmission. With the wide color gamut, these kinds of vertically coupled Al nanohole/nanodisk arrays show the capabilities for high-resolution full-color printing. Compared to existing transmissive plasmonic color filters, the configuration in this work has the advantages of a simple fabrication process and using cheap aluminum materials.
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We demonstrated a tunable structural color filter based on an asymmetric Fabry-Perot cavity employing germanium antimony tellurium alloy Ge2Sb2Te5 (GST) as a switchable ultrathin lossy layer. The color tunability and switch mechanism of our designed structure were investigated by both simulation and analytical approaches. Both numerical simulations and analytical results show that the tunable reflective colors can be generated through the reversible phase transition of GST from amorphous to crystalline. Additionally, the generated colors possess high brightness, high saturation, and a wide gamut. Our designed structure will inspire phase-transition-based systems' potential applications in colorimetric sensing, smart windows, full-color printing and displays, anti-counterfeiting, and data encryption.
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Plasmonic nanostructures with strong Fano resonance are of fundamental interest. Here, our systematic simulations show that rational positioning of a silver plasmonic heptamer above a highly reflective substrate mirror can significantly enhance its intrinsic Fano-resonance intensity. The silver nanodisk heptamer positioned at an appropriate distance above the reflective substrate enables 2.4 times field enhancement and 3.6 times deeper Fano-dip respectively compared to the heptamer directly placed on silicon oxide substrate. Besides, our results indicate that the Fano-dip position does not shift when the silver nanodisk heptamer gradually shifts away from the reflective substrate mirror (≥60 nm).
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Broad-band and high-efficiency polarization converter is an imperative component in communication systems, but its functionality often clashes with the constraint of materials. Herein we theoretically and numerically demonstrate that a broad-band and high-efficiency 90° polarization rotator around 1550 nm can be realized using an ultrathin and geometry-optimized composite structure. Based on simulation results, the reflection efficiency and operation bandwidth is up to ≈80% and ≈300 nm, respectively, for the 90° polarization rotator. With similar concept, we also demonstrate a quarter-wave plate with an efficiency of 94% and bandwidth of 110 nm. The electric filed distribution indicates that the conversion behaviors are caused by the strong magnetic coupling in the designed composite structure. Furthermore, the polarization ellipticity properties are investigated to further understand the broad-band effect of the proposed polarization convertors.
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Seeking for the best possible substrates for surface-enhanced Raman spectroscopy (SERS) is of great interest for single-molecule-level detection applications. Lithographic plasmonic nanostructures are supposed to enable uniform enhancement and thus have attracted extensive interest in the past decade. In this work, we propose and demonstrate a lithographic three-dimensional (3D) donut-like gold nanoring array as a SERS substrate with an enhancement factor (EF) up to 3.84 × 107. This 3D nanoring array could be directly fabricated using electron-beam-lithography-defined templates without any additional lift-off process and thus promises ultraclean metallic surfaces. Meanwhile, the 3D configuration allows multiple hot spots for improving SERS performance compared to planar counterparts with comparable plasmon resonance position. Systematic experiments and simulations were conducted to gain understanding of the origin of the improved SERS performance. The results imply that the 3D donut-like gold nanorings with multiple hot spots can serve as a promising configuration for SERS applications.
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Understanding the mechanistic information on many kinetic processes requires the exploration of dynamic rotational information on the target object at the single particle (or molecule) level. In this work, we developed a new strategy, total internal reflection scattering (TIRS) microscopy, to determine the full three-dimensional (3D) angular information on a single gold nanorod (GNR) close to the liquid/solid interface. It was found that the 3D orientational information on individual GNR could be readily elucidated by using p-polarized TIRS illumination through deciphering the orientation-coded intensity distribution pattern in a single TIRS image. In comparison with the previously reported strategies, this method does not require complicated focal plane correction, affording a versatile pathway to track the rotational dynamics close to the interface in a high throughput manner. The methodology presented here, therefore, demonstrates a promising approach that can be applied to fluidic membranes, including membranes with polymers, bound proteins, and so on.
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Gaps with single-nanometer dimensions (<10 nm) between metallic nanostructures enable giant local field enhancements for surface enhanced Raman scattering (SERS). Monolayer graphene is an ideal candidate to obtain a sub-nanometer gap between plasmonic nanostructures. In this work, we demonstrate a simple method to achieve a sub-nanometer gap by dewetting a gold film supported on monolayer graphene grown on copper foil. The Cu foil can serve as a low-loss plasmonically active metallic film that supports the imaginary charge oscillations, while the graphene can not only create a stable sub-nanometer gap for massive plasmonic field enhancements but also serve as a chemical enhancer. We obtained higher SERS enhancements in this graphene-gapped configuration compared to those in Au nanoparticles on Cu film or on graphene-SiO2-Si. Also, the Raman signals measured maintained their fine features and intensities over a long time period, indicating the stability of this Au-graphene-Cu hybrid configuration as an SERS substrate.
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Single-crystal silicon nanostructures have attracted much attention in recent years due in part to their unique optical properties. In this work, we demonstrate direct fabrication of single-crystal silicon nanotubes with sub-10 nm walls which show low reflectivity. The fabrication was based on a cryogenic inductively coupled plasma reactive ion etching process using high-resolution hydrogen silsesquioxane nanostructures as the hard mask. Two main etching parameters including substrate low-frequency power and SF6/O2 flow rate ratio were investigated to determine the etching mechanism in the process. With optimized etching parameters, high-aspect-ratio silicon nanotubes with smooth and vertical sub-10 nm walls were fabricated. Compared to commonly-used antireflection silicon nanopillars with the same feature size, the densely packed silicon nanotubes possessed a lower reflectivity, implying possible potential applications of silicon nanotubes in photovoltaics.
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Pesticide residues threaten the ecological environment and human health. Therefore, developing high performance SERS substrate to achieve highly sensitive detection of pesticide residues is meaningful. In this study, based on the strategy of combining "hot spots" engineering and material hybridization, we construct a novel hybrid SERS substrate by depositing Ag nanoflowers (NFs) on ZnO nanorods (NRs). Benefiting from the synergistic effect of electromagnetic enhancement and charge transfer effect, the Ag NFs@ZnO NRs substrate exhibits a low detection limit (10-13 M) for crystal violet molecules. This SERS substrate has good uniformity with a relative standard deviation of 7.463 %. Besides, owning to the photocatalytic property of ZnO NRs, the hybrid substrate can degrade probe molecules after SERS detection and realize recyclability. As a demonstration, we employed our SERS substrate for the trace detection of pesticide residues on apple surface and in river water. This study provides a new idea for improving the SERS performance of hybrid substrates.
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A plasmonic refractive index sensor based on surface plasmon polaritons (SPPs) that consist of metal-insulator-metal (MIM) waveguides and a whistle-shaped cavity is proposed. The transmission properties were simulated numerically by using the finite element method. The Fano resonance phenomenon can be observed in their transmission spectra, which is due to the coupling of SPPs between the transmission along the clockwise and anticlockwise directions. The refractive index-sensing properties based on the Fano resonance were investigated by changing the refractive index of the insulator of the MIM waveguide. Modulation of the structural parameters on the Fano resonance and the optics transmission properties of the coupled structure of two MIM waveguides with a whistle-shaped cavity were designed and evaluated. The results of this study will help in the design of new photonic devices and micro-sensors with high sensitivity, and can serve as a guide for future application of this structure.
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Surface plasmons in metals promise many fascinating properties and applications in optics, sensing, photonics and nonlinear fields. Plasmonic nanostructures with extremely small features especially demonstrate amazing new effects as the feature sizes scale down to the sub-nanometer scale, such as quantum size effects, quantum tunneling, spill-out of electrons and nonlocal states etc. The unusual physical, optical and photo-electronic properties observed in metallic structures with extreme feature sizes enable their unique applications in electromagnetic field focusing, spectra enhancing, imaging, quantum photonics, etc. In this review, we focus on the new effects, fabrication and applications of plasmonic metal nanostructures with extremely small features. For simplicity and consistency, we will focus our topic on the plasmonic metal nanostructures with feature sizes of sub-nanometers. Subsequently, we discussed four main and typical plasmonic metal nanostructures with extremely small features, including: (1) ultra-sharp plasmonic metal nanotips; (2) ultra-thin plasmonic metal films; (3) ultra-small plasmonic metal particles and (4) ultra-small plasmonic metal nanogaps. Additionally, the corresponding fascinating new effects (quantum nonlinear, non-locality, quantum size effect and quantum tunneling), applications (spectral enhancement, high-order harmonic wave generation, sensing and terahertz wave detection) and reliable fabrication methods will also be discussed. We end the discussion with a brief summary and outlook of the main challenges and possible breakthroughs in the field. We hope our discussion can inspire the broader design, fabrication and application of plasmonic metal nanostructures with extremely small feature sizes in the future.
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We report a strong one-photon photoluminescence (PL) behavior of a silver nanowire directly coupled gold film. The PL peak position of the silver nanowire-coupled gold film deviates from the intrinsic interband transition of gold materials and is not sensitive to the diameter change of the silver nanowire. We attribute this strong PL behavior to the intraband transition of hot electrons dominated by high-order gap plasmons, which are excited in the ultra-small gap formed by an ultra-thin polyvinyl pyrrolidone (PVP) layer coated on the silver nanowire. The results show that the energy required for the strong PL of the heterogeneous system mainly comes from the gold film, acting as an incident energy absorber enhanced by the high-order gap plasmons, while the silver nanowire acts an efficient incident energy focusing antenna. In situ Raman scattering spectra and time-resolved PL intensity integral curves were used to record the carbonization and disappearance process of PVP. The understanding of the PL behavior of the silver nanowire directly coupled gold film proves the universality of plasmon-modulated PL theory and is also of great significance to improve the generation and utilization efficiency of hot electrons with high-order gap plasmons in the fields of catalysis and incident energy capture.
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Fano resonance can be achieved by the destructive interference between a superradiant bright mode and a subradiant dark mode. A variety of artificial plasmonic oligomers have been fabricated to generate Fano resonance for its extensive applications. However, the Fano resonance in plasmonic oligomer systems comes from the interaction of all metal particles, which greatly limits the tunability of the Fano resonance. Besides, only a single Fano resonance is supported by many existing plasmonic oligomers, while multiple Fano resonances mostly occur in complex and multilayer structures, whose fabrication is greatly challenging. Here, a simple asymmetric plasmonic molecule consisting of a central metal disk and two side-coupled parallel metal rods is demonstrated. The simulation and experimental results clearly show that double Fano resonances appear in the transmission spectrum. In addition, the two Fano peaks can be independently tuned and single/double Fano peak switching can be achieved by changing one rod length or the gap distances between the rods and the disk. The modulation method is simple and effective, which greatly increases the tunability of the structure. The proposed asymmetric artificial plasmonic molecule can have applications in multi-channel optical switches, filters and biosensors. Moreover, the controllable plasmonic field intensity in the gap between the disk and rods also provides a new control means for plasmon-induced photocatalytic reactions and biosynthesis.
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Seeking for ultrasensitive and low-cost substrates is highly demandable for practical applications of surface-enhanced Raman scattering (SERS) technology. In this work, we report an ultrasensitive SERS-active substrate based on wet-chemistry-synthesized vertically aligned large-area TiO2 nanosheets (NSs) decorated by densely packed gold nanoparticles (Au NPs) with sub-5 nm gaps. Via a multistep successive deposition process, three-dimensional-stacked Au NPs sandwiched by a 3 nm SiO2 layer were assembled onto the TiO2 NS, enabling numerous hotspots due to the formation of both ultratiny plasmonic gaps and semiconductor/metal interfaces. Experimental results show that the fabricated substrate displays a detection limit down to 10 fM (10-14 M) without involving any condensation process by using the crystal violet as probe molecules. Control experiments and electromagnetic simulations indicate that the nanogaps defined by the 3 nm spacer are essential for the obtained excellent SERS performance. With its ultrasensitive detection capability, we demonstrate that the fabricated SERS substrate can be used for the trace analysis of melamine in milk.
Asunto(s)
Análisis de los Alimentos/métodos , Oro/química , Nanopartículas del Metal/química , Leche/química , Triazinas/análisis , Animales , Dióxido de Silicio/químicaRESUMEN
For cancer diagnosis, technologies must be capable of molecular recognition, and they must possess a built-in pattern recognition component for efficient imaging and discrimination of targeted cancer cells. Surface enhanced Raman scattering (SERS) tags based on plasmonically active nanoparticles hold promise for accurate and efficient cancer cell recognition, owing to ultra-narrow peak and sensitive optical properties. However, a complex fingerprint spectrum increases data analysis difficulty, making it necessary to develop multicolor SERS tags with a simple fingerprint spectrum. To address this, we herein fabricated SERS-encoded nanoparticles (NPs) with stable and simple fingerprint spectrum through synthesis of isotopic cellular Raman-silent graphene-isolated-Au-nanocrystals (GIANs) and conjugation with phospholipid-polyethylene glycol-linked aptamers to target proteins overexpressed on the cancer cell surface. GIANs, which possess the properties of graphitic nanomaterials, such as super-stable optical properties and high Raman cross-section, showed enhanced SERS signals. The 2D-band Raman shift of GIAN, which located in the cellular Raman-silent region, was easily regulated through fabrication of isotopic GIANs without changing their molecular structure. Such GIAN tags demonstrated multiplexed Raman imaging capability, both in vivo and in vitro, with low background interference. Moreover, cell membrane protein (nucleolin, mucin and epithelial cell adhesion molecule)-specific, aptamer-conjugated isotopic GIANs were fabricated and feasibly applied to built-in coding for rapid imaging and pattern recognition of targeted cancer cells. Such isotopic GIAN-aptamer-encoders show high potential for efficient cancer cell identification and diagnosis.
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Highly sensitive and low-cost surface-enhanced Raman scattering (SERS) substrates are essential for practical applications of SERS. In this work, we report an extremely simple but effective approach to achieve sensitive SERS detection of molecules (down to 10-10 M) by using a particle/molecule/film sandwich configuration. Compared to conventional SERS substrates which are preprepared to absorb analyte molecules for detection, the proposed sandwich configuration is achieved by postassembling a flexible transparent gel tape embedded with plasmonic nanoparticles onto an Au film decorated with to-be-detected analyte molecules. In such a configuration, the individual plasmonic gel tape and Au film have low or no SERS activity but the final assembled sandwich structure shows strong SERS signal due to the formation of numerous hot spots at the particle-film interface, where the analyte molecules themselves serve as both spacer and signal probes. Because of its simple configuration, we demonstrate that the proposed SERS substrate can be obtained over a large area with extremely low cost. Particularly, because of the on-demand nature and the flexibility, such a postassembly strategy provides an ideal solution to detect the pesticide residue on fruit surfaces with significantly enhanced sensitivity.