Plasmonic Arrays Research Articles

High-Speed Plasmonic Electro-Optic Beam Deflectors.

Highly integrated active nanophotonics addressing both device footprint and operation speed demands is a key enabling technology for the next generation optical networks. Plasmonic systems have proven to be a serious contender to alleviate current performance limitations in electro-optic devices. Here, we demonstrate a plasmonic optical phased array (OPA) consisting of two 10 μm long plasmonic phase shifters, utilized to control the far-field radiation pattern of two subwavelength-separated emitters for aliasing-free beam steering with an angular range of ±5° and flat frequency response up to 18 GHz (with the potential bandwidth of 1.2 THz). Extreme optical and electrostatic field confinement with great spatial overlap results in high phase modulation efficiency (VπL = 0.24 Vcm). The demonstrated approach of using plasmonic lithium niobate technology for optical beam manipulation offers inertia-free, robust, ultracompact, and high-speed beam steering.

Tuning higher order electric field resonances in plasmonic hexagonal arrays by oxygen-plasma treatment

Experimental and simulation studies show that a hexagonal array of polystyrene particles on a gold substrate, capped with gold semi-shells, results in increased optical confinement of the resonance modes in comparison with those for arrays without metallic substrate or capping. Well-ordered arrays of polystyrene beads were fabricated by convective deposition, a solution-based self-assembly process. The polystyrene particles exhibited strong optical concentration, with photonic and plasmonic modes as detected in optical spectra and modelling. The resonance wavelengths of the plasmonic hexagonal array were modified by treating the hexagonal arrays with oxygen plasma at fixed power of 150 W for time periods of 0–10 min. The plasma treatment reduced the vertical height of the polystyrene particles, and the resonances were tuned and sharpened after plasma treatment. This increase is attributed to the improved uniformity of the gold semi-shell coating distributed over the polystyrene particles. Additionally, the plasma treatment increased the refractive index of the polystyrene particles due to cross-linking. Devices with these plasmonic hexagonal arrays enable enhanced light–matter interactions, with the flexibility to post-tune the resonance wavelengths.

Plasmon-enhanced fluorescence correlation spectroscopy for super-localized detection of nanoscale subcellular dynamics

In this report, we investigate plasmon-enhanced imaging fluorescence correlation spectroscopy (p-FCS). p-FCS takes advantage of extreme light confinement by localization at nanogap-based plasmonic nanodimer arrays (PNAs) for enhanced signal-to-noise ratio (SNR) and improved precision by registration with surface plasmon microscopy images. Theoretical results corroborate the enhancement by PNAs in the far-field. Near-field scanning optical microscopy was used to confirm near-field localization experimentally. Experimental confirmation was also conducted with fluorescent nanobeads. The concept was further applied to studying the diffusion dynamics of lysosomes in HEK293T cells stimulated by phorbol 12-myristate 13-acetate treatment. It was found that lysosomes demonstrate stronger super-diffusive behavior with relatively weaker sub-diffusion after stimulation. SNR measured of p-FCS was improved by 9.77 times over conventional FCS. This report is expected to serve as the foundation for an enhanced analytical tool to explore subcellular dynamics.

Double-Langmuir model for optimized nanohole array-based plasmonic biosensors

The sensing mechanism of plasmonic nanohole arrays is investigated and a novel model is proposed to interpret their optical response over a wide dynamic range of concentrations (10-13-10-5 M), based on a double-Langmuir model. This model describes the signal response of the analyte binding as the sum of two independent contributions which are related to two different surface regions of the biosensor, namely the top gold surface of the nanohole array and the lateral gold area inside the nanoholes. Numerical simulations highlight the different near-field behaviour of these two regions and their very different refractive index sensitivities, which both support the double-Langmuir model. This is corroborated by experimental biosensing measurements with gold nanohole arrays with hexagonal symmetry, synthesized by nanosphere lithography. Their sensing performances are optimized by numerical simulations by changing their geometrical parameters (i.e., lattice constant, nanohole diameter and height) in order to achieve a maximum sensitivity. For the biosensing experiments, the biotin-streptavidin complex is used as a benchmark test for the optimized nanohole array and a robust calibration is provided by the double-Langmuir model obtaining a limit of detection of 0.3 ng/mL, which corresponds to an absolute analyte quantity of 0.02 fmol.

Multipolar Lattice Resonances in Plasmonic Finite-Size Metasurfaces

Collective lattice resonances in regular arrays of plasmonic nanoparticles have attracted much attention due to a large number of applications in optics and photonics. Most of the research in this field is concentrated on the electric dipolar lattice resonances, leaving higher-order multipolar lattice resonances in plasmonic nanostructures relatively unexplored. Just a few works report exceptionally high-Q multipolar lattice resonances in plasmonic arrays, but only with infinite extent (i.e., perfectly periodic). In this work, we comprehensively study multipolar collective lattice resonances both in finite and in infinite arrays of Au and Al plasmonic nanoparticles using a rigorous theoretical treatment. It is shown that multipolar lattice resonances in the relatively large (up to 6400 nanoparticles) finite arrays exhibit broader full width at half maximum (FWHM) compared to similar resonances in the infinite arrays. We argue that our results are of particular importance for the practical implementation of multipolar lattice resonances in different photonics applications.

Dual polarized engineering the extinction cross-section of a dielectric wire using graphene-based oligomers

In this paper, graphene-coated spherical nanoparticles are arranged around an infinite length dielectric cylinder to enhance its extinction cross-section. Initially, a single longitudinal one-dimensional periodic array is considered in different loci concerning the transverse electric (TE) incident plane wave. It is observed that regardless of the position of the particles, the extinction cross-section of the dielectric cylinder is considerably enhanced with respect to the bare one. Later, by increasing the number of longitudinal plasmonic arrays around the cylinder, each residing in a different azimuthal direction, the extinction cross-section is further manipulated to observe double pronounced Fano resonances. The origin of the Fano resonances is described by considering their planar counterparts constructed by the periodic assembly of plasmonic oligomers. Finally, the hexamer configuration is considered as the prototype, and the effect of various optical, geometrical, and material parameters on the optical response is investigated in detail. Interestingly, due to the spherical symmetry of the cells, the extinction cross-section is also enhanced for the transverse magnetic (TM) incident wave, which is unattainable using a continuous plasmonic cover made of metal or graphene. The potential application of our proposed structure is in the design of reconfigurable conformal optical absorbers and sensors.

Plasmon-driven light harvesting in poly(vinyl alcohol) films for precise surface topography modulation.

Efficient light harvesting is essential for advanced photonic devices. Complex micro/nano surface relief structures can be produced via light-triggered mechanical movement, but limited in organic active molecular units. In this Letter, we propose to embed noble-metal particles into light-inactive polyvinyl alcohol matrix to construct a light harvesting system driven by plasmon for inscription of surface relief gratings. Ultra-small-sized silver nuclei are generated in the polymer by pre-thermal treatment, acting as an accelerator for the subsequent photoinduced particle growth, hydrogen group cleavage, and matrix softening. Based on such properties, a complex plasmonic array carrying ultra-high-density information is achieved with peristrophic multiplexing holography. This Letter paves a bright way to realize data storage, information encryption, and optical microcavity.

Mid-infrared radiative emission from bright hot plasmons in graphene.

Carrier excitation and decay processes in graphene are of broad interest since relaxation pathways that are not present in conventional materials are enabled by a gapless Dirac electronic band structure. Here, we report that a previously unobserved decay pathway-hot plasmon emission-results in Fermi-level-dependent mid-infrared emission in graphene. Our observations of non-thermal contributions to Fermi-level-dependent radiation are an experimental demonstration of hot plasmon emission arising from a photo-inverted carrier distribution in graphene achieved via ultrafast optical excitation. Our calculations indicate that the reported plasmon emission process can be several orders of magnitude brighter than Planckian emission mechanisms in the mid-infrared spectral range. Both the use of gold nanodisks to promote scattering and localized plasmon excitation and polarization-dependent excitation measurements provide further evidence for bright hot plasmon emission. These findings define an approach for future work on ultrafast and ultrabright graphene emission processes and mid-infrared light source applications.

Understanding radiative transitions and relaxation pathways in plexcitons

Summary Molecular aggregates on plasmonic nanoparticles have emerged as attractive systems for the studies of polaritonic light-matter states, called plexcitons. Such systems are tunable, scalable, easy to synthesize, and offer sub-wavelength confinement, all while giving access to the ultrastrong light-matter coupling regime, promising a plethora of applications. However, the complexity of these materials prevented the understanding of their excitation and relaxation phenomena. Here, we follow the relaxation pathways in plexcitons and conclude that while the metal destroys the optical coherence, the molecular aggregate coupled to surface processes significantly contributes to the energy dissipation. We use two-dimensional electronic spectroscopy with theoretical modeling to assign the different relaxation processes to either molecules or metal nanoparticle. We show that the dynamics beyond a few femtoseconds has to be considered in the language of hot electron distributions instead of the accepted lower and upper polariton branches and establish the framework for further understanding.

Rapid and sensitive multiplex molecular diagnosis of respiratory pathogens using plasmonic isothermal RPA array chip

The current clinically available multiplex molecular diagnostic technologies are difficult to apply to onsite diagnostic platforms due to their large and sophisticated instrumentation, long amplification times and limited number of simultaneous detections. We developed a plasmonic isothermal recombinase polymerase amplification (RPA) array chip for rapid and sensitive multiplex molecular detection. The 3D plasmonic substrate composed of Au nanoparticles (NPs) on dense Au nanopillars (NPOP) showed highly enhanced plasmon-enhanced fluorescence (PEF) of RPA products with long DNA amplicons (~200 bp). The plasmonic 4-plex RPA array chip successfully detected bacterial DNA within 30 min and viral RNA within 40 min; the sensitivity of the plasmonic RPA array chip was comparable to or 10-fold higher than that of the 4-pelx liquid-phase RPA and 4-plex liquid-phase PCR techniques. Additionally, no cross-reactivity was observed. The 4-plex plasmonic RPA array chip was preliminary evaluated using clinical respiratory viral-positive nasopharyngeal swab samples. This approach enables rapid, sensitive and high-multiplex molecular detection and can be used in the realization of a simplified and miniaturized platform for onsite multiplex molecular diagnostics.

Dissipation engineered directional filter for quantum ratchets

We demonstrate transport rectification in a hermitian Hamiltonian quantum ratchet by a dissipative, dynamic impurity. While the bulk of the ratchet supports transport in both directions, the properly designed loss function of the local impurity acts as a direction-dependent filter for the moving states. We analyse this scheme theoretically by making use of Floquet-S-Matrix theory. In addition, we provide the direct experimental observation of one-way transmittance in periodically modulated plasmonic waveguide arrays containing a local impurity with engineered losses.

Tuning the Thermoresponsive Behavior of Surface-Attached PNIPAM Networks: Varying the Crosslinker Content in SI-ATRP.

The synthesis and thermoresponsive properties of surface-attached poly(N-isopropylacrylamide)-co-N,N′-methylene bisacrylamide (PNIPAM-co-MBAM) networks are investigated. The networks are formed via SI-ARGET-ATRP (“grafting-from”) on thiol-based initiator-functionalized gold films. This method is reliable, well controlled, fast, and applicable to patterned surfaces (e.g., nanopores) for networks with dry thicknesses >20 nm. Surface-attached PNIPAM-co-MBAM gels are swollen below their volume phase transition temperature but above collapse without complete expulsion of water (retain ∼50 vol %). The swelling/collapse transition is studied using complementary SPR and QCMD techniques. The ratio between swollen and collapsed heights characterizes the thermoresponsive behavior and is shown to not depend on network height but to vary with MBAM content. The higher the proportion of the crosslinker, the lower the magnitude of the phase transition, until all responsiveness is lost at 5 mol % MBAM. The temperature range of the transition is broadened for more crosslinked PNIPAM-co-MBAM gels but remains centered around 32 °C. Upon reswelling, less crosslinked networks display sharp transitions, while for those containing ≥3 mol % MBAM, transitions remain broad. This tunable behavior persists for gels on nanostructured gold surfaces. Investigating PNIPAM-co-MBAM networks on gold plasmonic nanowell arrays is a starting point for expanding their scope as thermo-controlled nanoactuators.

Plasmon-Enhanced Sunlight Harvesting in Thin-Film Solar Cell by Randomly Distributed Nanoparticle Array.

In this paper, a randomly distributed plasmonic aluminum nanoparticle array is introduced on the top surface of conventional GaAs thin-film solar cells to improve sunlight harvesting. The performance of such photovoltaic structures is determined through monitoring the modification of its absorbance due to changing its structural parameters. A single Al nanoparticle array is integrated over the antireflective layer to boost the absorption spectra in both visible and near-infra-red regimes. Furthermore, the planar density of the plasmonic layer is presented as a crucial parameter in studying and investigating the performance of the solar cells. Then, we have introduced a double Al nanoparticle array as an imperfection from the regular uniform single array as it has different size particles and various spatial distributions. The comparison of performances was established using the enhancement percentage in the absorption. The findings illustrate that the structural parameters of the reported solar cell, especially the planar density of the plasmonic layer, have significant impacts on tuning solar energy harvesting. Additionally, increasing the plasmonic planar density enhances the absorption in the visible region. On the other hand, the absorption in the near-infrared regime becomes worse, and vice versa.

Tuning Gold Nanoparticle Size with Fixed Interparticle Spacing in Large-Scale Arrays: Implications for Plasmonics and Nanoparticle Etching Masks

Gold nanoparticles play an important role in plasmonic arrays, including, but not limited to, photovoltaic, biomedical, sensing, optical, and catalytic applications. For plasmonic arrays, control o...

Analyte Co-localization at Electromagnetic Gap Hot-Spots for Highly Sensitive (Bio)molecular Detection by Plasmon Enhanced Spectroscopies.

Electromagnetic hot-spots at ultranarrow plasmonic nanogaps carry immense potential to drive detection limits down to few molecules in sensors based on surface-enhanced Raman or fluorescence spectroscopies. However, leveraging the EM hot-spots requires access to the gaps, which in turn depends on the size of the analyte in relation to gap distances. Herein, we leverage a well-calibrated process based on self-assembly of block copolymer colloids on a full-wafer level to produce high-density plasmonic nanopillar arrays exhibiting a large number (>1010 cm-2) of uniform interpillar EM hot-spots. The approach allows convenient handles to systematically vary the interpillar gap distances down to a sub-10 nm regime. The results show compelling trends of the impact of analyte dimensions in relation to the gap distances toward their leverage over interpillar hot-spots and the resulting sensitivity in SERS-based molecular assays. Comparing the detection of labeled proteins in surface-enhanced Raman and metal-enhanced fluorescence configurations further reveal the relative advantage of fluorescence over Raman detection while encountering the spatial limitations imposed by the gaps. Quantitative assays with limits of detection down to picomolar concentrations are realized for both small organic molecules and proteins. The well-defined geometries delivered by a nanofabrication approach are critical to arriving at realistic geometric models to establish meaningful correlation between the structure, optical properties, and sensitivity of nanopillar arrays in plasmonic assays. The findings emphasize the need for the rational design of EM hot-spots that takes into account the analyte dimensions to drive ultrahigh sensitivity in plasmon-enhanced spectroscopies.

Structure-adjustable colloidal silver nanoparticles on polymers grafted cellulose paper-based highly sensitive and selective SERS sensing platform with analyte enrichment function

• AgNSs with various dimeters were fabricated by adjusting the amount of reducing agents (NaBH 4 ). • AgNSs grafted PMMA-treated paper platform were easily prepared by a one-step synthesis. • SERS ultradetection of platform was obtained 10 –10 M with an EF of 1.2 × 10 8 . • An excellent reproducibility of Raman signal with RSD of 10.39% was obtained. • An outstanding selectivity each probe molecule in an analyte mixture solution of R6G and CV at 10 −8 M was achieved. The synthesis procedures and processes for evaluating the SERS performance of AgNSs grafted PMMA treated paper platform. Paper-based sensing platforms have become one of the hot topics in spectroscopic technique for chemical and biological detections. However, it has been still challenging to detect molecules at trace levels owing to its intrinsic interconnected porous structures related to the fibril structure of paper and hydrophilic characteristic. Herein, a cellulose paper combined molecular polymers and hybridized chain reaction that led to hydrophobic functionalization with static water contact angles>90° for surface-enhanced Raman scattering (SERS) was proposed. During the fabrication, the formation of the ultrasensitive SERS is supported by interconnection of silver nanoparticles (NPs) of varying diameters from 20 to 50 nm and concentration in the range of 2–6 mL on one side of the paper substrate to achieve excellent quantification capability based on hotspots engineering-based clusters and analyte enrichment system, particularly, AgNPs with diameter of 30 nm exhibit the highest Raman signals at 532 nm excitation. The resulting plasmonic arrays show SERS detection of CV molecules at a low concentration of 10 –10 M with an enhancement factor of 1.2 × 10 8 and excellent reproducibility with RSD of Raman signal as low as 10.39%. An outstanding selectivity each probe molecule in an analyte mixture solution of R6G and CV at diluted concentration (10 −8 M) of the platform was obtained. These outcomes could be designated to the more target molecules trapped in the hotspots and cluster of AgNPs after activated molecular enrichment mechanism underlying hydrophobic layer correlated with natural evaporation.

Room-Temperature Coupling of Single Photon Emitting Quantum Dots to Localized and Delocalized Modes in a Plasmonic Nanocavity Array

Single photon sources, especially those based on solid state quantum emitters, are key elements in future quantum technologies. What is required is the development of broadband, high quantum efficiency, room temperature, single photon sources, which can also be tunably coupled to optical cavities, which could lead to the development of all-optical quantum communication platforms. In this regard, the deterministic coupling of single photon sources to plasmonic nanocavity arrays has a great advantage due to a long propagation length and delocalized nature of surface lattice resonances. Guided by these considerations, we report experiments on the room temperature tunable coupling of single photon emitting colloidal quantum dots (CQDs) to localized surface plasmon and surface lattice resonance modes in plasmonic nanocavity arrays. Using a time-resolved photoluminescence measurement on isolated CQD, we report the significant advantage of surface lattice resonances in realizing a much higher Purcell effect, despite the large dephasing of CQDs, with values of ∼22 and ∼6 for coupling to the lattice and localized modes, respectively. We present measurements on the antibunching of CQDs coupled to these modes with g(2)(0) values in the quantum domain, providing evidence for effective cooperative behavior. We present a density matrix treatment of the coupling of CQDs to plasmonic and lattice modes enabling us to model the experimental results on Purcell factors as well as on the antibunching. We also provide experimental evidence of indirect excitation of remote CQDs mediated by the lattice modes and propose a model to explain these observations. Our study demonstrates the possibility of developing nanophotonic platforms for single photon operations and communications with broadband quantum emitters and plasmonic nanocavity arrays since these arrays can generate entanglement between spatially separated quantum emitters.

Light emitting polymers in two dimensional plasmonic multi wavelength random laser

Red, Green and Blue Multi wavelength lasing is desired in two dimensional flexible plasmonic multi-layer structure based on light emitting polymers and gold nanostructure. For this purpose, gold nano-structure is covered by three different light emitting polymers with poly-vinyl-pyrolydone as spacer layers. To achieve multi-wavelengths random laser, these six layers are coated over the poly-dimethyl siloxane substrate by main surface roughness and the sample is pumped by nanosecond green laser. The lasing due to band-edge lattice plasmons in arrays of plasmonic nano rods in a homogeneous environment is collected by spectrometer. Our results show emission peaks for every wavelength region with the minimum value of threshold lasing and the maximum of emission intensity.

Enhancing Vibrational Light-Matter Coupling Strength beyond the Molecular Concentration Limit Using Plasmonic Arrays.

Vibrational strong coupling is emerging as a promising tool to modify molecular properties by making use of hybrid light–matter states known as polaritons. Fabry–Perot cavities filled with organic molecules are typically used, and the molecular concentration limits the maximum reachable coupling strength. Developing methods to increase the coupling strength beyond the molecular concentration limit are highly desirable. In this Letter, we investigate the effect of adding a gold nanorod array into a cavity containing pure organic molecules using FT-IR microscopy and numerical modeling. Incorporation of the plasmonic nanorod array that acts as artificial molecules leads to an order of magnitude increase in the total coupling strength for the cavity with matching resonant frequency filled with organic molecules. Additionally, we observe a significant narrowing of the plasmon line width inside the cavity. We anticipate that these results will be a step forward in exploring vibropolaritonic chemistry and may be used in plasmon based biosensors.

Investigations of Shape, Material and Excitation Wavelength Effects on Field Enhancement in SERS Advanced Tips.

This article, a part of the larger research project of Surface-Enhanced Raman Scattering (SERS), describes an advanced study focusing on the shapes and materials of Tip-Enhanced Raman Scattering (TERS) designated to serve as part of a novel imager device. The initial aim was to define the optimal shape of the “probe”: tip or cavity, round or sharp. The investigations focused on the effect of shape (hemi-sphere, hemispheroid, ellipsoidal cavity, ellipsoidal rod, nano-cone), and the effect of material (Ag, Au, Al) on enhancement, as well as the effect of excitation wavelengths on the electric field. Complementary results were collected: numerical simulations consolidated with analytical models, based on solid assumptions. Preliminary experimental results of fabrication and structural characterization are also presented. Thorough analyses were performed around critical parameters, such as the plasmonic metal—Silver, Aluminium or Gold—using Rakic model, the tip geometry—sphere, spheroid, ellipsoid, nano-cone, nano-shell, rod, cavity—and the geometry of the plasmonic array: cross-talk in multiple nanostructures. These combined outcomes result in an optimized TERS design for a large number of applications.