Direct detection of photoinduced magnetic force at the nanoscale reveals magnetic nearfield of structured light.

We demonstrate experimentally the detection of magnetic force at optical frequencies, defined as the dipolar Lorentz force exerted on a photoinduced magnetic dipole excited by the magnetic component of light. Historically, this magnetic force has been considered elusive since, at optical frequencies, magnetic effects are usually overshadowed by the interaction of the electric component of light, making it difficult to recognize the direct magnetic force from the dominant electric forces. To overcome this challenge, we develop a photoinduced magnetic force characterization method that exploits a magnetic nanoprobe under structured light illumination. This approach enables the direct detection of the magnetic force, revealing the magnetic nearfield distribution at the nanoscale, while maximally suppressing its electric counterpart. The proposed method opens up new avenues for nanoscopy based on optical magnetic contrast, offering a research tool for all-optical spin control and optomagnetic manipulation of matter at the nanoscale.

Asymmetric surface wave excitation through metasurface-edge diffraction.

The selective excitation of localized surface wave modes remains a challenge in the design of both leaky-wave and bound-wave devices. In this Letter, we show how the truncation of a metasurface can play an important role in breaking the spatial inversion symmetry in the excitation of surface waves supported by the structure. This is done by combining a large anisotropy in the dispersion relation and the presence of an edge that also serves as a coupling mechanism between the plane wave excitation and the induced surface waves. By resorting to the exact solution to the scattering problem based on a discrete Wiener-Hopf technique, we show that by inverting the component of the impinging wavevector parallel to the truncation, two distinct surface waves are excited.

Optical magnetic field enhancement at nanoscale: a nanoantenna comparative study.

We show and compare various metallic and dielectric nanostructures for local magnetic field enhancement at optical frequency. We elaborate on the origin of the magnetic field enhancement in each structure and define figures of merit to compare the ability of the structures to enhance the magnetic field. We show that dielectric structures can be a good alternative to their plasmonic counterpart due to their low loss. The magnetic field enhancement of these structures can be utilized in studying magnetic dipole transitions, magnetic imaging, chirality, and enhanced spectroscopy applications.

Exclusive Magnetic Excitation Enabled by Structured Light Illumination in a Nanoscale Mie Resonator.

Recent work has shown that optical magnetism, generally considered a challenging light-matter interaction, can be significant at the nanoscale. In particular, the dielectric nanostructures that support magnetic Mie resonances are low-loss and versatile optical magnetic elements that can effectively manipulate the magnetic field of light. However, the narrow magnetic resonance band of dielectric Mie resonators is often overshadowed by the electric response, which prohibits the use of such nanoresonators as efficient magnetic nanoantennas. Here, we design and fabricate a silicon (Si) truncated cone magnetic Mie resonator at visible frequencies and excite the magnetic mode exclusively by a tightly focused azimuthally polarized beam. We use photoinduced force microscopy to experimentally characterize the local electric near-field distribution in the immediate vicinity of the Si truncated cone at the nanoscale and then create an analytical model of such structure that exhibits a matching electric field distribution. We use this model to interpret the PiFM measurement that visualizes the electric near-field profile of the Si truncated cone with a superior signal-to-noise ratio and infer the magnetic response of the Si truncated cone at the beam singularity. Finally, we perform a multipole analysis to quantitatively present the dominance of the magnetic dipole moment contribution compared to other multipole contributions into the total scattered power of the proposed structure. This work demonstrates the excellent efficiency and simplicity of our method of using Si truncated cone structure under APB illumination compared to other approaches to achieve dominant magnetic excitations.

Longitudinal Monitoring of Biofilm Formation via Robust Surface-Enhanced Raman Scattering Quantification of Pseudomonas aeruginosa-Produced Metabolites.

Detection of bacterial metabolites at low concentrations in fluids with complex background allows for applications ranging from detecting biomarkers of respiratory infections to identifying contaminated medical instruments. Surface-enhanced Raman scattering (SERS) spectroscopy, when utilizing plasmonic nanogaps, has the relatively unique capacity to reach trace molecular detection limits in a label-free format, yet large-area device fabrication incorporating nanogaps with this level of performance has proven difficult. Here, we demonstrate the advantages of using chemical assembly to fabricate SERS surfaces with controlled nanometer gap spacings between plasmonic nanospheres. Control of nanogap spacings via the length of the chemical crosslinker provides uniform SERS signals, exhibiting detection of pyocyanin, a secondary metabolite of Pseudomonas aeruginosa, in aqueous media at concentration of 100 pg·mL-1. When using machine learning algorithms to analyze the SERS data of the conditioned medium from a bacterial culture, having a more complex background, we achieve 1 ng·mL-1 limit of detection of pyocyanin and robust quantification of concentration spanning 5 orders of magnitude. Nanogaps are also incorporated in an in-line microfluidic device, enabling longitudinal monitoring of P. aeruginosa biofilm formation via rapid pyocyanin detection in a medium effluent as early as 3 h after inoculation and quantification in under 9 h. Surface-attached bacteria exposed to a bactericidal antibiotic were differentially less susceptible after 10 h of growth, indicating that these devices may be useful for early intervention of bacterial infections.

Driving Chemical Reactions in Plasmonic Nanogaps with Electrohydrodynamic Flow.

Nanoparticles from colloidal solution-with controlled composition, size, and shape-serve as excellent building blocks for plasmonic devices and metasurfaces. However, understanding hierarchical driving forces affecting the geometry of oligomers and interparticle gap spacings is still needed to fabricate high-density architectures over large areas. Here, electrohydrodynamic (EHD) flow is used as a long-range driving force to enable carbodiimide cross-linking between nanospheres and produces oligomers exhibiting sub-nanometer gap spacing over mm2 areas. Anhydride linkers between nanospheres are observed via surface-enhanced Raman scattering (SERS) spectroscopy. The anhydride linkers are cleavable via nucleophilic substitution and enable placement of nucleophilic molecules in electromagnetic hotspots. Atomistic simulations elucidate that the transient attractive force provided by EHD flow is needed to provide a sufficient residence time for anhydride cross-linking to overcome slow reaction kinetics. This synergistic analysis shows assembly involves an interplay between long-range driving forces increasing nanoparticle-nanoparticle interactions and probability that ligands are in proximity to overcome activation energy barriers associated with short-range chemical reactions. Absorption spectroscopy and electromagnetic full-wave simulations show that variations in nanogap spacing have a greater influence on optical response than variations in close-packed oligomer geometry. The EHD flow-anhydride cross-linking assembly method enables close-packed oligomers with uniform gap spacings that produce uniform SERS enhancement factors. These results demonstrate the efficacy of colloidal driving forces to selectively enable chemical reactions leading to future assembly platforms for large-area nanodevices.

Electric field enhancement with plasmonic colloidal nanoantennas excited by a silicon nitride waveguide.

We investigate the feasibility of CMOS-compatible optical structures to develop novel integrated spectroscopy systems. We show that local field enhancement is achievable utilizing dimers of plasmonic nanospheres that can be assembled from colloidal solutions on top of a CMOS-compatible optical waveguide. The resonant dimer nanoantennas are excited by modes guided in the integrated silicon nitride waveguide. Simulations show that 100-fold electric field enhancement builds up in the dimer gap as compared to the waveguide evanescent field amplitude at the same location. We investigate how the field enhancement depends on dimer location, orientation, distance and excited waveguide mode.

Sub-micron silicon nitride waveguide fabrication using conventional optical lithography.

We demonstrate a novel technique to fabricate sub-micron silicon nitride waveguides using conventional contact lithography with MEMS-grade photomasks. Potassium hydroxide anisotropic etching of silicon facilitates line reduction and roughness smoothing and is key to the technique. The fabricated waveguides is measured to have a propagation loss of 0.8dB/cm and nonlinear coefficient of γ = 0.3/W/m. A low anomalous dispersion of <100ps/nm/km is also predicted. This type of waveguide is highly suitable for nonlinear optics. The channels naturally formed on top of the waveguide also make it promising for plasmonics and quantum efficiency enhancement in sensing applications.

Fano resonances in metasurfaces made of linear trimers of plasmonic nanoparticles.

We investigate Fano resonances in planar two-dimensional periodic arrays of linear trimers of plasmonic nanoparticles that appear under plane wave incidence. The observed Fano resonances are associated to resonances belonging to the trimer (metamolecule) itself, where some are found to be strongly affected by the array periodicity. We observe that array-dependent resonances appearing for oblique incidence are resistant to losses, whereas narrow dipolar-like Fano resonances associated mainly to the metamolecule, which appear also under normal incidence, disappear when losses are too high. In particular, we prove the latter by theoretical (dipolar approximation) and full-wave simulations, in good agreement. We propose that the use of very low-loss plasmonic materials or the use of gain materials to mitigate plasmonic losses may lead to (high-quality factor) dipolar-like Fano resonances under normal incidence, exhibiting a certain degree of fabrication defect tolerance, which might be employed to improve sensors, lasing, switching, and nonlinear devices, for example.

Graphene-based tunable hyperbolic metamaterials and enhanced near-field absorption.

We investigate a novel implementation of hyperbolic metamaterial (HM) at far-infrared frequencies composed of stacked graphene sheets separated by thin dielectric layers. Using the surface conductivity model of graphene, we derive the homogenization formula for the multilayer structure by treating graphene sheets as lumped layers with complex admittances. Homogenization results and limits are investigated by comparison with a transfer matrix formulation for the HM constituent layers. We show that infrared iso-frequency wavevector dispersion characteristics of the proposed HM can be tuned by varying the chemical potential of the graphene sheets via electrostatic biasing. Accordingly, reflection and transmission properties for a film made of graphene-dielectric multilayer are tunable at terahertz frequencies, and we investigate the limits in using the homogenized model compared to the more accurate transfer matrix model. We also propose to use graphene-based HM as a super absorber for near-fields generated at its surface. The power emitted by a dipole near the surface of a graphene-based HM is increased dramatically (up to 5 × 10(2) at 2 THz), furthermore we show that most of the scattered power is directed into the HM. The validity and limits of the homogenized HM model are assessed also for near-fields and show that in certain conditions it overestimates the dipole radiated power into the HM.

Effect of irregularities of nanosatellites position and size on collective electric and magnetic plasmonic resonances in spherical nanoclusters.

Spherical nanoclusters (NCs) with a central dielectric core surrounded by several satellite plasmonic nanospheres have been recently investigated as aggregates supporting electric and magnetic collective resonances. Notably, the collective magnetic resonance has been exploited to provide magnetic properties in optics, i.e., materials with macroscopic relative permeability different from unity. The NCs discussed in this paper can be realized using state-of-the-art nanochemistry self-assembly techniques. Accordingly, perfectly regular disposition of the nanoplasmonic satellites is not possible and this paper constitutes the first comprehensive analysis of the effect of such irregularities onto the electric and magnetic collective resonances. In particular we will show that the peak of the scattering cross section associated to the magnetic resonance is very sensitive to certain irregularities and significantly less to others. It is shown here that "artificial magnetic" properties of NCs are preserved for certain degrees of irregularities of the nanosatellites positions, however they are strongly affected by irregularities in the plasmonic nanosatellites sizes and by the presence of "defects" caused by the absence of satellites in the process of self-assembly around the dielectric core. The "artificial electric" resonance is instead less affected by irregularities mainly because of its wider frequency bandwidth.

Comparison of electric field enhancements: linear and triangular oligomers versus hexagonal arrays of plasmonic nanospheres.

We investigate local electromagnetic field enhancements in oligomers of plasmonic nanospheres. We first evaluate via full-wave simulations the field between spheres in several oligomer systems: linear dimers, linear trimers, trimers 60°, trimers 90° and linear quadrumers. To gain a better understanding of the field enhancement values, we compare the results with local fields in a hexagonal close-packed (HCP) configuration with same structural dimensions. We then inter-relate the field enhancement values found via full-wave simulations to SERS enhancements of actual fabricated self-assembled oligomers. We find that linear oligomers provide the largest field enhancement values. Finally, we provide closed-form formulas for the prediction of the resonance frequency responsible for field enhancement in linear oligomers, namely dimers, trimers and quadrumers, modeling each nanosphere as a single electric dipole. These formulas provide with resonance values less than 7% shifted when compared to full-wave results even when the gap between spheres is only about one fifth of the radius, showing the powerfulness of dipolar approximations. The results shown in this paper demonstrate that ad hoc clusters of nanospheres can be designed and fabricated to obtain larger field enhancements than with the HCP structure and this may pave the way for the development of improved sensors for molecular spectroscopy.

Directing cluster formation of Au nanoparticles from colloidal solution.

Discrete clusters of closely spaced Au nanoparticles can be utilized in devices from photovoltaics to molecular sensors because of the formation of strong local electromagnetic field enhancements when illuminated near their plasmon resonance. In this study, scalable, chemical self-organization methods are shown to produce Au nanoparticle clusters with uniform nanometer interparticle spacing. The performance of two different methods, namely electrophoresis and diffusion, for driving the attachment of Au nanoparticles using a chemical cross-linker on chemically patterned domains of polystyrene-block-poly(methyl methacrylate) (PS-b-PMMA) thin films are evaluated. Significantly, electrophoresis is found to produce similar surface coverage as diffusion in 1/6th of the processing time with an ~2-fold increase in the number of Au nanoparticles forming clusters. Furthermore, average interparticle spacing within Au nanoparticle clusters was found to decrease from 2-7 nm for diffusion deposition to approximately 1-2 nm for electrophoresis deposition, and the latter method exhibited better uniformity with most clusters appearing to have about 1 nm spacing between nanoparticles. The advantage of such fabrication capability is supported by calculations of local electric field enhancements using electromagnetic full-wave simulations from which we can estimate surface-enhanced Raman scattering (SERS) enhancements. In particular, full-wave results show that the maximum SERS enhancement, as estimated here as the fourth power of the local electric field, increases by a factor of 100 when the gap goes from 2 to 1 nm, reaching values as large as 10(10), strengthening the usage of electrophoresis versus diffusion for the development of molecular sensors.

An optical leaky wave antenna with Si perturbations inside a resonator for enhanced optical control of the radiation.

We investigate the directive radiation at 1550 nm from an optical leaky wave antenna (OLWA) with semiconductor perturbations made of silicon (Si). We study the radiation pattern dependence on the physical dimensions, number of perturbations and carrier densities in these semiconductor perturbations through optical excitations at a visible wavelength, 625 nm. In this detailed theoretical study we show the correlation between the pump power absorbed in the perturbations, the signal guided in the waveguide and the radiation through leakage. To overcome the limited control of the radiation intensity through excess carrier generation in Si, we present a new design with the OLWA integrated with a Fabry-Pérot resonator (FPR). We provide analytical and numerical studies of the enhanced radiation performance of the OLWA antenna inside the FPR, and derive closed-form formulas accounting for LW reflection at the edges of the FPR. A discussion on the constructive and destructive radiation by the direct and reflected leaky waves in the FPR resonator is provided. Results shown in this paper exhibit 3 dB variation of the radiation and pave the way for further optimization and theoretical developments.

Composite material made of plasmonic nanoshells with quantum dot cores: loss-compensation and ε-near-zero physical properties.

A theoretical investigation of loss-compensation capabilities in composite materials made of plasmonic nanoshells is carried out by considering quantum dots (QDs) as the nanoshells' cores. The QD and metal permittivities are modeled according to published experimental data. We determine the modes with real or complex wavenumber able to propagate in a 3D periodic lattice of nanoshells. Mode analysis is also used to assess that only one propagating mode is dominant in the composite material whose optical properties can hence be described via homogenization theory. Therefore, the material effective permittivity is found by comparing different techniques: (i) the mentioned mode analysis, (ii) Maxwell Garnett mixing rule and (iii) the Nicolson-Ross-Weir method based on transmission and reflection when considering a metamaterial of finite thickness. The three methods are in excellent agreement, because the nanoshells considered in this paper are very subwavelength, thus justifying the parameter homogenization. We show that QDs are able to provide loss-compensated ε-near-zero metamaterials and also loss-compensated metamaterials with large negative values of permittivity. Besides compensating for losses, the strong gain via QD can provide optical amplification with particular choices of the nanoshell and lattice dimensions.

Non-lithographic SERS substrates: tailoring surface chemistry for Au nanoparticle cluster assembly.

Near-field plasmonic coupling and local field enhancement in metal nanoarchitectures, such as arrangements of nanoparticle clusters, have application in many technologies from medical diagnostics, solar cells, to sensors. Although nanoparticle-based cluster assemblies have exhibited signal enhancements in surface-enhanced Raman scattering (SERS) sensors, it is challenging to achieve high reproducibility in SERS response using low-cost fabrication methods. Here an innovative method is developed for fabricating self-organized clusters of metal nanoparticles on diblock copolymer thin films as SERS-active structures. Monodisperse, colloidal gold nanoparticles are attached via a crosslinking reaction on self-organized chemically functionalized poly(methyl methacrylate) domains on polystyrene-block-poly(methyl methacrylate) templates. Thereby nanoparticle clusters with sub-10-nanometer interparticle spacing are achieved. Varying the molar concentration of functional chemical groups and crosslinking agent during the assembly process is found to affect the agglomeration of Au nanoparticles into clusters. Samples with a high surface coverage of nanoparticle cluster assemblies yield relative enhancement factors on the order of 109 while simultaneously producing uniform signal enhancements in point-to-point measurements across each sample. High enhancement factors are associated with the narrow gap between nanoparticles assembled in clusters in full-wave electromagnetic simulations. Reusability for small-molecule detection is also demonstrated. Thus it is shown that the combination of high signal enhancement and reproducibility is achievable using a completely non-lithographic fabrication process, thereby producing SERS substrates having high performance at low cost.

Dual polarized near-field focusing plate for near-field optical focusing in two dimensions.

We introduce a dual polarized near-field focusing plate (DP-NFFP) with focusing in two dimensions, designed to operate at the near infrared frequency of 193 THz (λ(0) = 1550 nm). Subwavelength focusing in two dimensions, for both incident polarizations, is achieved at a distance of a quarter wavelength from the DP-NFFP. The design procedure is described in detail and the proposed design could be easily scaled to other working frequencies, from microwave to optics. We show that the use of ideal lossless (i.e., perfect electric conductor) or real lossy (i.e., silver) metals provide with subwavelength focusing at 193 THz, indicating that metal losses do not significantly affect the DP-NFFP performance, and thus confirming the design feasibility at the near-infrared frequency. Results are validated by using two distinct full-wave simulators.

Complex bound and leaky modes in chains of plasmonic nanospheres.

Bound and leaky modes with complex wavenumber in chains (linear arrays) of plasmonic nanospheres are characterized for both longitudinal and transverse polarization states (with respect to the array axis). The proposed method allows for the description of each mode evolution when varying frequency. As a consequence, full characterization of the guided modes with complex wavenumber is provided in terms of propagation direction, guidance or radiance, proper or improper, and physical or nonphysical conditions. Each nanosphere is modeled according to the single dipole approximation, and the metal permittivity is described by the Drude model. Modal wavenumbers are obtained by computing the complex zeroes of the homogeneous equation characterizing the field in the one dimensional periodic array. The required periodic Green's function is analytically continued into the complex wavenumber space by using the Ewald method. Furthermore, a parametric analysis of the mode wavenumbers is performed with respect to the geometrical parameters of the array.

Effective model and investigation of the near-field enhancement and subwavelength imaging properties of multilayer arrays of plasmonic nanospheres.

When a small radiating or scattering object is placed near a multilayer array of plasmonic nanospheres, on the other side the optical near field is enhanced due to the excitation of resonant modes in the layers. For some particular frequencies, the field behind the array is concentrated in a subwavelength region, creating a super resolution effect. Resonating layers are able to reproduce (transport) part of the evanescent spectrum to the other side of these layers which otherwise would decay rapidly. We explore the mechanism of evanescent field transport and subwavelength field concentration on the other side of the layered material and show the relationship between near-field enhancement, field concentration, and modal dispersion characteristics. A detailed investigation of these phenomena is carried out by using an effective numerical model based on the array scanning method (ASM) combined with the Ewald method to accelerate the convergence of the dyadic Green function calculation. The subwavelength-sized spheres forming the arrays are represented as single dipole radiators, and the model of their interactions takes into account all the radiative and reactive field components.

Silicon-based optical leaky wave antenna with narrow beam radiation.

We propose a design of a dielectric (silicon nitride) optical leaky wave antenna (OLWA) with periodic semiconductor (silicon) corrugations, capable of producing narrow beam radiation. The optical antenna radiates a narrow beam because a leaky wave (LW) with low attenuation constant is excited at one end of the corrugated dielectric waveguide. We show that pointing angle, beam-width, and operational frequency are all related to the LW complex wavenumber, whose value depends on the amount of silicon perturbations in the waveguide. In this paper, the propagation constant and the attenuation coefficient of the LW in the periodic structure are extracted from full-wave simulations. The far-field radiation patterns in both glass and air environments predicted by LW theory agree well with the ones obtained by full-wave simulations. We achieve a directive radiation pattern in glass environment with about 17.5 dB directivity and 1.05 degree beam-width at the operative free space wavelength of 1.55 µm, pointing at a direction orthogonal to the waveguide (broadside direction). We also show that the use of semiconductor corrugations facilitate electronic tuning of the radiation pattern via carrier injection.