Optical Near-field Enhancement Research Articles

Dielectric metasurface evolution from bulk to monolayer by strong coupling of quasi-BICs for second harmonic boosting

2D materials are promising candidates as nonlinear optical components for on-chip devices due to their ultrathin structure. In general, their nonlinear optical responses are inherently weak due to the short interaction thickness with light. Recently, there has been great interest in using quasi-bound states in the continuum (q-BICs) of dielectric metasurfaces, which are able to achieve remarkable optical near-field enhancement for elevating the second harmonic generation (SHG) emission from 2D materials. However, most studies focus on the design of combining bulk dielectric metasurfaces with unpatterned 2D materials, which suffer considerable radiation loss and limit near-field enhancement by high-quality q-BIC resonances. Here, we investigate the dielectric metasurface evolution from bulk silicon to monolayer molybdenum disulfide (MoS2), and discover the critical role of meta-atom thickness design on enhancing near-field effects of two q-BIC modes. We further introduce the strong-coupling of the two q-BIC modes by oblique incidence manipulation, and enhance the localized optical field on monolayer MoS2 dramatically. In the ultraviolet and visible regions, the MoS2 SHG enhancement factor of our design is 105 times higher than that of conventional bulk metasurfaces, leading to an extremely high nonlinear conversion efficiency of 5.8%. Our research will provide an important theoretical guide for the design of high-performance nonlinear devices based on 2D materials.

Highly Localized Optical Field Enhancement at Neon Ion Sputtered Tungsten Nanotips.

We present laser-driven rescattering of electrons at a nanometric protrusion (nanotip), which is fabricated with an in situ neon ion sputtering technique applied to a tungsten needle tip. Electron energy spectra obtained before and after the sputtering show rescattering features, such as a plateau and high-energy cutoff. Extracting the optical near-field enhancement in both cases, we observe a strong increase of more than 2-fold for the nanotip. Accompanying finite-difference time-domain (FDTD) simulations show a good match with the experimentally extracted near-field strengths. Additionally, high electric field localization for the nanotip is found. The combination of transmission electron microscope imaging of such nanotips and the determination of the near-field enhancement by electron rescattering represent a full characterization of the electric near-field of these intriguing electron emitters. Ultimately, nanotips as small as single nanometers can be produced, which is of utmost interest for electron diffraction experiments and low-emittance electron sources.

Recent progress of gold nanostructures and their applications.

For noble metals, such as gold (Au) and silver (Ag), it is well-known that surface plasmons of their nanocrystals have significant spatial confinement and propagation loss due to the strong damping effect and the scattering between the plasmons and phonons. Noble metal nanostructures are usually referred to as "plasmonic nanostructures" in many studies. Based on the resonance effect of surface plasmons, the electromagnetic field can be localized on the subwavelength scale, which induces a booming new field of nanophotonics. Among the various nanostructures, Au nanostructures have received extensive attention both in fundamental research and technological fields due to their unique localized surface plasmon characteristics. These characteristics include strong optical extinction, near-field enhancement, and far-field scattering. By changing either the morphological parameters or the surrounding medium of nanostructures, the localized surface plasmon resonance (SPR) of Au nanostructures can be tuned in a large spectral region from visible to near infrared (Vis-NIR) wavelength. Corresponding to the experimental research, there are several numerical techniques that enable modeling the optical characteristics of Au nanostructures in different shapes and assemblies. The most popular technique is the finite-difference time-domain (FDTD) method for modeling various nanostructures and nanoscale optical devices. The accuracy of the computational models has been proven by reliable experimental data. In this review, we focused on Au nanostructures of different morphologies, such as nanorods, nanocubes, nanobipyramids and nanostars. Then combined with FDTD simulations, we described the effect of morphological parameters and the surrounding medium on the SPR properties of Au nanostructures. More and more achievements indicate that the surface plasmon effect is promising in many technical fields. In the last part, we summarize some typical applications of plasmonic Au nanostructures, such as high sensitivity sensors, photothermal conversion with hot electron effects and photoelectric devices, as well as plasmonic nanolasers.

Substrate-Free Fabrication of Single-Crystal Two-Dimensional Gold Nanoplates for Catalytic Application.

Two-dimensional (2D) gold nanoplates (AuNPLs) have shown potential in catalysis, photonics, electronics, sensing, and biomedicine fields due to their high aspect ratio, fascinating surface chemistry, and quantum-size effect. Therefore, the synthesis of substrate-free, size-controlled single-crystal gold (Au) nanoplates is highly desirable for the development of catalysis and optical near-field enhancement applications. EDTA and hydroxide anions were used in this study to stimulate the formation of microscale single-crystal gold nanoplates under hydrothermal conditions. The reaction temperature, amount of EDTA, and hydroxyl anions all have a significant effect on the morphologies and size distributions of the gold nanoplates. The gold nanoplates had an average side length of between 3 and 11 μm. The application of the microscale single-crystal gold nanoplates as a nanocatalyst proved their excellent catalytic activity and recyclability for the catalysis of 4-nitrophenol to 4-aminophenol, implying that the large-size gold nanoplates were promising in heterogeneous catalysis applications.

Strengthening optical enhancement with AgxAu1−x alloy and Ag/Au heteromaterial sub-micro disk arrays

Material modification on plasmonic nanostructures is recognized as one of many approaches to increase optical near-field enhancement and resonance wavelength tuning. In this work, with finite-difference time-domain simulation, we showed that closed-hexagonal sub-micro disk arrays of the Ag x Au1−x alloy increase electric-field enhancement in the near-infrared spectra at reduced Ag fraction in the alloy, while the arrays of pure Ag does so in the visible spectra. For the enhancement factor in the near-infrared region, the Au array is dominant around the wavelength of 800 nm, whereas the Ag0.74Au0.24 array is slightly stronger at 820 nm. Furthermore, the local confinement in the near-infrared region (800-900 nm) is strengthened by the heteromaterial array of Ag/Au sub-micro disks with alternating rows, which can boost the electric field enhancement at 1.3 and 3.9 times better than those of the pure Au and Ag arrays, respectively. The Ag, Au and Ag/Au plasmonic hexagonal arrays yield the Purcell factors of 2.42 × 105, 1.17 × 104 and 2.72 × 104, respectively, at wavelengths of 695 nm, 828 nm and 795 nm that would be suitable for spontaneous emission rate enhancement in quantum dots.

The total optical force exerted on black phosphorus coated dielectric cylinder pairs enhanced by localized surface plasmon

Non-invasive manipulation and trapping of nanoparticles, molecules, and cells are essential in a variety of fields. The total optical force and near-field enhancement via localized surface plasmon resonance in the dielectric cylinder pairs coated with black phosphorus (DCPs-BP) are studied analytically and numerically in this work. In the DCPs-BP structure, the total optical force between the two cylinders can reach over 1000 pN/(mW μm). Specifically for the polystyrene particle captured in the center of the DCPs-BP structure, the optical trapping force up to 4000 pN/(mW μm) can be achieved. These results provide new avenues for the successful manipulation and capture of nanoscale particles.

Strong-field spectra and optical near-field enhancement at aluminium needle tips

We study the rescattering of photoemitted electrons at aluminium needle tips. For various laser intensities we measure electron energy spectra to identify telltale features of strong-field rescattering, in particular a plateau with near-constant count rate and a high-energy cutoff. This rescattering process is used to investigate the geometry-dependent enhanced optical near-field at the apex of the aluminium tip. A large near-field enhancement, extracted from the spectral data, is supported by 3D finite-difference time-domain simulations. A systematic theoretical investigation of the near-field enhancement at aluminium tips shows a strong dependence on tip opening angle and radius of curvature.

Near-Infrared II Thermoplasmonics of Cuprous Selenide Multilayer Nanoshells: The Role of the Plasmonic Core.

We present a numerical investigation of the plasmonic and photothermal properties of two different types of cuprous selenide (Cu2-xSe) concentric multilayer nanoshells (CMNSs), heteroCMNSs and homoCMNSs, comprising an outer Cu2-xSe nanoshell and an intermediate silica layer but with a different nanoparticle core of either Au or Cu2-xSe. Numerical calculations of optical absorption, near-field enhancement, and local temperature increase are performed with varied dimensions. The plasmon modes from both types of CMNSs are interpreted by combining the plasmon hybridization theory with the surface charge distribution. The two CMNSs exhibit remarkable near-infrared II (NIR-II) plasmonic properties tunable by controlling the interaction between the inner core and the Cu2-xSe nanoshell. The distinct temperature increase distributions between the two CMNSs are identified at their NIR-II resonance wavelengths. The correlation between the partial absorption and the temperature increase of the inner core and Cu2-xSe nanoshell suggests the thermal interplay between the components.

Back-Reflected Performance-Enhanced Flexible Perovskite Photodetectors through Substrate Texturing with Femtosecond Laser.

Recently, enhancing the performance of flexible perovskite photodetectors through facile and effective means has gained greater attention. In contrast to typical approaches through modifying light-active materials, we present here a simple but effective design by improving light-matter interactions through near-field optical interference on a back-reflected substrate, whose architecture includes a morphologically flat top surface and a backscattering surface textured with micro/nanostructures by the femtosecond laser direct writing. A CH3NH3PbI3 perovskite film and poly(ethylene terephthalate) are selected as the light-active and base materials, respectively. Under a 1 V bias voltage actuation and 532 nm laser irradiation at an intensity of 10 mW cm-2, the flexible device exhibits excellent performance in photoresponsivity (47.1 mA W-1), detectivity (3.7 × 1011 Jones), and on/off ratio (4600). Due to the near-field optical enhancement of the substrate and the strong light-matter interaction, the above performance parameters are enhanced by at least 5 times over a wide spectral range of 220-780 nm. Such enhancement behaviors are independent of active material properties and therefore can be compatible with other operations such as crystalline transformation, doping, and interface modification. Moreover, the alteration of stress distribution on the structured substrate facilitates the bending robustness and stability. These features highlight the potential of back-reflected design in the development of flexible perovskite photoelectric devices, which are especially suitable for large-scale industrial production.

Probing optical resonances of silicon nanostructures using tunable-excitation Raman spectroscopy.

Optical materials with a high refractive index enable effective manipulation of light at the nanoscale through strong light confinement. However, the optical near field, which is mainly confined inside such high-index nanostructures, is difficult to probe with existing measurement techniques. Here, we exploit the connection between Raman scattering and the stored electric energy to detect resonance-induced near-field enhancements in silicon nanostructures. We introduce a Raman setup with a wavelength-tunable laser, which allows us to tune the Raman excitation wavelength and thereby identify Fabry-Pérot and Mie type resonances in silicon thin films and nanodisk arrays, respectively. We measure the optical near-field enhancement by comparing the Raman response on and off resonance. Our results show that tunable-excitation Raman spectroscopy can be used as a complimentary far-field technique to reflection measurements for nanoscale characterization and quality control. As proof-of-principle for the latter, we demonstrate that Raman spectroscopy captures fabrication imperfections in the silicon nanodisk arrays, enabling an all-optical quality control of metasurfaces.

Detection of norovirus-like particles with an external force-assisted near-field illumination biosensor

Optical near-field enhancement at a surface where a total internal reflection occurs is an effective phenomenon that can enhance optical signals from markers conjugated with biological materials on the surface. The enhanced signal can be an effective tool to detect trace amounts of a biological substance. An external force-assisted near-field illumination biosensor is based on a sandwich assay that uses magnetic particles instead of a sensor surface to capture the targets. This sensing method detects light signals from targets sandwiched between magnetic particles and optical markers. The signal of the sandwiched target can be easily distinguished from optical noise by observing the movement of the signal induced by an external magnetic field. In this study, we improved the detection ability by using 60 nm Ø gold nanoparticles as markers. Norovirus virus-like particles were added to a buffer or a contaminated water sample and successfully detected using this system.

Surface Plasmon-Polariton: A Novel Way To Initiate Azide-Alkyne Cycloaddition.

Plasmon catalysis has recently generated tremendous interest in the field of modern chemistry. Application of plasmon introduces the principally new stimulus for the activation of organic reactions, keeping the optical energy concentrated in the vicinity of plasmonic structure, creating an optical near-field enhancement as well as hot electron injection. In this work, for the first time, we presented a new way for the initiation of the azide-alkyne cycloaddition (AAC) using the surface plasmon-polariton wave, supported by the gold grating. With this concept in hand, the plasmon-active gold grating was functionalized with 4-ethynylbenzenediazonium compound. Then, surface-grafted 4-ethynylphenyl groups were plasmon activated and clicked with 4-azidobenzoic acid. Additional experiments allowed to exclude the potential effect of photon, heating, and metal impurities confirmed the key role of surface plasmon-polariton AAC activation. For the investigation of plasmon-induced AAC mechanism, 4-azidophenyl groups (instead of 4-ethynylphenyl groups) were also grafted to the grating surface. Further careful evaluation of reaction kinetics demonstrates that the AAC reaction rate is significantly higher in the case of acetylene activation than in the case of azide activation.

Theoretical study on femtosecond laser optical breakdown threshold in water mediated by aluminum nanoparticle coated with silica.

A strongly coupled finite element model of the optical breakdown during femtosecond laser pulse interaction, with different morphology of aluminum nanoparticles in water, was developed. This model provided new insight into the optical breakdown dependence on the nanoparticles' morphology and assembly. This model was used to theoretically investigate a 300 fs laser pulse interaction with uncoupled and plasmon coupled aluminum coated silica shell nanoparticles. This study revealed how the nanoparticles' one-dimensional assembly affected the optical breakdown threshold of its surrounding mediums. The optical breakdown threshold had much stronger dependence on the optical near-field enhancement than on the nanostructure's extinction cross-section. The maximum electric field that is outside of the aluminum nanoparticles, with 2 nm silica shell and 2 nm gap, was more than 4 times greater to the one inside of the aluminum nanoparticles. For dimer and trimer configuration, the calculated lattice cross-section temperatures at each breakdown threshold were below their melting point. It is suggested that water could be ionized by aluminum/silica (core/shell) nanostructure during femtosecond laser exposures without nanoparticles consumption. This model could increase understanding of the aluminum nanoparticle-mediated optical breakdown in water.

Surface-enhanced circular dichroism by multipolar radiative coupling.

We present numerical investigation of the mechanism of surface-enhanced circular dichroism of a chiral medium near nanoantennas. Strong circular dichroism was observed from the chiral medium surrounding nanoantennas with multipolar resonant modes, and the strong circular dichroism was more correlated to the multipolar resonances than to nearfield enhancement or optical helicity enhancement. According to this observation, we suggest multipolar radiative coupling between the nanoantennas and chiral medium as a possible mechanism of the strong chiral response. This work clarifies a mechanism of surface-enhanced chiral responses and would be useful for designing an enantiomeric-sensing platform and realizing devices relying on strong chirality, such as topological metamaterials for scattering-immune propagation of light and negative index metamaterials.

Double-resonant enhancement of third-harmonic generation in graphene nanostructures.

Intriguing and unusual physical properties of graphene offer remarkable potential for advanced, photonics-related technological applications, particularly in the area of nonlinear optics at the deep-subwavelength scale. In this study, we use a recently developed numerical method to illustrate an efficient mechanism that can lead to orders of magnitude enhancement of the third-harmonic generation in graphene diffraction gratings. In particular, we demonstrate that by taking advantage of the geometry dependence of the resonance wavelength of localized surface-plasmon polaritons of graphene ribbons and discs one can engineer the spectral response of graphene gratings so that strong plasmonic resonances exist at both the fundamental frequency and third-harmonic (TH). As a result of this double-resonant mechanism for optical near-field enhancement, the intensity of the TH can be increased by more than six orders of magnitude.This article is part of the themed issue 'New horizons for nanophotonics'.

Analytic Optimization of Near-Field Optical Chirality Enhancement.

We present an analytic derivation for the enhancement of local optical chirality in the near field of plasmonic nanostructures by tuning the far-field polarization of external light. We illustrate the results by means of simulations with an achiral and a chiral nanostructure assembly and demonstrate that local optical chirality is significantly enhanced with respect to circular polarization in free space. The optimal external far-field polarizations are different from both circular and linear. Symmetry properties of the nanostructure can be exploited to determine whether the optimal far-field polarization is circular. Furthermore, the optimal far-field polarization depends on the frequency, which results in complex-shaped laser pulses for broadband optimization.

Improved optical enhancement using double-width plasmonic gratings with nanogaps

Plasmonic grating structures have been shown effective at increasing near-field optical enhancement. A double-width plasmonic grating design is introduced, where each period has two alternating metal widths separated by a nanogap. With this new design, analysis has shown that plasmonic resonances couple between each metal section, resulting in even greater optical enhancement compared with single-width gratings. The geometry that gives the greatest optical enhancement has been determined with a computational model. This work demonstrates that the increased enhancement is due to hybridized modes that couple between the two grating segments.

The role of morphology and coupling of gold nanoparticles in optical breakdown during picosecond pulse exposures.

This paper presents a theoretical study of the interaction of a 6 ps laser pulse with uncoupled and plasmon-coupled gold nanoparticles. We show how the one-dimensional assembly of particles affects the optical breakdown threshold of its surroundings. For this purpose we used a fully coupled electromagnetic, thermodynamic and plasma dynamics model for a laser pulse interaction with gold nanospheres, nanorods and assemblies, which was solved using the finite element method. The thresholds of optical breakdown for off- and on-resonance irradiated gold nanosphere monomers were compared against nanosphere dimers, trimers, and gold nanorods with the same overall size and aspect ratio. The optical breakdown thresholds had a stronger dependence on the optical near-field enhancement than on the mass or absorption cross-section of the nanostructure. These findings can be used to advance the nanoparticle-based nanoscale manipulation of matter.

Reversible Association of Nitro Compounds with p-Nitrothiophenol Modified on Ag Nanoparticles/Graphene Oxide Nanocomposites through Plasmon Mediated Photochemical Reaction.

Because localized surface plasmon resonance in nanostructures of noble metals is accompanied by interesting physical effects such as optical near-field enhancement, heat release, and the generation of hot electrons, it has been employed in a wide range of applications, including plasmon-assisted chemical reactions. Here, we use a composite of silver nanoparticles and graphene oxide (Ag@GO) as the catalytic as well as the analytic platform for plasmon-assisted chemical reactions. Through time-dependent surface-enhanced Raman scattering experiments, it is found that p-nitrothiophenol (pNTP) molecules on Ag@GO can be associated with nitro compounds such as nitrobenzene and 1-nitropropane to form azo compounds when aided by the plasmons. Furthermore, the reaction rate can be modulated by varying the wavelength and power of the excitation laser as well as the nitro compounds used. In addition, the aforementioned coupling reaction can be reversed. We demonstrate that the oxidation of azo compounds on Ag@GO using KMnO4 leads to the dissociation of the N═N double bond in the azo compounds and that the rate of bond dissociation can be accelerated significantly via laser irradiation. Furthermore, the pNTP molecules on Ag@GO can be recovered after the oxidation reaction. Finally, we demonstrate that the plasmon-assisted coupling reaction allows for the immobilization of nitro-group-containing fluorophores at specific locations on Ag@GO.

Nanoplasmonics tuned "click chemistry".

Nanoplasmonics is a growing field of optical condensed matter science dedicated to optical phenomena at the nanoscale level in metal systems. Extensive research on noble metallic nanoparticles (NPs) has emerged within the last two decades due to their ability to keep the optical energy concentrated in the vicinity of NPs, in particular, the ability to create optical near-field enhancement followed by heat generation. We have exploited these properties in order to induce a localised "click" reaction in the vicinity of gold nanostructures under unfavourable experimental conditions. We demonstrate that this reaction can be controlled by the plasmonic properties of the nanostructures and we propose two physical mechanisms to interpret the observed plasmonic tuning of the "click" chemistry.