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Enhancing the circular dichroism signals of chiral plasmonic nanostructures is vital for realizing miniaturized functional chiroptical devices, such as ultrathin wave plates and high-performance chiral biosensors. Rationally assembling individual plasmonic metamolecules into coupled nanoclusters or periodic arrays provides an extra degree of freedom to effectively manipulate and leverage the intrinsic circular dichroism of the constituent structures. Here, we show that sophisticated manipulation over the geometric parameters of a plasmonic stereo-metamolecule array enables selective excitation of its surface lattice resonance mode either by left- or right-handed circularly polarized incidence through diffraction coupling, which can significantly amplify the differential absorption and hence the intrinsic circular dichroism. In particular, since the diffraction coupling requires no index-matching condition and its handedness can be switched by manipulating the refractive index of either the superstrate or the substrate, it is therefore possible to achieve dynamic tuning and active control of the intrinsic circular dichroism response without the need of modifying structure parameters. Our proposed system provides a versatile platform for ultrasensitive chiral plasmonics biosensing and light field manipulation.

Metal nanoparticles supporting plasmons are widely used to enhance electromagnetic fields, resulting in strong light–matter interactions at the nanoscale in a diverse range of applications. Recently, it has been shown that when metal nanorods are periodically arranged with proper lattice periods, surface lattice resonances (SLRs) can be excited and near fields can be greatly enhanced over extended volumes. In this work, we report significant near field enhancement over even larger volumes by placing the metal nanorod array within a Fabry–Pérot (F-P) microcavity. Simulation results show that by taking advantage of strong coupling between the SLR and the photonic F-P resonances, the electric field intensity of the bonding split mode can be enhanced by up to 1935 times, which is about three times of the enhancement of the SLR, and the greatly enhanced field can extend over most of the F-P microcavity. We further show that the F-P resonances of both odd and even orders can strongly couple to the SLR by varying the nanorods position from the middle of the microcavity. We expect that the proposed plasmonic-photonic coupling system will find promising applications in nanolasers, nonlinear optics and sensing.

We investigate the chiro-optical properties of the electromagnetic near-field associated with the excitation of collective optical resonances (surface lattice resonances) in achiral plasmonic lattices. These arrays are specially designed to support dispersive resonances with nontrivial, multipolar near-field distributions in the surroundings of the nanostructure, which gives rise to an enhanced chiro-optical response. The presence of these multipolar resonances in lattices without explicitly broken mirror symmetry is experimentally confirmed by far-field extinction measurements, while the angular, spectral, and spatial dependence of the associated chiral near-field are numerically simulated. In contrast with typical pseudochiral systems, the extended chiro-optical near-field response appears even at normal incidence. We believe that surface lattice resonances in achiral plasmonic lattices can be potentially utilized as a substrate for enhanced background-free enantioselectivity and tunable chiral molecule recognition over large areas.

Engineering nanostructures with exceptionally high-Q resonances mediated by the Fano-type hybridization between discrete states associated with the periodicity of the structure and broadband resonances excited on constituent scatterers are the emerging field in optics and photonics. These collective lattice resonances (CLRs) attracted a lot of attention in recent years due to a number of their exciting applications in sensing, optical filtering, structural color printing, fluorescence enhancement, nanoscale lasing, and nonlinear optics, which resulted in a rapidly growing number of fundamental and experimental studies. CLRs have been discovered for arrays of plasmonic metal nanoparticles with strong electric dipole resonances nearly four decades ago. Thereafter, the scope of CLRs has gradually extended to all-dielectric and magneto-optical nanoparticles, 2D materials and other types of constituents, which has broadened the range of CLRs applicability and enriched their properties. We provide a comprehensive review of the recent progress in this field with a special emphasis on advances far beyond plasmonics.

Dielectric metasurfaces have shown prominent applications in nonlinear optics due to strong field enhancement and low dissipation losses at the nanoscale. Chalcogenide glasses are one of the promising materials for the observation of nonlinear effects thanks to their high intrinsic nonlinearities. Here, we demonstrate, experimentally and theoretically, that significant second harmonic generation (SHG) can be obtained within amorphous Selenium (Se)-based chalcogenide metasurfaces by exploiting the coupling between lattice and particle resonances. We further show that the high-quality factor resonance at the origin of the SHG can be tuned over a wide wavelength range using a simple and versatile fabrication approach. The measured second harmonic intensity is orders of magnitude higher than that from a dewetted Se film consisting of random Se nanoparticles. The achieved conversion efficiency in the resonance region is of the order of 10−6 which is comparable with direct bandgap materials and at least two orders of magnitude higher than that of conventional plasmonics- and Si-based structures. Fabricated via a simple and scalable technique, these all-dielectric architectures are ideal candidates for the design of flat nonlinear optical components on flexible substrates.

We report on reversible all-optical emission control and lasing in plasmonic nanoparticle lattices. By incorporating photochromic molecules into the liquid gain medium composed of organic fluorescent molecules, we realize all-optical control over gain and absorption, the two key parameters associated with both conventional and nanoscale lasing. We demonstrate reversible photoswitching between two distinct modes of operation: (1) spontaneous emission to the lattice mode, characterized by broad emission line width, low emission intensity, and large angular distribution; and (2) lasing action, characterized by very narrow (sub-nm) line widths due to the emergence of increased gain and temporal coherence in the system, approximately 3 orders of magnitude increase in emission intensity, and narrow 0.7° angular divergence of the beam. A rate-equation model is employed to describe the operation of the switchable plasmonic laser. Our results provide the first demonstration of optically tunable losses in plasmonic lattice lasers, which is an important milestone for the development of active plasmonics and paves the way for ultrafast all-optical switching of plasmonic nanolasers. acceptedVersion

The field of magnetoplasmonics exploits interactions between light and magnetic matter at the nanoscale for light manipulation and resonant magneto-optics. One of the great challenges of this field is overcoming optical losses in magnetic metals. Here, we exploit surface plasmon polaritons (SPPs) excited at the interface of an SiO2 / Au bilayer to induce strong magneto-optical responses on the Ni nanodisks of a periodic array. Using a reference system made of Au nanodisks, we show that optical losses in Ni hardly broaden the linewidth of SPP-driven magnetooptical signals. Loss mitigation is attained because the free electrons in the Ni nanodisks are driven into forced oscillations away from their plasmon resonance. By varying the SiO2 layer thickness and lattice constant of the Ni nanodisk array, we demonstrate tailoring of intense magneto-optical Kerr effects with a spectral linewidth down to ~25 nm. Our results provide important hints on how to circumvent optical losses and enhance magneto-optical signals via the design of off-resonance magnetoplasmonic driving mechanisms., This work was supported by the Academy of Finland under Project No. 316857, Funder Id: http://dx.doi.org/10.13039/501100002341 and by the Aalto Centre for Quantum Engineering. M.K. acknowledges support from the European Commission (Marie SkłodowskaCurie IF EMPHASIS – DLV-748429). Lithography was performed at the Micronova Nanofabrication Centre, supported by Aalto University.

openaire: EC/H2020/745115/EU//OPLD Nanoscale coherent light sources offer potentially ultrafast modulation speeds, which could be utilized for novel sensors and optical switches. Plasmonic periodic structures combined with organic gain materials have emerged as promising candidates for such nanolasers. Their plasmonic component provides high intensity and ultrafast nanoscale-confined electric fields, while organic gain materials offer fabrication flexibility and a low acquisition cost. Despite reports on lasing in plasmonic arrays, lasing dynamics in these structures have not been experimentally studied yet. Here we demonstrate, for the first time, an organic dye nanoparticle-array laser with more than a 100 GHz modulation bandwidth. We show that the lasing modulation speed can be tuned by the array parameters. Accelerated dynamics is observed for plasmonic lasing modes at the blue side of the dye emission.

We report on lasing at visible wavelengths in arrays of ferromagnetic Ni nanodisks overlaid with an organic gain medium. We demonstrate that by placing an organic gain material within the mode volume of the plasmonic nanoparticles both the radiative and, in particular, the high ohmic losses of Ni nanodisk resonances can be compensated. Under increasing pump fluence, the systems exhibit a transition from lattice-modified spontaneous emission to lasing, the latter being characterized by highly directional and sub-nanometer line width emission. By breaking the symmetry of the array, we observe tunable multimode lasing at two wavelengths corresponding to the particle periodicity along the two principal directions of the lattice. Our results are relevant for loss-compensated magnetoplasmonic devices and topological photonics.

We demonstrate that a periodic lattice of detuned resonators can suppress the THz extinction at the central resonant frequency, leading to an enhanced transparency due to diffraction. The system consists of metallic rods of two different sizes, each of them supporting a strong half-wavelength (λ/2) resonance, which are spatially displaced within the unit cell of the lattice. Using a coupled dipole model we show that the diffraction enhanced transparency (DET) window has its origin in the interference between two surface lattice resonances, arising from the diffractively enhanced radiative coupling of the λ/2 resonances in the lattice. Group-index measurements show that the THz field is strongly delayed by more than 4 orders of magnitude at the transparency window. Since DET does not involve the near-field coupling of resonators, the fabrication tolerance to imperfections is expected to be very high. This remarkable response renders these systems as very interesting components for THz communication.

Because of their large figures of merit, surface lattice resonances (SLRs) in metal nanoparticle arrays are very promising for chemical and biomolecular sensing in both liquid and gas media. SLRs are sensitive to refractive index changes both near the surface of the nanoparticles (surface sensitivity) and in the volume between them (bulk sensitivity). Because of its intrinsic surface-sensitivity and a power law dependence on electric fields, second harmonic generation (SHG) spectroscopy can improve upon both the surface and volume sensitivities of SLRs. In this report on SHG spectroscopy of plasmonic nanoparticles, we show that the SHG signal is greatly increased (up to 450 times) by the SLRs. We also demonstrate very narrow resonances in SHG intensity (∼5 nm fwhm). We illustrate how the SHG resonances are highly sensitive to SLRs by varying the fundamental wavelength, angle of incidence, nanoparticle material, and lattice constant of the arrays. Finally, we identify an SHG resonance (10 nm fwhm) that is electric dipole forbidden and can be attributed to higher-order multipoles, enhanced by the strong near-fields of SLRs. Our results open up new and very promising avenues for chemical and biomolecular sensing based on SHG spectroscopy of SLRs.

We study lasing in regular arrays made from aluminum nanoparticles. We show that these structures function as laser sources at visible wavelengths, even when scaled to an order of magnitude smaller areas compared to existing literature. The aluminum nanoparticles provide a robust platform for studying lasing in plasmonic systems, even when the optical losses are higher compared to silver or gold.

We investigate the radiative coupling between localized surface plasmon resonances (LSPRs) and Rayleigh anomalies (RAs) in periodic arrays of metallic nanorods with varying dimensions but equal lattice constants. The dimensions of the nanorods determine the energy and line width of the LSPR and, thus, enable tailoring of the mixed LSPR-RA states: surface lattice resonances (SLRs). We present variable angle light extinction experimental spectra for five arrays with different nanorod width and explain our results with numerical simulations. The numerical simulations are done for driven and undriven systems, with the latter revealing the SLR eigenmode properties for the first time. We provide a plane wave model that interprets the near- and far-fields of these eigenmodes, describing the intricate behavior of confinement and radiative loss versus in-plane momentum. The SLR line width, band gap associated with the coupled modes, and field extension into the surrounding dielectric are tunable via the dimensions of the nanorods.

Combining localized surface plasmons (LSPs) and diffractive surface waves (DSWs) in metallic nanoparticle gratings leads to the emergence of collective hybrid plasmonic-photonic modes known as surface lattice resonances (SLRs). These show reduced losses and therefore a higher Q factor with respect to pure LSPs, at the price of larger volumes. Thus, they can constitute a flexible and efficient platform for light-matter interaction. However, it remains an open question if there is, in terms of the Q/V ratio, a sizable gain with respect to the uncoupled LSPs or DSWs. This is a fundamental point to shed light upon if such modes want to be exploited, for instance, for cavity quantum electrodynamic effects. Here, using aluminum nanoparticle square gratings with unit cells consisting of narrow-gap disk dimers-a geometry featuring a very small modal volume-we demonstrate that an enhancement of the Q/V ratio with respect to the pure LSP and DSW is obtained for SLRs with a well-defined degree of plasmon hybridization. Simultaneously, we report a 5× increase of the Q/V ratio for the gap-coupled LSP with respect to that of the single nanoparticle. These outcomes are experimentally probed against the Rabi splitting, resulting from the coupling between the SLR and a J-aggregated molecular dye, showing an increase of 80% with respect to the DSW-like SLR sustained by the disk LSP of the dimer. The results of this work open the way toward more efficient applications for the exploitation of excitonic nonlinearities in hybrid plasmonic platforms.

The field of magnetoplasmonics exploits interactions between light and magnetic matter at the nanoscale for light manipulation and resonant magneto-optics. One of the great challenges of this field is overcoming optical losses in magnetic metals. Here, we exploit surface plasmon polaritons (SPPs) excited at the interface of an SiO2/Au bilayer to induce strong magneto-optical responses on the Ni nanodisks of a periodic array. Using a reference system made of Au nanodisks, we show that optical losses in Ni hardly broaden the linewidth of SPP-driven magneto-optical signals. Loss mitigation is attained because the free electrons in the Ni nanodisks are driven into forced oscillations away from their plasmon resonance. By varying the SiO2 layer thickness and lattice constant of the Ni nanodisk array, we demonstrate tailoring of intense magneto-optical Kerr effects with a spectral linewidth down to ~25 nm. Our results provide important hints on how to circumvent optical losses and enhance magneto-optical signals via the design of off-resonance magnetoplasmonic driving mechanisms.

Dielectric metasurfaces have shown prominent applications in nonlinear optics due to strong field enhancement and low dissipation losses at the nanoscale. Chalcogenide glasses are one of the promising materials for the observation of nonlinear effects thanks to their high intrinsic nonlinearities. Here, we demonstrate, experimentally and theoretically, that significant second harmonic generation (SHG) can be obtained within amorphous Selenium (Se)-based chalcogenide metasurfaces by exploiting the coupling between lattice and particle resonances. We further show that the high-quality factor resonance at the origin of the SHG can be tuned over a wide wavelength range using a simple and versatile fabrication approach. The measured second harmonic intensity is orders of magnitude higher than that from a dewetted Se film consisting of random Se nanoparticles. The achieved conversion efficiency in the resonance region is of the order of 10−6 which is comparable with direct bandgap materials and at least two orders of magnitude higher than that of conventional plasmonics- and Si-based structures. Fabricated via a simple and scalable technique, these all-dielectric architectures are ideal candidates for the design of flat nonlinear optical components on flexible substrates.