Electrically Excited Plasmonic Ultraviolet Light Sources.

The emission of photons from metal-insulator-metal (MIM) nanojunctions through inelastic tunneling of electrically driven electrons is a well-acknowledged approach to develop miniaturized light sources and ultradense photonic instruments. Generally, the existing research in the optimization of electromigrated tunneling junctions is principally centered on the generation of visible and near-infrared lights. This study reports on the near-ultraviolet (NUV, λ ≈ 355 nm) light emission from enhanced tunneling of electrons using aluminum nanoelectrodes. Compared to conventional noble metals, the high electron density and low screening of aluminum enable supporting of pronounced local fields at high energies (i.e, ultraviolet (UV)). As the color of light can be straightforwardly determined by the properties of tunneling structures, the exquisite features of aluminum have empowered the fashioning of tunneling devices that are able to effectively sustain plasmons at short wavelengths and emit UV light with high photon yield. This demonstration is a breakthrough in the generation of high-energy beams using electrically excited aluminum tunneling platforms, which promisingly accelerates the implementation of electrically tunable and ultradense UV light sources.

Electrically Driven Hot-Carrier Generation and Above-Threshold Light Emission in Plasmonic Tunnel Junctions.

Above-threshold light emission from plasmonic tunnel junctions, when emitted photons have energies significantly higher than the energy scale of incident electrons, has attracted much recent interest in nano-optics, while the underlying physics remains elusive. We examine above-threshold light emission in electromigrated tunnel junctions. Our measurements over a large ensemble of devices demonstrate a giant (∼104) material-dependent photon yield (emitted photons per incident electrons). This dramatic effect cannot be explained only by the radiative field enhancement due to localized plasmons in the tunneling gap. Emission is well described by a Boltzmann spectrum with an effective temperature exceeding 2000 K, coupled to a plasmon-modified photonic density of states. The effective temperature is approximately linear in the applied bias, consistent with a suggested theoretical model describing hot-carrier dynamics driven by nonradiative decay of electrically excited localized plasmons. Electrically generated hot carriers and nontraditional light emission could open avenues for active photochemistry, optoelectronics, and quantum optics.

Monolithic Metal Dimer-on-Film Structure: New Plasmonic Properties Introduced by the Underlying Metal.

Dimers, two closely spaced metallic nanostructures, are one of the primary nanoscale geometries in plasmonics, supporting high local field enhancements in their interparticle junction under excitation of their hybridized "bonding" plasmon. However, when a dimer is fabricated on a metallic substrate, its characteristics are changed profoundly. Here we examine the properties of a Au dimer on a Au substrate. This structure supports a bright "bonding" dimer plasmon, screened by the metal, and a lower energy magnetic charge transfer plasmon. Changing the dielectric environment of the dimer-on-film structure reveals a broad family of higher-order hybrid plasmons in the visible region of the spectrum. Both of the localized surface plasmons resonances (LSPR) of the individual dimer-on-film structures as well as their collective surface lattice resonances (SLR) show a highly sensitive refractive index sensing response. Implementation of such all-metal magnetic-resonant nanostructures offers a promising route to achieve higher-performance LSPR- and SLR-based plasmonic sensors.

Toroidal Dipole-Enhanced Third Harmonic Generation of Deep Ultraviolet Light Using Plasmonic Meta-atoms.

The harmonic generation of light with plasmonic and all-dielectric nanostructures has gained much recent interest. This approach is especially promising for short wavelength (i.e., ultraviolet (UV)) generation, where conventional nonlinear crystals reach their limits both in transparency and in their ability to achieve phase-matching between the input and output fields. Here, we demonstrate that the third harmonic generation of deep UV light in an indium tin oxide (ITO) film can be substantially enhanced by a metasurface consisting of metallic toroidal meta-atoms covered with an alumina layer for protection against laser-induced damage. This approach combines the benefits of the large nonlinear susceptibility of ITO with the unique field enhancement properties of a toroidal metasurface. This ITO-meta-atom combination produces a third harmonic signal at a wavelength of 262 nm that is nominally five times larger than that of an ITO film patterned with a conventional hotspot-enhanced plasmonic dimer array. This result demonstrates the potential for toroidal meta-atoms as the active engineered element in a new generation of enhanced nonlinear optical materials and devices.

Azimuthally and radially excited charge transfer plasmon and Fano lineshapes in conductive sublayer-mediated nanoassemblies.

Here, the plasmon responses of both symmetric and antisymmetric oligomers on a conductive substrate under linear, azimuthal, and radial polarization excitations are analyzed numerically. By observing charge transfer plasmons under cylindrical vector beam (CVB) illumination for what we believe is the first time, we show that our studies open new horizons to induce significant charge transfer plasmons and antisymmetric Fano resonance lineshapes in metallic substrate-mediated plasmonic nanoclusters under both azimuthal and radial excitation as CVBs.

Hot electron generation by aluminum oligomers in plasmonic ultraviolet photodetectors.

We report on an integrated plasmonic ultraviolet (UV) photodetector composed of aluminum Fano-resonant heptamer nanoantennas deposited on a Gallium Nitride (GaN) active layer which is grown on a sapphire substrate to generate significant photocurrent via formation of hot electrons by nanoclusters upon the decay of nonequilibrium plasmons. Using the plasmon hybridization theory and finite-difference time-domain (FDTD) method, it is shown that the generation of hot carriers by metallic clusters illuminated by UV beam leads to a large photocurrent. The induced Fano resonance (FR) minimum across the UV spectrum allows for noticeable enhancement in the absorption of optical power yielding a plasmonic UV photodetector with a high responsivity. It is also shown that varying the thickness of the oxide layer (Al2O3) around the nanodisks (tox) in a heptamer assembly adjusted the generated photocurrent and responsivity. The proposed plasmonic structure opens new horizons for designing and fabricating efficient opto-electronics devices with high gain and responsivity.

Transition from capacitive coupling to direct charge transfer in asymmetric terahertz plasmonic assemblies.

We experimentally and numerically analyze the charge transfer THz plasmons using an asymmetric plasmonic assembly of metallic V-shaped blocks. The asymmetric design of the blocks allows for the excitation of classical dipolar and multipolar modes due to the capacitive coupling. Introducing a conductive microdisk between the blocks, we facilitated the excitation of the charge transfer plasmons and studied their characteristics along with the capacitive coupling by varying the size of the disk.

Enhancement of photothermal heat generation by metallodielectric nanoplasmonic clusters.

A four-member homogenous quadrumer composed of silver core-shell nanostructures is tailored to enhance photothermal heat generation efficiency in sub-nanosecond time scale. Calculating the plasmonic and photothermal responses of metallic cluster, we show that it is possible to achieve thermal heat flux generation of 64.7 µW.cm-2 and temperature changes in the range of ΔT = 150 K, using Fano resonant effect. Photothermal heat generation efficiency is even further enhanced by adding carbon nanospheres to the offset gap between particles and obtained thermal heat flux generation of 93.3 µW.cm-2 and temperature increase of ΔT = 172 K. It is also shown that placement of dielectric spheres gives rise to arise collective magnetic dark plasmon modes that improves the quality of the observed Fano resonances. The presented data attests the superior performance of the proposed metallodielectric structures to utilize in practical tumor and cancer therapies and drug delivery applications.

Tailoring the negative-refractive-index metamaterials composed of semiconductor-metal-semiconductor gold ring/disk cavity heptamers to support strong Fano resonances in the visible spectrum.

In this study, we investigated numerically the plasmon response of a planar negative-index metamaterial composed of symmetric molecular orientations of Au ring/disk nanocavities in a heptamer cluster. Using the plasmon hybridization theory and considering the optical response of an individual nanocluster, we determined the accurate geometrical sizes for a ring/disk nanocavity heptamer. It is shown that the proposed well-organized nanocluster can be tailored to support strong and sharp Fano resonances in the visible spectrum. Surrounding and filling the heptamer clusters by various metasurfaces with different chemical characteristics, and illuminating the structure with an incident light source, we proved that this configuration reflects low losses and isotropic features, including a pronounced Fano dip in the visible spectrum. Technically, employing numerical methods and tuning the geometrical sizes of the structure, we tuned and induced the Fano dip in the visible range, while the dark and bright plasmon resonance extremes are blueshifted to shorter wavelengths dramatically. Considering the calculated transmission window, we quantified the effective refractive index for the structure, while the substance of the substrate material was varied. Using Si, GaP, and InP semiconductors as substrate materials, we calculated and compared the corresponding figure of merit (FOM) for different regimes. The highest possible FOM was obtained for the GaP-Au-GaP negative-refractive-index metamaterial composed of ring/disk nanocavity heptamers as 62.4 at λ∼690 nm (arounnd the position of the Fano dip). Despite the outstanding symmetric nature of the suggested heptamer array, we provided sharp Fano dips by the appropriate tuning of the geometrical and chemical parameters. This study yields a method to employ ring/disk nanocavity heptamers as a negative-refractive-index metamaterial in designing highly accurate localization of surface plasmon resonance sensing devices and biochemical sensors.

Electromagnetic plasmon propagation and coupling through gold nanoring heptamers: a route to design optimized telecommunication photonic nanostructures.

In this work, a configuration of bulk gold nanorings with certain geometrical sizes has been utilized for designing efficient photonic subwavelength nanostructures. We verify that adjacent heptamers based on gold nanorings are able to couple and transport magnetic plasmon resonance along a nanoring array in chrysene and triphenylene molecule orientations. This magnetic resonance transmission is caused by an antiphase circular current through the heptamer arrays. An orientation model of nanoring heptamers helps us to provide efficient optical structures with a remarkable decay length and a trivial ratio of destructive interferences. Exploiting the robust magnetic plasmon resonance coupling effect between heptamers arrays, we would be able to propose a practical plasmonic waveguide, a Y-shaped optical power divider (splitter), and an ON/OFF router that is operating based on destructive and constructive interferences. The quality of power splitting has been discussed comprehensively and also, the effect of undesirable occasions on the functioning performance of the proposed router has been investigated numerically. Ultimately, we verify that employing heptamers based on gold nanorings leads us to propose efficient plasmonic nanostructures and devices that are able to work in the telecommunication spectrum.

Advances in Plasmonics and Nanophotonics.

Recent developments in subwavelength localization of light have paved the way of novel research directions in the field of optics, plasmonics, and nanophotonics [...].

Functionalized terahertz plasmonic metasensors: Femtomolar-level detection of SARS-CoV-2 spike proteins.

Effective and efficient management of human betacoronavirus severe acute respiratory syndrome (SARS)-CoV-2 virus infection i.e., COVID-19 pandemic, required sensitive and selective sensors with short sample-to-result durations for performing desired diagnostics. In this direction, one appropriate alternative approach to detect SARS-CoV-2 virus protein at low level i.e., femtomolar (fM) is exploring plasmonic metasensor technology for COVID-19 diagnostics, which offers exquisite opportunities in advanced healthcare programs, and modern clinical diagnostics. The intrinsic merits of plasmonic metasensors stem from their capability to squeeze electromagnetic fields, simultaneously in frequency, time, and space. However, the detection of low-molecular weight biomolecules at low densities is a typical drawback of conventional metasensors that has recently been addressed using toroidal metasurface technology. This research is focused on the fabrication of a miniaturized plasmonic immunosensor based on toroidal electrodynamics concept that can sustain robustly confined plasmonic modes with ultranarrow lineshapes in the terahertz (THz) frequencies. By exciting toroidal dipole mode using our quasi-infinite metasurface and a judiciously optimized protocol based on functionalized gold nanoparticles (AuNPs) conjugated with the specific monoclonal antibody specific to spike protein (S1) of SARS-CoV-2 virus onto the metasurface, the resonance shifts for diverse concentrations of the spike protein are monitored. Possessing molecular weight around ~76 kDa allowed to detect the presence of SARS-CoV-2 virus protein with significantly low as limit of detection (LoD) was achieved as ~4.2 fM. We envisage that outcomes of this research will pave the way toward the use of toroidal metasensors as practical technologies for rapid and precise screening of SARS-CoV-2 virus carriers, symptomatic or asymptomatic, and spike proteins in hospitals, clinics, laboratories, and site of infection.

Functional Charge Transfer Plasmon Metadevices.

Reducing the capacitive opening between subwavelength metallic objects down to atomic scales or bridging the gap by a conductive path reveals new plasmonic spectral features, known as charge transfer plasmon (CTP). We review the origin, properties, and trending applications of this modes and show how they can be well-understood by classical electrodynamics and quantum mechanics principles. Particularly important is the excitation mechanisms and practical approaches of such a unique resonance in tailoring high-response and efficient extreme-subwavelength hybrid nanophotonic devices. While the quantum tunneling-induced CTP mode possesses the ability to turn on and off the charge transition by varying the intensity of an external light source, the excited CTP in conductively bridged plasmonic systems suffers from the lack of tunability. To address this, the integration of bulk plasmonic nanostructures with optothermally and optoelectronically controllable components has been introduced as promising techniques for developing multifunctional and high-performance CTP-resonant tools. Ultimate tunable plasmonic devices such as metamodulators and metafilters are thus in prospect.

Increased Intraband Transitions in Smaller Gold Nanorods Enhance Light Emission.

Photoinduced light emission from plasmonic nanoparticles has attracted considerable interest within the scientific community because of its potential applications in sensing, imaging, and nanothermometry. One of the suggested mechanisms for the light emission from plasmonic nanoparticles is the plasmon-enhanced radiative recombination of hot carriers through inter- and intraband transitions. Here, we investigate the nanoparticle size dependence on the photoluminescence through a systematic analysis of gold nanorods with similar aspect ratios. Using single-particle emission and scattering spectroscopy along with correlated scanning electron microscopy and electromagnetic simulations, we calculate the emission quantum yields and Purcell enhancement factors for individual gold nanorods. Our results show strong size-dependent quantum yields in gold nanorods, with higher quantum yields for smaller gold nanorods. Furthermore, by determining the relative contributions to the photoluminescence from inter- and intraband transitions, we deduce that the observed size dependence predominantly originates from the size dependence of intraband transitions. Specifically, within the framework of Fermi's golden rule for radiative recombination of excited charge carriers, we demonstrate that the Purcell factor enhancement alone cannot explain the emission size dependence and that changes in the transition matrix elements must also occur. Those changes are due to electric field confinement enhancing intraband transitions. These results provide vital insight into the intraband relaxation in metallic nanoconfined systems and therefore are of direct importance to the rapidly developing field of plasmonic photocatalysis.

Magneto-plasmonic nanostars for image-guided and NIR-triggered drug delivery.

Smart multifunctional nanoparticles with magnetic and plasmonic properties assembled on a single nanoplatform are promising for various biomedical applications. Owing to their expanding imaging and therapeutic capabilities in response to external stimuli, they have been explored for on-demand drug delivery, image-guided drug delivery, and simultaneous diagnostic and therapeutic (i.e. theranostic) applications. In this study, we engineered nanoparticles with unique morphology consisting of a superparamagnetic iron oxide core and star-shaped plasmonic shell with high-aspect-ratio gold branches. Strong magnetic and near-infrared (NIR)-responsive plasmonic properties of the engineered nanostars enabled multimodal quantitative imaging combining advantageous functions of magnetic resonance imaging (MRI), magnetic particle imaging (MPI), photoacoustic imaging (PAI), and image-guided drug delivery with a tunable drug release capacity. The model drug molecules bound to the core-shell nanostars were released upon NIR illumination due to the heat generation from the core-shell nanostars. Moreover, our simulation analysis showed that the specific design of the core-shell nanostars demonstrated a pronounced multipolar plasmon resonance, which has not been observed in previous reports. The multimodal imaging and NIR-triggered drug release capabilities of the proposed nanoplatform verify their potential for precise and controllable drug release with different applications in personalized medicine.

Generation of magnetoelectric photocurrents using toroidal resonances: a new class of infrared plasmonic photodetectors.

The detection of photons by plasmonic subwavelength devices underpins spectroscopy, low-power wavelength division multiplexing for short-distance optical communication, imaging, and time-gated distance measurements. In this work, we demonstrate infrared light-sensing using toroidal dipole-resonant plasmonic multipixel meta-atoms. As a key factor, the toroidal dipolar mode is an extremely localized electromagnetic excitation independent of the conventional multipoles. The exquisite behavior of this mode enables significant enhancements in the localized electromagnetic field and absorption cross-section, which boost the field confinement at the metal-dielectric interfaces. The proposed novel approach offers an advanced photodetection of the incident light based on substantial confinement of electromagnetic fields in a tiny spot, giving rise to the generation of hot carriers and a large photocurrent. Using both n- and p-type silicon (Si) substrates, we exploited the free-carrier absorption advantage of p-type Si to devise a high-responsivity device. Our findings show an unprecedented performance for infrared plasmonic photodetectors with low noises, high detectivity and remarkable internal quantum efficiency (IQE). Moreover, the tailored photodetection device provides a significant linear dynamic range of 46 dB and a fast operation speed. Our narrowband infrared light sensing photodevice offers a promising approach for further research studies over the optoelectronic and plasmonic tools and paves a viable route for low-dimensional photonic systems.

Gated graphene island-enabled tunable charge transfer plasmon terahertz metamodulator.

Graphene-enhanced optoelectronic terahertz (THz) signal processing offers an exquisite potential for tailoring extreme-subwavelength platforms to develop tunable and highly-responsive photonic tools. In this study, we propose a hybrid graphene island-mediated THz metadevice to support tunable charge transfer plasmon (CTP) resonances. We show that bias variations in the gated graphene significantly change the metadevice transmittance at the CTP frequency, while the capacitive dipolar mode remains unchanged. Our numerical and experimental studies show that tuning the conductivity of the graphene islands between a cluster of metallic blocks provides an active and exotic control over the charge transition across the assembly. To experimentally prove the viability of our concept in a practical photonic application, we utilized the presented tunable system as a high modulation-depth THz modulator. This enabled us to facilitate a THz modulation speed of 19 µs and 21 µs for rising and falling durations, respectively, with a modulation depth of 72%.

Polydopamine-Stabilized Aluminum Nanocrystals: Aqueous Stability and Benzo[a]pyrene Detection.

Aluminum nanocrystals have emerged as an earth-abundant material for plasmonics applications. Al nanocrystals readily oxidize in aqueous-based solutions, however, transforming into highly stratified γ-AlOOH nanoparticles with a 700% increase in surface area in a matter of minutes. Here we show that by functionalizing Al nanocrystals with the bioinspired polymer polydopamine, their stability in aqueous media is dramatically increased, maintaining their integrity in aqueous solution for over 2 weeks with no discernible structural changes. Polydopamine functionalization also provides a molecular capture layer that enables the capture of polycyclic aromatic hydrocarbon pollutants in H2O samples and their detection by surface-enhanced Raman spectroscopy, when polydopamine-stabilized Al nanocrystal aggregates are used as substrates. This approach was used to detect a prime carcinogenic H2O pollutant, benzo[a]pyrene with a sensitivity in the sub part-per-billion range.

Extreme sensitive metasensor for targeted biomarkers identification using colloidal nanoparticles-integrated plasmonic unit cells.

Engineered terahertz (THz) plasmonic metamaterials have emerged as promising platforms for quick infection diagnosis, cost-effective and real-time pharmacology applications owing to their non-destructive and harmless interaction with biological tissues in both in vivo and in vitro assays. As a recent member of THz metamaterials family, toroidal metamaterials have been demonstrated to be supporting high-quality sharp resonance modes. Here we introduce a THz metasensor based on a plasmonic surface consisting of metamolecules that support ultra-narrow toroidal resonances excited by the incident radiation and demonstrate detection of an ultralow concertation targeted biomarker. The toroidal plasmonic metasurface was designed and optimized through extensive numerical studies and fabricated by standard microfabrication techniques. The surface then functionalized by immobilizing the antibody for virus-envelope proteins (ZIKV-EPs) for selective sensing. We sensed and quantified the ZIKV-EP in the assays by measuring the spectral shifts of the toroidal resonances while varying the concentration. In an improved protocol, we introduced gold nanoparticles (GNPs) decorated with the same antibodies onto the metamolecules and monitored the resonance shifts for the same concentrations. Our studies verified that the presence of GNPs enhances capturing of biomarker molecules in the surrounding medium of the metamaterial. By measuring the shift of the toroidal dipolar momentum (up to Δω~0.35 cm-1) for different concentrations of the biomarker proteins, we analyzed the sensitivity, repeatability, and limit of detection (LoD) of the proposed toroidal THz metasensor. The results show that up to 100-fold sensitivity enhancement can be obtained by utilizing plasmonic nanoparticles-integrated toroidal metamolecules in comparison to analogous devices. This approach allows for detection of low molecular-weight biomolecules (≈13 kDa) in diluted solutions using toroidal THz plasmonic unit cells.