We investigate the impact of the dipole-active modes formed via the mode-mixing of the dipole mode with higher-order surface plasmon modes of a nanoegg on the radiative decay rate and quantum yield of an excited molecule near the nanoegg. The Purcell factor, rate of power dissipation by the emitter, antenna efficiency of the nanoegg, as well as quantum yield enhancement of the emitter, were studied using the quasistatic approximation and the semiclassical theory of radiation, following the Gersten-Nitzan and Ford-Weber approaches. Compared to the concentric nanoshell, we show that the dielectric core-metallic shell nanoegg is a more efficient plasmonic nanoantenna for radiative decay rate enhancement of single emitters. The quantum yield of the emitter was found to be more enhanced near the nanoshell, while its emission rate was found to be more enhanced near the nanoegg.
Plasmonic gratings of different periodicities are fabricated on top of Silicon nanocrystals embedded in Silicon Dioxide. Purcell enhancements of up to 2 were observed, which matches the value from simulations. Plasmonic enhancements are observed for the first three orders of the plasmonic modes, with the peak enhancement wavelength varying with the periodicity. Biharmonic gratings are also fabricated to extract the enhanced emission from the first order plasmonic mode, resulting in enhancements with quality factors of up to 16.
A type of Tamm states inside metal-insulator-metal (MIM) waveguides is proposed. An impedance based transfer matrix method is adopted to study and optimize it. With the participation of the plasmonic Tamm states, fields could be enhanced twice: the ffirst is due to the coupling between a normal waveguide and a nanoscaled plasmonic waveguide and the second is due to the strong localization and field enhancement of Tamm states. As shown in our 2D coupling configuration, |E|^2 is enhanced up to 1050 times when 1550 nm light is coupled from an 300 nm Si slab waveguide into an 40 nm MIM waveguide.
Recent years have seen increased interest to plasmonic enhancement of nonlinear optical effects, yet there remains an uncertainty of what are the limits of this enhancement. We present a simple and physically transparent theory of plasmonic enhancement of third order nonlinear optical processes achieved in plasmonic structures and show that while huge enhancement of effective nonlinear index can be attained, the most relevant figure of merit, the of phase shift per one absorption length remains very low. This means that while on one hand nonlinear plasmonic materials are not well suitable for …
Efficient manipulation and long distance transport of single-photons is a key component in nanoscale quantum optics. In this letter, we study the emission properties of an individual light emitter placed into a nanofiber and coupled to a metallic nanoparticle. We find that plasmonic field enhancement together with the nanofiber optical confinement uniquely and synergistically contribute to an overall increase of emission rates as well as quantum yields.
We theoretically examine plasmonic resonance between two close metallic grains separated by a gap of width much less than the length of the incident electromagnetic wave. Resonance conditions are established and the electric field enhancement is found. Our general arguments are confirmed by analytic solution of the problem for simplest geometries. We discuss an extension of our results to more complex cases.
Recent experiments with film-coupled nanoparticles suggest that the impact of spatial dispersion is enhanced in plasmonic structures where high wavevector guided modes are excited. More advanced descriptions of the optical response of metals than Drude's are thus probably necessary in plasmonics. We show that even in classical prism coupler experiments, the plasmonic enhancement of spatial dispersion can be leveraged to make such experiments two orders of magnitude more sensitive. The realistic multilayered structures involved rely on layers that are thick enough to rule our any other phenomen…
We report that hybridizing semiconductor quantum dots with plasmonic metamaterial leads to a multi-fold intensity increase and narrowing of their photoluminescence spectrum. The luminescence enhancement is a clear manifestation of the cavity quantum electrodynamics Purcell effect that can be controlled by the metamaterial's design. This observation is an essential step towards understanding loss compensation in metamaterials with gain media and for developing metamaterial-enhanced gain media.
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 fie…
We investigate a short (~1.5μm) partially-corrugated tapered waveguide structure for mode coupling from a silicon micro-slab to a plasmonic nano-gap waveguide at the optical communication frequency. More than 80% transmission efficiency is reported numerically for the first time. The result indicates that the corrugated waveguide structure should not only be helpful for realizing full on-chip silicon plasmonic devices but also a good choice for mode coupling enhancement from dielectric waveguides to plasmonic waveguides. Meanwhile, we point out that the coupling mechanism reported here is diff…
We investigate the scattering and absorption properties of anisotropic metal-dielectric core-shell nanoparticles. It is revealed that the radially anisotropic dielectric layer can accelerate the evanescent decay of the localized resonant surface modes, leading to Q-factor and absorption rate enhancement. Moreover, the absorption cross section can be maximized to reach the single resonance absorption limit. We further show that such artificial anisotropic cladding materials can be realized by isotropic layered structures, which may inspire many applications based on scattering and absorption of…
We report the possibility to generate tremendous light-field enhancements within shallow nano-trenches made in a high index dielectric material, because of resonant behaviours reminiscent of what we get with sub-wavelength plasmonic cavities. The high quality factors are explained through a modal analysis and can be tuned with appropriate design rules. The thin dielectric void gratings here simulated could be a relevant alternative to plasmon-based devices for chemical sensing, or could be used as efficient wavelength-selective photo-absorbers by taking weakly absorbing materials.
Quasi-crystals are intriguing as they exhibit rotational symmetry and long range ordering but lack translational symmetry. 2-dimensional metal-dielectric patterns are interesting to make use of surface plasmon polariton (SPP) mediated local field enhancement and for near dispersionless SPP modes. In plasmonic crystals, the orientation and periodicity of the pattern dictate the polarization response and the discrete plasmon resonances while the interfaces define the plasmon dispersion. However, unique properties of plasmonic quasicrystals lead to polarization independence, designable k-space an…
We study how the collective effects of nanoparticles arranged in rectangular arrays influence their temporal plasmon response and field enhancement property. By systematically changing the lattice constant for arrays containing identical metal nanorods, we experimentally demonstrate how grating induced effects affect the position and, more importantly, the broadening of extinction spectra. We correlate these effects with the achievable field enhancement and the temporal duration of plasmon transients and formulate criteria for the generation of enhanced few-cycle localized plasmon oscillations…
Over the last few years, optical nanoantennas are continuously attracting interest owing to their ability to efficiently confine, localize resonance, and significantly enhanced electromagnetic fields at subwavelength scale. However, such strong confinement can be further enhanced by using an appropriate combination of optical nanoantenna and Slanted Bound states in the continuum cavities. Here, we propose to synergistically bridge the plasmonic nanoantenna and high optical quality-factor cavities to numerically demonstrate three orders of magnitude local intensity enhancement. The proposed hyb…
We couple photoluminescent semiconducting 7-atom wide armchair edge graphene nanoribbons to plasmonic nanoantenna arrays and demonstrate an enhancement of the photoluminescence and Raman scattering intensity of the nanoribbons by more than one order of magnitude. The increase in signal allows us to study Raman spectra with high signal-to-noise ratio. Using plasmonic enhancement we are able to detect the off-resonant Raman signals from the modified radial breathing-like mode (RBLM) due to physisorbed molecules, the 3rd order RBLM, and C-H vibrations. We find excellent agreement between data and…
We present an optical mode solver for a whispering gallery resonator coupled to an adjacent arbitrary shaped nano-particle that breaks the axial symmetry of the resonator. Such a hybrid resonator-nanoparticle is similar to what was recently used for bio-detection and for field enhancement. We demonstrate our solver by parametrically studying a toroid-nanoplasmonic device and get the optimal nano-plasmonic size for maximal enhancement. We investigate cases near a plasmonic resonance as well as far from a plasmonic resonance. Unlike common plasmons that typically benefit from working near their …
Plasmonically enhanced fluorescence is a widely studied and applied phenomenon, however only a comparative theoretical and experimental analyses of coupled fluorophores and plasmonic nanoresonators makes it possible to uncover, how this phenomenon can be controlled. A numerical optimization method was applied to design configurations that are capable of resulting in an enhancement of excitation and emission, moreover of both phenomena simultaneously in coupled Cy5 dye molecule and gold nanorod systems. Parametric sensitivity studies revealed, how the fluorescence enhancement depends on the mol…
We analytically study the spontaneous emission of a single optical dipole emitter in the vicinity of a plasmonic nanoshell, based on the Lorenz-Mie theory. We show that the fluorescence enhancement due to the coupling between optical emitter and sphere can be tuned by the aspect ratio of the core-shell nanosphere and by the distance between the quantum emitter and its surface. In particular, we demonstrate that both the enhancement and quenching of the fluorescence intensity are associated with plasmonic Fano resonances induced by near- and far-field interactions. These Fano resonances have as…
Unidirectional wave propagation in nonreciprocal structures enables exciting opportunities to control and enhance wave-matter interactions in extreme ways. Within this context, here we investigate the possibility of using terminated unidirectional plasmonic waveguides to enhance typically weak nonlinear effects by orders of magnitude. We theoretically demonstrate remarkable levels of electric field enhancement and confinement (field hot-spots) when the unidirectional waveguiding structure is terminated with a suitable boundary that fully stops the one-way mode. Such a large field enhancement, …
A plasmonic nanoantenna probed by a plane-polarized optical field in a medium with no gain materials can show zero absorption or even amplification, while exhibiting maximal polarizability. This occurs through coupling to an adjacent nanoantenna in a specially designed metamolecule, which is pumped by an orthogonal optical field with phase shift. The introduced scheme is a classical counterpart of an effect known in quantum optics as enhancement of the index of refraction (EIR). In contrary to electromagnetically induced transparency (EIT), where the medium is rendered highly dispersive at the…
The electromagnetic response of subwavelength wires coated with a graphene monolayer illuminated by a linearly polarized plane waves is investigated. The results show that the scattering and extintion cross-sections of the coated wire can be dramatically enhanced when the incident radiation resonantly excites localized surface plasmons. The enhancements occur for p--polarized incident waves and for excitation frequencies that correspond to complex poles in the coefficients of the multipole expansion for the scattered field. By dynamically tuning the chemical potential of graphene, the spectral…
The search for miniaturized components for nonlinear optical processes needs a way to overcome the efficiency loss due to the effective size reduction of the active medium. We investigate here a combination of a nanosized nonlinear dielectric crystal and metallic nanoantennas that benefits from both the intrinsic nonlinear conversion efficiency of the nonlinear medium and the local-field enhancement of plasmonic resonances in metallic nanostructures. Careful comparison between experiments and numerical simulations reveals that the observed 10 to 1000 fold enhancement in Second Harmonic Generat…
Cascaded optical field enhancement (CFE) can be realized in some specially designed multiscale plasmonic nanostructures, where the generation of extremely strong field at nanoscale volume is crucial for many applications, for example, surface enhanced Raman spectroscopy (SERS). Here, we propose a strategy of realizing a high-quality plasmonic nanoparticle-in-cavity (PIC) nanoantenna array, where strong coupling between a nanoparticle dark mode with a high order nanocavity bright mode can produce Fano resonance at a target wavelength. The Fano resonance can effectively boost the CFE in the PIC,…
We demonstrate theoretically and experimentally a two-scale architecture able to achieve giant field enhancement by simultaneously exploiting both the Rayleigh anomaly and localized surface plasmon resonance. Metallic oligomers composed of colloidal nanospheres are well-known for the ability to strongly enhance the near-field at their plasmonic resonance. However, due to intrinsic nonlocality of the dielectric response of the metals along with their inherent loss, the achievable field enhancement has an ultimate constraint. In this paper we demonstrate that combining plasmonic resonance enhanc…
Enhancement of magneto-optical effects in hybrid magneto-plasmonic systems has attracted considerable recent attention owing to their potential for building non-reciprocal nanophotonic devices. Quantitative understanding on the fundamental origin and contributing mechanisms for the enhancement is extremely crucial for optimizing applications. Here, we unravel the distinctly different physical origin of the giant enhancement of Faraday rotation and ellipticity in a hybrid magneto-plasmonic system, namely, waveguided magneto-plasmonic crystal for excitation with transverse electric (TE) and tran…
We consider a periodically gated two-dimensional electron system, with a central gate finger biased independently creating a tunable plasmonic cavity in a planar plasmonic crystal. We demonstrate that the plasmons resonantly excited in the periodic plasmonic lattice by incident terahertz radiation can strongly pump the cavity plasmon modes leading to a deep sub-wavelength concentration of terahertz energy with giant electric field enhancement factor up to 10000.
The transverse magneto-optical Kerr effect (TMOKE) in magnetite-based magneto-plasmonic crystals is studied experimentally and theoretically. We analyze angle-resolved TMOKE spectra from two types of structures where noble metallic stripes are incorporated inside a thin magnetite film or located on top of a homogeneous film. A multiple wide band enhancement of the TMOKE signal in transmission is demonstrated. The complex dielectric permittivity and gyration are experimentally determined using the ellipsometry technique as well as Faraday rotation and ellipticity measurements. The obtained para…
Plasmonic enhancement of nonlinear light-matter interaction can be achieved via dedicated optimization of resonant plasmonic modes that are spectrally matched to the different wavelengths involved in the particular nonlinear optical process. In this work, we investigate the generation and enhancement of broadband four-wave mixing (FWM) in a plasmonic azimuthally chirped grating (ACG). The azimuthally varying grating periodicity in an ACG offers a well-defined channel to mediate the near field and the far field over a broad range of wavelengths. However, the particular mechanism responsible for…
Plasmonic enhancement of nonlinear optical processes confront severe limitations arising from the strong dispersion of metal susceptibilities and small interaction volumes that hamper desirable phase-matching-like conditions. Maximizing nonlinear interactions in nanoscale systems require simultaneous excitation of resonant modes that spatially and constructively overlap at all wavelengths involved in the process. Here, we present a hybrid rectangular patch antenna design for optimal second harmonic generation (SHG) that is characterized by a non-centrosymmetric dielectric/ferroelectric materia…
Synthetic perovskites with photovoltaic properties open a new era in solar photovoltaics. Due to high optical absorption perovskite-based thin-film solar cells are usually considered as fully absorbing solar radiation on condition of ideal blooming. However, is it really so? The analysis of the literature data has shown that the absorbance of all photovoltaic pervoskites has the spectral hole at infrared frequencies where the solar radiation spectrum has a small local peak. This absorption dip results in the decrease of the optical efficiency of thin-film pervoskite solar cells by nearly 3% an…
Single molecule detection provides detailed information about molecular structures and functions, but it generally requires the presence of a fluorescent marker which can interfere with the activity of the target molecule or complicate the sample production. Detecting a single protein with its natural UV autofluorescence is an attractive approach to avoid all the issues related to fluorescence labelling. However, the UV autofluorescence signal from a single protein is generally extremely weak. Here, we use aluminum plasmonics to enhance the tryptophan autofluorescence emission of single protei…
Multiexcitonic transitions and emission of several photons per excitation comprise a very attractive feature of semiconductor quantum dots for optoelectronics applications. However, these higher-order radiative processes are usually quenched in colloidal quantum dots by Auger and other non-radiative decay channels. To increase the multiexcitonic quantum efficiency, several groups have explored plasmonic enhancement, so far with moderate results. By controlled positioning of individual quantum dots in the near field of gold nanocone antennas, we enhance the radiative decay rates of monoexcitons…
We investigate light scattering by coated spheres composed of a dispersive plasmonic core and a dielectric shell. By writing the absorption cross-section in terms of the internal electromagnetic fields, we demonstrate it is an observable sensitive to interferences that ultimately lead to the Fano effect. Specially, we show that unconventional Fano resonances, recently discovered for homogeneous spheres with large dielectric permittivities, can also occur for metallic spheres coated with single dielectric layers. These resonances arise from the interference between two electromagnetic modes wit…
Multiple surface plasmon-polariton (SPP) waves excited at the interface of a homogeneous isotropic metal and a chiral sculptured thin film (STF) impregnated with silver nanoparticles were theoretically assessed for the multiple-SPP-waves-based sensing of a fluid uniformly infiltrating the chiral STF. The Bruggemann homogenization formalism was used in two different modalities to determine the three principal relative permittivity scalars of the silver-nanoparticle-impregnated chiral STF infiltrated uniformly by the fluid. The dynamic sensitivity increased when silver nanoparticles were present…
We theoretically analyse photonic-plasmonic coupling between a high Q whispering gallery mode (WGM) resonator and a core-shell nanoparticle. Blue and red shifts of WGM resonances are shown to arise from crossing of the photonic and plasmonic modes. Level repulsion in the hybrid system is further seen to enable sensitivity enhancements in WGM sensors: maximal when the two resonators are detuned by half the plasmon linewidth. Approximate bounds are given to quantify possible enhancements. Criteria for reactive vs. resistive coupling are also established.
Recent investigations on optical nonlinearities of plasmonic materials suggest their responses may be even beyond the usual perturbative description. To better understand these surprisingly strong responses, we develop here a simple but general approach to describe the nonlinear optical response of plasmonic materials up to $n$th perturbation order. We apply the approach to understand spectral broadening occurring in resonant metasurfaces and investigate the enhancement of high-harmonic generation from multiply-resonant metasurfaces, predicting an over million-fold enhancement of higher harmon…
Optical activity is a fundamental phenomenon originating from the chiral nature of crystals and molecules. While intrinsic chiroptical responses of ordinary chiral materials to circularly polarized light are relatively weak, they can be enhanced by specially tailored nanostructures. Here, nanorod metamaterials, comprising a dense array of vertically aligned gold nanorods, is shown to provide significant enhancement of the circular dichroism response of an embedded material. A nanorod composite, acting as an artificial uniaxial crystal, is filled with chiral mercury sulfide nanocrystals embedde…
A tri-layer metamaterial perfect absorber of light, consisting of (Al/ZnS/Al) films with the top aluminium layer patterned as an array of circular disk nanoantennas, is investigated for resonantly enhancing Raman scattering from C-60 fullerene molecules deposited on the metamaterial. The metamaterial is designed to have resonant bands due to plasmonic and electromagnetic resonances at the Raman pump frequency (725 nm) as well as Stokes emission bands. The Raman scattering from C60 on the metamaterial with resonantly matched bands is measured to be enhanced by an order of magnitude more than fr…
We theoretically investigate several types of plasmonic slot waveguides for enhancing the measured signal in Raman spectroscopy, which is a consequence of electric field and Purcell factor enhancements, as well as an increase in light-matter interaction volume and the Raman signal collection efficiency. An intuitive methodology is presented for calculating the accumulated Raman enhancement factor of an ensemble of molecules in waveguide sensing, which exploits an analytical photon Green function expansion in terms of the waveguide normal modes, and we combine this with a quantum optics formali…
A plasmonic coupled-cavity system, which consists of a quarter-wave coupler cavity, a resonant Fabry-Perot detector nanocavity, and an off-resonant reflector cavity, is used to enhance the localization of surface plasmons in a plasmonic detector. The coupler cavity is designed based on transmission line theory and wavelength scaling rules in the optical regime, while the reflector cavity is derived from off-resonant resonator structures to attenuate transmission of plasmonic waves. We observed strong coupling of the cavities in simulation results, with an 86% improvement of surface plasmon loc…
Extreme mid-infrared field enhancement and anapoles in high-index plasmonic metamaterials
School of Physics and Astronomy, University of Birmingham（伯明翰大学物理与天文学学院）；NanoPhotonics Centre, Cavendish Laboratory, University of Cambridge（剑桥大学卡文迪许实验室纳米光子学中心）
By modifying the density of optical states at the location of an emitter, weak cavity-emitter coupling can enable a host of potential applications in quantum optics, from the development of low- threshold lasers to brighter single-photon sources for quantum cryptography. Although some of the first demonstrations of spontaneous emission modification occurred in metallic structures, it was only after the recent demonstration of cavity quantum electrodynamics effects in dielectric optical cavities that metal-based optical cavities were considered for quantum optics applications. Advantages of met…
Plasmonic nanoantenna is of promising applications in optical sensing, single-molecular detection, and enhancement of optical nonlinear effect, surface optical spectroscopy, photochemistry, photoemission, photovoltaics, etc. Here we show that in a carefully-designed dimer gap-antenna made by two metallic nanorods, the longitudinal plasmon antenna mode (AM) of bonding dipoles can compete with the transverse plasmonic cavity modes (CMs), yielding dramatically enhanced or suppressed scattering efficiency, depending on the CMs symmetry characteristics (e.g., the radial order n and the azimuthal qu…
Highly nonlinear optical processes, such as multiphoton photoemission, require high intensities, typically achieved with ultrashort laser pulses and, hence, were first observed with the advent of picosecond laser technology. An alternative approach for reaching the required field intensities is offered by localized optical resonances such as plasmons. Here, we demonstrate localized multiphoton photoemission from plasmonic nanostructures under continuous-wave illumination. We use synthesized plasmonic gold nanostars, which exhibit sharp tips with structural features smaller than 5 nm, leading t…
We introduce a modular approach for efficiently interfacing photonic integrated circuits with deep-sub-wavelength hybrid plasmonic functionality. We demonstrate that an off-the-shelf silicon-on-insulator waveguide can be post-processed into an integrated hybrid plasmonic circuit by evaporating a silica and gold nanolayer. The circuit consists of a plasmonic rotator and a nanofocusser module, which together result in nano-scale, nonlinear wavelength conversion. We experimentally characterize each module, and demonstrate an intensity enhancement of $>200$ in a calculated mode area of $50\,{\rm n…
Chemiphores are entities, which exhibit wide-band light emission without any external light source but just due to the chemical reaction resulting in the chemiluminescence effect. Since the chemiphores usually have low quantum efficiency, chemiluminescence is a weak optical effect. We found that plasmonic nanoparticles can efficiently enhance the peculiar effect of chemiluminescence due to the acceleration of the radiative decay of the chemiphore excited state which, in turn, enlarges the chemiluminescence yield. Correspondingly, plasmonic nanoparticles are nanoparticles with sub-wavelength si…
Enhancement and suppression of nonlinear processes in coupled systems of plasmonic converters and quantum emitters are well-studied theoretically, numerically and experimentally, in the past decade. Here, in difference, we explicitly demonstrate --with a single equation-- how the presence of a Fano resonance leads to cancellation of nonresonant terms in a four-wave mixing process. Cancellation in the denominator gives rise to enhancement in the nonlinearity. The explicit demonstration, we present here, guides us to the method for achieving more and more orders of magnitude enhancement factors …
Localized surface plasmon polaritons in conducting structures give rise to enhancements of electromagnetic local fields and extinction efficiencies. Resonant conducting structures are conventionally fabricated with a fixed geometry that determines their plasmonic response. Here, we challenge this conventional approach by demonstrating the photo-generation of plasmonic materials (THz plasmonic antennas) on a flat semiconductor layer by the structured optical illumination through a spatial light modulator. Free charge carriers are photo-excited only on selected areas, which enables the definitio…
Plasmonic antennas are key elements to control the luminescence of quantum emitters. However, the antenna's influence is often hidden by quenching losses. Here, the luminescence of a quantum dot coupled to a gold dimer antenna is investigated. Detailed analysis of the multiply excited states quantifies the antenna's influence on the excitation intensity and the luminescence quantum yield separately.
It is now well established that, due to excitation of localized surface plasmon resonances in plasmonic nanosystems, the electric field from an external irradiation source is greatly amplified in their vicinity. Surface plasmon mediated electric field amplification near plasmonic nanosystems is of vital importance for; light absorption enhancement of solar cells, molecular detection using surface enhanced Raman spectroscopy, proximity measurement of biological macromolecules such as proteins, lipids and nucleic acids using plasmon enhanced FRET, cancer therapy using photothermal effects, just …
Control of nonlinear response of nanostructures via path interference effects, i.e. Fano resonances, has been studied extensively. In such materials, a frequency conversion process which takes place near a hot spot has been considered. Here, we study a different case. The frequency conversion process takes place along the body of a nonlinear crystal. Metal nanoparticle-quantum emitter dimers control the down-conversion process, taking place throughout the crystal body, via introducing interfering conversion paths. Dimers behave as interaction centers. We show that a 2 order of magnitude enhanc…
We present a new design of plasmonic nanoantenna with a slant gap for optical chirality engineering. At resonance, the slant gap provides highly enhanced electric field parallel to external magnetic field with a phase delay of 90 degree, resulting in enhanced optical chirality. We show by numerical simulations that upon linearly polarized excitation our achiral nanoantenna can generate near field with enhanced optical chirality that can be tuned by the slant angle and resonance condition. Our design can be easily realized and may find applications in circular dichroism enhancement.
