Polarization dependence of second harmonic generation from plasmonic nanoprism arrays.

The second order nonlinear optical response of gold nanoprisms arrays is investigated by means of second harmonic generation (SHG) experiments and simulations. The polarization dependence of the nonlinear response exhibits a 6-fold symmetry, attributed to the local field enhancement through the excitation of the surface plasmon resonances in bow-tie nanoantennas forming the arrays. Experiments show that for polarization of the input light producing excitation of the plasmonic resonances in the bow-tie nanoantennas, the SHG signal is enhanced; this despite the fact that the linear absorption spectrum is not dependent on polarization. The results are confirmed by electrodynamic simulations which demonstrate that SHG is also determined by the local field distribution in the nanoarrays. Moreover, the maximum of SHG intensity is observed at slightly off-resonance excitation, as implemented in the experiments, showing a close relation between the polarization dependence and the structure of the material, additionally revealing the importance of the presence of non-normal electric field components as under focused beam and oblique illumination.

Circular dichroism enhancement in plasmonic nanorod metamaterials.

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 a 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 embedded in a transparent polymer. The metamaterial, being inherently achiral, enables optical activity enhancement or suppression. Unique properties of inherently achiral structures to tailor optical activities pave a way for flexible characterization of optical activity of molecules and nanocrystal-based compounds.

Controlling second-harmonic generation at the nanoscale with monolithic AlGaAs-on-AlOx antennas.

We review recent achievements in the field of nanoscale nonlinear AlGaAs photonics based on all-dielectric optical antennas. After discussing the motivation and main technological challenges for the development of an AlGaAs monolithic platform for χ (2) nonlinear nanophotonics, we present numerical and experimental investigations of the second-order nonlinear response and physical reasons for high efficiency of second-order nonlinear interactions in the AlGaAs nano-antennas. In particular, we emphasize the role of the dipolar resonances at the fundamental frequency and the multipolar resonances at the second harmonic wavelength. We also discuss second-harmonic generation directionality and show possible strategies to engineer the radiation pattern of nonlinear antennas.

Nonlocality-driven supercontinuum white light generation in plasmonic nanostructures.

Structured plasmonic metals are widely employed for achieving nonlinear functionalities at the nanoscale due to their ability to confine and enhance electromagnetic fields and strong, inherent nonlinearity. Optical nonlinearities in centrosymmetric metals are dominated by conduction electron dynamics, which at the nanoscale can be significantly affected by the nonlocal effects. Here we show that nonlocal corrections, being usually small in the linear optical response, define nonlinear properties of plasmonic nanostructures. Using a full non-perturbative time-domain hydrodynamic description of electron plasma under femtosecond excitation, we numerically investigate harmonic generation in metallic Archimedean nanospirals, revealing the interplay between geometric and nonlocal effects. The quantum pressure term in the nonlinear hydrodynamic model results in the emergence of fractional nonlinear harmonics leading to broadband coherent white-light generation. The described effects present a novel class of nonlinear phenomena in metallic nanostructures determined by nonlocality of the electron response.

Boundary effects in finite size plasmonic crystals: focusing and routing of plasmonic beams for optical communications.

Plasmonic crystals, which consist of periodic arrangements of surface features at a metal-dielectric interface, allow the manipulation of optical information in the form of surface plasmon polaritons. Here we investigate the excitation and propagation of plasmonic beams in and around finite size plasmonic crystals at telecom wavelengths, highlighting the effects of the crystal boundary shape and illumination conditions. Significant differences in broad plasmonic beam generation by crystals of different shapes are demonstrated, while for narrow beams, the propagation from a crystal onto the smooth metal film is less sensitive to the crystal boundary shape. We show that by controlling the boundary shape, the size and the excitation beam parameters, directional control of propagating plasmonic modes and their behaviour such as angular beam splitting, focusing power and beam width can be efficiently achieved. This provides a promising route for robust and alignment-independent integration of plasmonic crystals with optical communication components.

Refractive index sensing with hyperbolic metamaterials: strategies for biosensing and nonlinearity enhancement.

Metamaterials with hyperbolic dispersion based on metallic nanorod arrays provide a flexible platform for the design of bio- and chemical sensors and nonlinear devices, allowing the incorporation of functional materials into and onto the plasmonic metamaterial. Here, we have investigated, both analytically and numerically, the dependence of the optical response of these metamaterials on refractive index variations in commonly used experimental sensing configurations, including transmission, reflection, and total internal reflection. The strategy for maximising refractive index sensitivity for different configurations has been considered, taking into account contributions from the superstrate, embedding matrix, and the metal itself. It is shown that the sensitivity to the refractive index variations of the host medium is at least 2 orders of magnitude higher than to the ones originating from the superstrate. It is also shown that the refractive index sensitivity increases for higher-order unbound and leaky modes of the metamaterial sensor. The impact of the transducer's thickness was also analysed showing significant increase of the sensitivity for the thinner metamaterial layers (down to few 0.01 fraction of wavelength and, thus, requiring less analyte) as long as modes are supported by the structure. In certain configurations, both TE and TM-modes of the metamaterial transducer have comparable sensitivities. The results provide the basis for the design of new ultrasensitive chemical and biosensors outperforming both surface plasmon polaritons and localised surface plasmons based transducers.

Spin-orbit coupling in surface plasmon scattering by nanostructures.

The spin Hall effect leads to the separation of electrons with opposite spins in different directions perpendicular to the electric current flow because of interaction between spin and orbital angular momenta. Similarly, photons with opposite spins (different handedness of circular light polarization) may take different trajectories when interacting with metasurfaces that break spatial inversion symmetry or when the inversion symmetry is broken by the radiation of a dipole near an interface. Here we demonstrate a reciprocal effect of spin-orbit coupling when the direction of propagation of a surface plasmon wave, which intrinsically has unusual transverse spin, determines a scattering direction of spin-carrying photons. This spin-orbit coupling effect is an optical analogue of the spin injection in solid-state spintronic devices (inverse spin Hall effect) and may be important for optical information processing, quantum optical technology and topological surface metrology.

Shaping plasmon beams via the controlled illumination of finite-size plasmonic crystals.

Plasmonic crystals provide many passive and active optical functionalities, including enhanced sensing, optical nonlinearities, light extraction from LEDs and coupling to and from subwavelength waveguides. Here we study, both experimentally and numerically, the coherent control of SPP beam excitation in finite size plasmonic crystals under focussed illumination. The correct combination of the illuminating spot size, its position relative to the plasmonic crystal, wavelength and polarisation enables the efficient shaping and directionality of SPP beam launching. We show that under strongly focussed illumination, the illuminated part of the crystal acts as an antenna, launching surface plasmon waves which are subsequently filtered by the surrounding periodic lattice. Changing the illumination conditions provides rich opportunities to engineer the SPP emission pattern. This offers an alternative technique to actively modulate and control plasmonic signals, either via micro- and nano-electromechanical switches or with electro- and all-optical beam steering which have direct implications for the development of new integrated nanophotonic devices, such as plasmonic couplers and switches and on-chip signal demultiplexing. This approach can be generalised to all kinds of surface waves, either for the coupling and discrimination of light in planar dielectric waveguides or the generation and control of non-diffractive SPP beams.

Magnetic dipole radiation tailored by substrates: numerical investigation.

Nanoparticles of high refractive index materials can possess strong magnetic polarizabilities and give rise to artificial magnetism in the optical spectral range. While the response of individual dielectric or metal spherical particles can be described analytically via multipole decomposition in the Mie series, the influence of substrates, in many cases present in experimental observations, requires different approaches. Here, the comprehensive numerical studies of the influence of a substrate on the spectral response of high-index dielectric nanoparticles were performed. In particular, glass, perfect electric conductor, gold, and hyperbolic metamaterial substrates were investigated. Optical properties of nanoparticles were characterized via scattering cross-section spectra, electric field profiles, and induced electric and magnetic moments. The presence of substrates was shown to have significant impact on particle's magnetic resonances and resonant scattering cross-sections. Variation of substrate material provides an additional degree of freedom in tailoring optical properties of magnetic multipoles, important in many applications.

Manipulating polarization of light with ultrathin epsilon-near-zero metamaterials.

One of the basic functionalities of photonic devices is the ability to manipulate the polarization state of light. Polarization components are usually implemented using the retardation effect in natural birefringent crystals and, thus, have a bulky design. Here, we have demonstrated the polarization manipulation of light by employing a thin subwavelength slab of metamaterial with an extremely anisotropic effective permittivity tensor. Polarization properties of light incident on the metamaterial in the regime of hyperbolic, epsilon-near-zero, and conventional elliptic dispersions were compared. We have shown that both reflection from and transmission through λ/20 thick slab of the metamaterial may provide nearly complete linear-to-circular polarization conversion or 90° linear polarization rotation, not achievable with natural materials. Using ellipsometric measurements, we experimentally studied the polarization conversion properties of the metamaterial slab made of the plasmonic nanorod arrays in different dispersion regimes. We have also suggested all-optical ultrafast control of reflected or transmitted light polarization by employing metal nonlinearities.

Biosynthesis of luminescent quantum dots in an earthworm.

The synthesis of designer solid-state materials by living organisms is an emerging field in bio-nanotechnology. Key examples include the use of engineered viruses as templates for cobalt oxide (Co(3)O(4)) particles, superparamagnetic cobalt-platinum alloy nanowires and gold-cobalt oxide nanowires for photovoltaic and battery-related applications. Here, we show that the earthworm's metal detoxification pathway can be exploited to produce luminescent, water-soluble semiconductor cadmium telluride (CdTe) quantum dots that emit in the green region of the visible spectrum when excited in the ultraviolet region. Standard wild-type Lumbricus rubellus earthworms were exposed to soil spiked with CdCl(2) and Na(2)TeO(3) salts for 11 days. Luminescent quantum dots were isolated from chloragogenous tissues surrounding the gut of the worm, and were successfully used in live-cell imaging. The addition of polyethylene glycol on the surface of the quantum dots allowed for non-targeted, fluid-phase uptake by macrophage cells.

Broadband and broadangle SPP antennas based on plasmonic crystals with linear chirp.

Plasmonic technology relies on the coupling of light to surface electromagnetic modes on smooth or structured metal surfaces. While some applications utilise the resonant nature of surface polaritons, others require broadband characteristics. We demonstrate unidirectional and broadband plasmonic antennas with large acceptance angles based on chirped plasmonic gratings. Near-field optical measurements have been used to visualise the excitation of surface plasmon polaritons by such aperiodic structures. These weakly aperiodic plasmonic crystals allow the formation of a trapped rainbow-type effect in a two-dimensional geometry as surface polaritons of different frequencies are coherently excited in different locations over the plasmonic structure. Both the crystal's finite size and the finite lifetime of plasmonic states are crucial for the generation of broadband surface plasmon polaritons. This approach presents new opportunities for building unidirectional, broadband and broad-angle plasmonic couplers for sensing purposes, information processing, photovoltaic applications and shaping and manipulating ultrashort optical pulses.

Photonic signal processing on electronic scales: electro-optical field-effect nanoplasmonic modulator.

We develop a highly efficient approach for the modulation of photonic signals at the nanoscale, combining an ultrasubwavelength plasmonic guiding scheme with a robust electroabsorption effect in degenerate semiconductors. We numerically demonstrate an active electro-optical field-effect nanoplasmonic modulator with a revolutionary size of just 25 × 30 × 100 nm(3), providing signal extinction ratios as high as 2 at switching voltages of only 1 V. The design is compatible with complementary metal-oxide-semiconductor (CMOS) technology and allows low-loss insertion in standard plasmonic and Si-photonic circuitry.

Designed ultrafast optical nonlinearity in a plasmonic nanorod metamaterial enhanced by nonlocality.

All-optical signal processing enables modulation and transmission speeds not achievable using electronics alone. However, its practical applications are limited by the inherently weak nonlinear effects that govern photon-photon interactions in conventional materials, particularly at high switching rates. Here, we show that the recently discovered nonlocal optical behaviour of plasmonic nanorod metamaterials enables an enhanced, ultrafast, nonlinear optical response. We observe a large (80%) change of transmission through a subwavelength thick slab of metamaterial subjected to a low control light fluence of 7 mJ cm(-2), with switching frequencies in the terahertz range. We show that both the response time and the nonlinearity can be engineered by appropriate design of the metamaterial nanostructure. The use of nonlocality to enhance the nonlinear optical response of metamaterials, demonstrated here in plasmonic nanorod composites, could lead to ultrafast, low-power all-optical information processing in subwavelength-scale devices.

Hyperspectral imaging with scanning near-field optical microscopy: applications in plasmonics.

We present the realisation of near-field spectroscopic measurements with fibre-tip-based scanning near-field microscopy. It allows the simultaneous acquisition of near-field images in a broad spectral range (400 nm to 1000 nm), thus recovering local spectroscopic information. This technique is essential in order to understand the resonant interaction of light with nanostructured material as the far-field and near-field spectral response can differ significantly, e.g., in the case of plasmonic nanostructures. Several example applications of hyperspectral near-field imaging are given for visualisation of Bloch modes in plasmonic crystals and plasmon-assisted transmission through a slit.

Amplified spontaneous emission of surface plasmon polaritons and limitations on the increase of their propagation length.

Amplified spontaneous emission of surface plasmon polaritons (SPPs) at the interface of a resonant gain medium has been observed. The amplification is accompanied by significant spectral narrowing and limits the gain available for compensation of SPP propagation losses. The effect is similar to the deteriorating influence of amplified spontaneous emission in laser resonators.

Plasmonic nanorod metamaterials for biosensing.

Label-free plasmonic biosensors rely either on surface plasmon polaritons or on localized surface plasmons on continuous or nanostructured noble-metal surfaces to detect molecular-binding events. Despite undisputed advantages, including spectral tunability, strong enhancement of the local electric field and much better adaptability to modern nanobiotechnology architectures, localized plasmons demonstrate orders of magnitude lower sensitivity compared with their guided counterparts. Here, we demonstrate an improvement in biosensing technology using a plasmonic metamaterial that is capable of supporting a guided mode in a porous nanorod layer. Benefiting from a substantial overlap between the probing field and the active biological substance incorporated between the nanorods and a strong plasmon-mediated energy confinement inside the layer, this metamaterial provides an enhanced sensitivity to refractive-index variations of the medium between the rods (more than 30,000 nm per refractive-index unit). We demonstrate the feasibility of our approach using a standard streptavidin-biotin affinity model and record considerable improvement in the detection limit of small analytes compared with conventional label-free plasmonic devices.

Amplification of surface plasmon polaritons in the presence of nonlinearity and spectral signatures of threshold crossover.

We describe the effects of nonlinearity on propagation of surface plasmon polaritons (SPPs) at an interface between a metal and an amplifying medium of the externally pumped two-level atoms. Using Maxwell equations we derive the nonlinear dispersion law and demonstrate that the nonlinear saturation of the linear gain leads to formation of stationary SPP modes with the intensities independent from the propagation distance. Transition to the regime of stationary propagation is similar to the threshold crossover in lasers and leads to narrowing of the SPP spectrum.

Optical nonlocalities and additional waves in epsilon-near-zero metamaterials.

We analyze the optical properties of plasmonic nanorod metamaterials in the epsilon-near-zero regime and show, both theoretically and experimentally, that the performance of these composites is strongly affected by nonlocal response of the effective permittivity tensor. We provide the evidence of interference between main and additional waves propagating in the room-temperature nanorod metamaterials and develop an analytical description of this phenomenon. Additional waves are present in the majority of low-loss epsilon-near-zero structures and should be explicitly considered when designing applications of epsilon-near-zero composites, as they represent a separate communication channel.

Single-photon excitation of surface plasmon polaritons.

We provide the quantum-mechanical description of the excitation of surface plasmon polaritons on metal surfaces by single photons. An attenuated-reflection setup is described for the quantum excitation process in which we find remarkably efficient photon-to-surface plasmon wave-packet transfer. Using a fully quantized treatment of the fields, we introduce the Hamiltonian for their interaction and study the quantum statistics during transfer with and without losses in the metal.