Anapole States in Gap-Surface Plasmon Resonators.

Anapole states associated with the destructive interference between dipole and toroidal moments result in suppressed scattering accompanied by strongly enhanced near fields. In this work, we comprehensively examine the anapole state formation in metal-insulator-metal configurations supporting gap surface-plasmon (GSP) resonances that are widely used in plasmonics. Using multipole decomposition, we show that in contrast to the common case of dielectric particles with out-of-phase superposition of electric and toroidal dipoles anapole states in GSP resonators are formed due to the compensation of magnetic dipole moments. Unlike anapole states in dielectric particles, magnetic anapole states in GSP resonator does not provide a pronounced suppression of scattering, but it features huge electric field enhancement, which we verify by numerical simulations and two-photon luminescence measurements. This makes the GSP resonator configuration very promising for use in a wide range of applications, ranging from nonlinear harmonic generation to absorption enhancement and sensing.

Highly Stable Monocrystalline Silver Clusters for Plasmonic Applications.

Plasmonic sensor configurations utilizing localized plasmon resonances in silver nanostructures typically suffer from the rapid degradation of silver under ambient atmospheric conditions. In this work, we report on the fabrication and detailed characterization of ensembles of monocrystalline silver nanoparticles (NPs), which exhibit a long-term stability of optical properties under ambient conditions without any protective treatments. Ensembles with different densities (surface coverages) of size-selected NPs (mean diameters of 12.5 and 24 nm) on quartz substrates are fabricated using the cluster-beam technique and characterized by linear spectroscopy, two-photon-excited photoluminescence, surface-enhanced Raman scattering microscopy, and transmission electron, helium ion, and atomic force microscopies. It is found that the fabricated ensembles of monocrystalline silver NPs preserve their plasmonic properties (monitored with optical spectroscopy) and strong field enhancements (revealed by surface-enhanced Raman spectroscopy) at least 5 times longer as compared to chemically synthesized silver NPs with similar sizes. The obtained results are of high practical relevance for the further development of sensors, resonators, and metamaterials utilizing the plasmonic properties of silver NPs.

Enhancement of two-photon photoluminescence and SERS for low-coverage gold films.

Electromagnetic field enhancement (FE) effects occurring in thin gold films 3-12-nm are investigated with two-photon photoluminescence (TPL) and Raman scanning optical microscopies. The samples are characterized using scanning electron microscopy images and linear optical spectroscopy. TPL images exhibit a strong increase in the level of TPL signals for films thicknesses 3-8-nm, near the percolation threshold. For some thicknesses, TPL measurements reveal super-cubic dependences on the incident power. We ascribe this feature to the occurrence of very strongly localized and enhanced electromagnetic fields due to multiple light scattering in random nanostructures that might eventually lead to white-light generation. Raman images exhibit increasing Raman signals when decreasing the film thickness from 12 to 6-nm and decreasing signal for the 3-nm-film. This feature correlates with the TPL observations indicating that highest FE is to be expected near the percolation threshold.

Plasmonic channel waveguides in random arrays of metallic nanoparticles.

We report detailed characterization of surface plasmon-polariton guiding along 1-, 1.5- and 2-µm-wide channels in high-density (~75 µm-2) random arrays of gold 70-nm-high and 50-nm-wide nanoparticles fabricated on a 70-nm-thin gold film supported by a 170-µm-thick silica substrate. The mode propagation losses, effective index dispersion, and scattering parameters are characterized using leakage-radiation microscopy, in direct and Fourier planes, in the wavelength range of 740-840 nm. It is found that the mode supported by 2-µm-wide channels propagates over > 10 µm in straight waveguides, with the corresponding S-bends and Y-splitters functioning reasonably well. The results show that the SPP waves can efficiently be guided by narrow scattering-free channels cut through randomly corrugated surface regions. The potential of this waveguiding mechanism is yet to be fully explored by tuning the scattering mean-free path and localization length via the density and size of random nanoparticles. Nevertheless, the results obtained are encouraging and promising diverse applications of these waveguide components in plasmonic circuitry.

On-chip detection of radiation guided by dielectric-loaded plasmonic waveguides.

We report a novel approach for on-chip electrical detection of the radiation guided by dielectric-loaded surface plasmon polariton waveguides (DLSPPW) and DLSPPW-based components. The detection is realized by fabricating DLSPPW components on the surface of a gold (Au) pad supported by a silicon (Si) substrate supplied with aluminum pads facilitating electrical connections, with the gold pad being perforated in a specific location below the DLSPPWs in order to allow a portion of the DLSPPW-guided radiation to leak into the Si-substrate, where it is absorbed and electrically detected. We present two-dimensional photocurrent maps obtained when the laser beam is scanning across the gold pad containing the fabricated DLSPPW components that are excited via grating couplers located at the DLSPPW tapered terminations. By comparing photocurrent signals obtained when scanning over a DLSPPW straight waveguide with those related to a DLSPPW racetrack resonator, we first determine the background signal level and then the corrected DLSPPW resonator spectral response, which is found consistent with that obtained from full wave numerical simulations. The approach developed can be extended to other plasmonic waveguide configurations and advantageously used for rapid characterization of complicated plasmonic circuits.

Tuning surface plasmons in interconnected hemispherical Au shells.

We present a new approach for making interconnected hemispherical shells by stripping Au from templates of anodized aluminum, where the metal thickness can be adjusted without affecting the outer radius of curvature, film roughness and the sharpness of the hemisphere contact areas. This provides increased understanding of the surface plasmon resonances (SPRs) observed for Film-On-Nanospheres (FONs) by decoupling these parameters, which are coupled in the case of FONs. Investigating the influence of the shell thicknesses on the spectral positions of SPRs for FONs involves a dielectric core with a fixed radius encased by a metal film with adjustable thickness. By performing linear reflection spectroscopy, we demonstrate a wide tunability of the SPR by tailoring the inner hemisphere diameter, while keeping the outer diameter fixed. Deposition of extra Au on top of thick, previously stripped hemispherical shells isolates optical response contributions from Au grain- and island-mediated roughness, and unsharpening contact areas in form of decreasing LSPR quality factor. Two-photon luminescence scanning optical microscopy of shells with different thicknesses, applying several different laser wavelengths, is exploited to map local electromagnetic hot spots and correlate the high field enhancements with the linear reflection spectroscopy measurements.

Polarization-resolved two-photon luminescence microscopy of V-groove arrays.

Using two-photon luminescence (TPL) microscopy and local reflection spectroscopy we investigate electromagnetic field enhancement effects from a µm-sized composition of 450-nm-deep V-grooves milled by focused ion beam in a thick gold film and assembled to feature, within the same structure, individual V-grooves as well as one- and two-dimensional 300-nm-period arrays of, respectively, parallel and crossed V-grooves. We analyze TPL signal levels obtained at different spatial locations and with different combinations of excitation and detection polarizations, discovering that the TPL emitted from the V-grooves is polarized in the direction perpendicular to that of the V-grooves. This feature implies that the TPL occurs solely in the form of (p-polarized) surface plasmon modes and originates therefore from the very bottom of V-grooves, where no photonic modes exist. Implications of the results obtained to evaluation of local field enhancements using TPL microscopy, especially when investigating extended structures exhibiting different radiation channels, are discussed.

Extraordinary optical transmission enhanced by nanofocusing.

We demonstrate that the phenomenon of extraordinary optical transmission (EOT) through perforated metal films can be further boosted up by utilizing nanofocusing of radiation in tapered slits. For one-dimensional arrays of tapered slits in optically thick suspended gold films, we show that the maximum transmission at resonance is achieved for taper angles in the range of 7-10 degrees increasing significantly in comparison with the transmission by straight slits. Transmission spectroscopy of fabricated 500 and 700 nm period tapered slits in a 180 nm thick gold film on a glass substrate demonstrates the enhanced EOT with the resonance transmission being as high as approximately 0.18 for the filling ratio of approximately 0.13 and showing good correspondence with theoretical results. It is also shown that the enhanced transmission can be achieved with either weak (2.5%) or strong (43%) reflection depending on the direction of light (normal) incidence.

Resonant plasmon nanofocusing by closed tapered gaps.

We study radiation nanofocusing by closed tapered gaps, i.e. metal V-grooves, under normal illumination, and discover that the local field inside a groove can be resonantly enhanced due to interference of counter-propagating gap plasmons. Considering V-grooves milled in gold, we analyze this phenomenon theoretically, deriving an analytic expression for the resonance condition and predicting more than 550-fold intensity enhancements at resonance, and observe it experimentally with two-photon photoluminescence microscopy, demonstrating more than 100-fold intensity enhancements.

Two-photon luminescence microscopy oflarge-area gold nanostructures on templates of anodized aluminum.

Using linear reflection spectroscopy and far-field two-photon luminescence (TPL) scanning optical microscopy, we characterize highly enhancing, large-area gold nanostructures formed on porous templates made by anodization of aluminum with either oxalic acid or phosphoric acid. These templates are formed by a newly developed, stepwise technique making use of protective top oxide layers facilitating continuously tunable interpore distances. The upper, porous alumina layers are subsequently removed and the remaining embossed barrier layer is used as template for the sputtered gold, where the density of gold particles covering the sample is adjusted by regulating the sputtering conditions. We observe spatially averaged field intensity enhancement (FE) factors of up to ~5.210(2) and bright spots in the TPL-images exhibiting maximum FE factors of up to approximately 1410(2) which is the largest estimated FE from any hitherto examined structures with our setup. We relate this large-area massive FE to constructive interference of surface plasmon (SP) polaritons scattered from the densely packed, randomly distributed gold particles and directly correlate this particle density with the strong and broad SP resonances as well as the magnitude of the FE factors. The average FE and the position of high enhancements in the TPL-images are dictated by the excitation wavelength, and the structures could evidently serve as versatile structures facilitating practical molecular sensing.

Surface enhanced Raman imaging: periodic arrays and individual metal nanoparticles.

Surface enhanced Raman scattering (SERS) from Rhodamine 6G homogenously adsorbed on both periodic arrays of and individual gold nanoparticles is investigated using high-resolution Raman imaging with polarized excitation. Rectangular 50-nm-high nanoparticles of different sizes chosen to ensure the presence of localized surface plasmon resonances close to the 532-nm excitation wavelength are fabricated with electron-beam lithography on the surface of a smooth gold film and arranged both individually (i.e., placed sufficiently far apart) and in 740-nm-period arrays. Linear reflection spectra and high-resolution Raman images obtained from arrays of nanoparticles are compared revealing good correspondence in the spectral dependences of reflection and local SERS enhancements (measured at the top of nanoparticles). The latter are related to those observed with individual nanoparticles. The results obtained emphasize the importance and quantify the influence of particle dimensions, polarized excitation, collctive resonances and SERS locations.

Laser Writing of Bright Colors on Near-Percolation Plasmonic Reflector Arrays.

Coloration by surface nanostructuring has attracted a great deal of attention by the virtue of making use of environment-friendly recyclable materials and generating nonbleaching colors. Recently, it was found possible to delegate the task of color printing to laser postprocessing that modifies carefully designed and fabricated nanostructures. Here we take the next crucial step in the development of structural color printing by dispensing with preformed nanostructures and using instead near-percolation metal films atop dielectric-metal sandwiches, that is, near-percolation plasmonic reflector arrays. Scanning rapidly (∼20 µm/s) across 4 nm-thin island-like gold films supported by 30 nm-thin silica layers atop 100 nm-thick gold layers with a strongly focused Ti-sapphire laser beam, while adjusting the average laser power from 1 to 10 mW, we produce bright colors varying from green to red by laser-heating-induced merging and reshaping of gold islands. Selection of strongly heated islands and their reshaping, both originating from excitation of plasmonic resonances, are strongly influenced by the polarization direction of laser illumination, so that the colors produced are well pronounced only when viewed with the same polarization. Conversely, the laser color writing with circular polarizations results in bright polarization-independent color images. The fabrication procedure for near-percolation reflector arrays is exceedingly simple and scalable to mass production, while the laser-induced modification occurs inherently with the subwavelength resolution. This combination of features makes the approach developed for laser color writing readily amenable for practical implementation and use in diverse applications ranging from nanoscale patterning for security marking to large-scale color printing for decoration.

Two-photon mapping of localized field enhancements in thin nanostrip antennas.

Resonant scattering and local field enhancements by 11-nm-thin gold nanostrip antennas due to constructive interference of counter propagating slow surface plasmon polaritons is investigated. We characterize nanostrips of widths between 50-530 nm using both reflection spectroscopy and nonlinear scanning optical microscopy, in which two-photon-excited photoluminescence (TPL) excited with a strongly focused laser beam at the wavelength 745 nm is detected. We use TPL images to map the local field enhancements from individual nanostrips at a resolution of 0.35 microm and compare results with theoretical calculated reflection spectra, enhancement levels and field distributions across the strip.

Localized field enhancements in fractal shaped periodic metal nanostructures.

Fractal shaped structures formed with a 100-nm-period square lattice of gold nanoparticles placed on a gold film are characterized by using far-field nonlinear scanning optical microscopy, in which two-photon photoluminescence (TPL) excited with a strongly focused laser beam (in the wavelength range of 730 - 790 nm) is detected. The TPL images recorded for all wavelengths exhibit diffraction-limited (~ 0.6 mum) bright spots corresponding to the field intensity enhancement of up to 150, whose positions are dictated by the incident light wavelength and polarization. We relate these field enhancements to the occurrence of constructive interference of surface plasmons (SPs), which are excited by the incident radiation (due to scattering by nanoparticles) and partially reflected by fractal shaped boundaries due to a difference in the SP effective index at a flat and periodically corrugated gold surface. The conjecture on SP index difference is verified with observations (using leakage radiation microscopy) of SP focusing by circular and waveguiding by rectangular areas filled with periodically arranged nanoparticles.

Optical reconfiguration and polarization control in semi-continuous gold films close to the percolation threshold.

Controlling and confining light by exciting plasmons in resonant metallic nanostructures is an essential aspect of many new emerging optical technologies. Here we explore the possibility of controllably reconfiguring the intrinsic optical properties of semi-continuous gold films, by inducing permanent morphological changes with a femtosecond (fs)-pulsed laser above a critical power. Optical transmission spectroscopy measurements show a correlation between the spectra of the morphologically modified films and the wavelength, polarization, and the intensity of the laser used for alteration. In order to understand the modifications induced by the laser writing, we explore the near-field properties of these films with electron energy-loss spectroscopy (EELS). A comparison between our experimental data and full-wave simulations on the exact film morphologies hints toward a restructuring of the intrinsic plasmonic eigenmodes of the metallic film by photothermal effects. We explain these optical changes with a simple model and demonstrate experimentally that laser writing can be used to controllably modify the optical properties of these semi-continuous films. These metal films offer an easy-to-fabricate and scalable platform for technological applications such as molecular sensing and ultra-dense data storage.

Plasmonic black metals via radiation absorption by two-dimensional arrays of ultra-sharp convex grooves.

Plasmonic black surfaces formed by two-dimensional arrays of ultra-sharp convex metal grooves, in which the incident radiation is converted into gap surface plasmon polaritons (GSPPs) and subsequently absorbed (via adiabatic nanofocusing), are fabricated and investigated experimentally for gold, nickel, and palladium, using scanning electron microscopy, optical microscopy, and reflection spectroscopy for their characterization. Absolute reflectivity spectra obtained for all fabricated arrays demonstrate very efficient and broadband absorption of unpolarized light exceeding the level of 95%, averaged over the investigated wavelength range of 400-985 nm. The highest averaged absorption level (~97%) is achieved with 250-nm-period arrays in palladium that also has the highest melting temperature (~1552°C), promising thereby potential applications for broadband absorption, e.g., within thermophotovoltaics. For one-dimensional arrays, GSPPs are excited only with the electric field polarized perpendicular to the groove orientation, resulting in 94-96% absorption of the appropriately polarized light for the arrays in nickel and palladium while featuring practically flat surface reflectivity spectra for the orthogonal polarization. The largest ratio (~10.7) between averaged reflectivities for orthogonal polarizations is achieved with the groove arrays in palladium, pointing thereby towards applications as broadband and low-dispersion linear polarizers operating in reflection, e.g., within ultra-fast optics.

Optical spectroscopy of single Si nanocylinders with magnetic and electric resonances.

Resonant electromagnetic properties of nanoparticles fabricated from high-index semiconductor or dielectric materials are very promising for the realization of novel nanoantennas and metamaterials. In this paper we study optical resonances of Si nanocylinders located on a silica substrate. Multipole analysis of the experimental scattering spectra, based on the decomposed discrete dipole approximation, confirms resonant excitation of electric and magnetic dipole modes in the Si nanocylinders. Influences of light polarization and incident angle on the scattering properties of the nanocylinders are studied. It is shown that the dependence of resonant excitation of the electric and magnetic modes in the nanocylinders on incident angle and polarization of light allows controlling and manipulating the scattered light in this system. The demonstrated properties of Si nanocylinders can be used for the realization of dielectric metasurfaces with different functional optical properties.

Identification of abnormal stem cells using Raman spectroscopy.

The clinical use of stem cells in cell-based therapeutics for degenerative diseases requires development of criteria for defining normal stem cells to ensure safe transplantation. Currently, identification of abnormal from normal stem cells is based on extensive ex vivo and in vivo testing. Raman microscopy is a label-free method for rapid and sensitive detection of changes in cells' bio-molecular composition. Here, we report that by using Raman spectroscopy, we were able to map the distribution of different biomolecules within 2 types of stem cells: adult human bone marrow-derived stromal stem cells and human embryonic stem cells and to identify reproducible differences in Raman's spectral characteristics that distinguished genetically abnormal and transformed stem cells from their normal counterparts. Raman microscopy can be prospectively employed as a method for identifying abnormal stem cells in ex vivo cultures prior to clinical transplantation.

Plasmonic black gold by adiabatic nanofocusing and absorption of light in ultra-sharp convex grooves.

Excitation of localized and delocalized surface plasmon resonances can be used for turning excellent reflectors of visible light, such as gold and silver, into efficient absorbers, whose wavelength, polarization or angular bandwidths are however necessarily limited owing to the resonant nature of surface plasmon excitations involved. Nonresonant absorption has so far been achieved by using combined nano- and micro-structural surface modifications and with composite materials involving metal nanoparticles embedded in dielectric layers. Here we realize nonresonant light absorption in a well-defined geometry by using ultra-sharp convex metal grooves via adiabatic nanofocusing of gap surface plasmon modes excited by scattering off subwavelength-sized wedges. We demonstrate experimentally that two-dimensional arrays of sharp convex grooves in gold ensure efficient (>87%) broadband (450-850 nm) absorption of unpolarized light, reaching an average level of 96%. Efficient absorption of visible light by nanostructured metal surfaces open new exciting perspectives within plasmonics, especially for thermophotovoltaics.

Direct observation of localized second-harmonic enhancement in random metal nanostructures.

Second harmonic (SH) scanning optical microscopy in reflection is used to image the gold film surface covered with randomly placed scatterers. SH images obtained with a tightly focused tunable (750-830 nm) laser beam show small (approximately 0.7 microm) and very bright (approximately 10(3) times the background) spots, whose locations depend on the wavelength and polarization of light. Comparing SH and fundamental harmonic (FH) images, we conclude that the localized SH enhancement occurs due to the overlap of FH and SH eigenmodes. The probability density function of the SH signal is found to follow the power-law dependence.