Surface-plasmon hopping along coupled coplanar cavities

International audience; We report on surface-plasmon propagation along coupled coplanar cavities periodically distributed in an otherwise unperturbed plasmonic crystal. We show that the dispersion of particular Bloch modes can exhibit multiple energy gaps that can be adjusted by choosing the cavity size. For resonant sizes, the composite crystals composed of juxtaposed cavities can support plasmon modes at frequencies within the gap of the unperturbed grating. In this case, we demonstrate that the surface-plasmon propagation relies on a hopping mechanism.

Nonlinear photon-assisted tunneling transport in optical gap antennas.

International audience; We introduce strongly coupled optical gap antennas to interface optical radiation with current-carrying electrons at the nanoscale. The transducer relies on the nonlinear optical and electrical properties of an optical gap antenna operating in the tunneling regime. We discuss the underlying physical mechanisms controlling the conversion involving d-band electrons and demonstrate that a simple two-wire optical antenna can provide advanced optoelectronic functionalities beyond tailoring the electromagnetic response of a single emitter. Interfacing an electronic command layer with a nanoscale optical device may thus be facilitated by the optical rectennas discussed here.

Measuring the magnetic dipole transition of single nanorods by spectroscopy and Fourier microscopy

International audience; Rare-earth doped nanocrystals possess optical transitions with significant either electric or magnetic dipole characters. They are of considerable interest for understanding and engineering light-matter interactions at the nanoscale with numerous applications in nanophotonics. Here, we study the 5 D 0 → 7 F 1 transition dipole vector in individual NaYF 4 : Eu 3+ nanorod crystals by Fourier and confocal micro-scopies. A single-crystal host matrix leads to narrow emission lines at room temperature that permit separation of the Stark sublevels resulting from the crystal-field splitting. We observe a fully magnetic transition and low variability of the transition dipole …

Preface to Volume 3

Sorting of Enhanced Reference Raman Spectra of a Single Amino Acid Molecule

In this contribution, we report the identification of the principal reference Raman spectra of a single cystein molecule. To that purpose, we design an active Surface Enhanced Raman Spectroscopy (SERS) template based on surfactant-less Chebyshev nanoparticles operating in a microfluidic platform. A principal component analysis is obtained from fluctuating spectra to sort the reference spectra of cystein. The assignment of Raman bands brings new insight into the conformation of an amino acid adsorbed onto gold nanoparticle.

Leakage radiation microscopy of surface plasmon coupled emission: investigation of gain-assisted propagation in an integrated plasmonic waveguide.

International audience; Using a single-mode dielectric-loaded surface plasmon polariton waveguide doped with quantum dots, we were able to slightly increase the propagation length of the mode by stimulated emission of plasmon. We analyse the amplification phenomenon in the visible range by combining leakage radiation microscopy and surface plasmon coupled emission techniques.

Mapping surface plasmon propagation by collection-mode near-field microscopy

Surface plasmon propagation along striped Gold structures has been investigated by collection-mode near-field microscopy, leading to map the field intensity at the structure surface and to assess the system behavior at the nanoscale.

Delocalization of Nonlinear Optical Responses in Plasmonic Nanoantennas

Remote excitation and emission of two-photon luminescence and second-harmonic generation are observed in micrometer long gold rod optical antennas upon local illumination with a tightly focused near-infrared femtosecond laser beam. We show that the nonlinear radiations can be emitted from the entire antenna and the measured far-field angular patterns bear the information regarding the nature and origins of the respective nonlinear processes. We demonstrate that the nonlinear responses are transported by the propagating surface plasmon at excitation frequency, enabling thereby polariton-mediated tailoring and design of nonlinear responses.

Excitation of surface plasmon polaritons guided mode by Rhodamine B molecules doped in PMMA stripe

In this letter we show the inclusion of Rhodamine B molecules (RhB) inside a dielectric-loaded surface plasmon waveguide enables for a precise determination of its optical characteristics. The principle relies on the coupling of the fluorescence emission of the dye to plasmonic waveguided modes allowed in of the structure. Using leakage radiation microscopy in real and reciprocal spaces, we measure the propagation constant of the mode and as well as their attenuation length.

An Electrical Tuner to Command Optical NanoAntennas

Optical antennas are passive device where fabrication designs decide operating frequency, gain and emission diagram. By introducing an electrically controllable load medium for the antenna, these characteristics can be externally controlled.

Ultrafast hybrid plasmonics

Abstract We review our recent studies of electromagnetic coupling and associated temporal dynamics of molecular excitations with plasmonic resonances supported by either localized or extended planar geometries. We focus on coherent interactions between plasmon resonances and molecular excitations, which are experimentally challenging due to the very short (∼10–100 fs) coherence times of plasmons. Recent experimental results and theoretical analysis for observing and controlling coherences between molecular excitations and plasmonic polarizations are shown. Advances will explore new directions in ultrafast coherent control of molecular excited states and energy dissipation processes, as well…

Differential method for modeling dielectric-loaded surface plasmon polariton waveguides

This paper demonstrates the efficiency of the differential method, a conventional grating theory, to investigate dielectric loaded surface plasmon polariton waveguides (DLSPPWs), known to be a potential solution for optical interconnects. The method is used to obtain the mode effective indices (both real and imaginary parts) and the mode profiles. The results obtained with the differential method are found to be in good agreement with those provided by the effective index method or finite elements. The versatility of the differential method is demonstrated by considering complex configurations such as trapezoidal waveguides or DLSPPWs lying on a finite width metal stripe.

Conformational Changes and Charge Transfer in Biomolecules Resolved Using Dynamic Enhanced Raman Correlation Spectroscopy

International audience; In this contribution, we report that conforma-tional changes of molecules that are often buried in a wide-distributed Gaussian distribution can be discerned by analyzing the dynamics of specific Raman lines. We investigate the pertinence of the auto-and cross-correlation functions applied to the dynamics of three Raman lines of an amino acid, the tryptophan. The cross-correlation between intensity and the Raman band is an indicator of the charge transfer during the diffusion limited reaction of tryptophan and the gold surface. The Pećlet number Pe can provide a valuable indicator of the convective and/or diffusive features of each Raman band. Adsorption induced confo…

Submicrometer in-plane integrated surface plasmon cavities.

International audience; The optical properties of in-plane integrated surface plasmon polariton (SPP) cavities comprised of a thin film area sandwiched between two one-dimensional Bragg SPP mirrors are investigated numerically and experimentally. We discuss the resonance condition of these cavities, and we analyze in details the physical origin of the dispersion of this resonance. On the basis of numerical results, we show that in-plane SPP cavities can be used to achieve local SPP field enhancement and antireflecting SPP layers. The numerical results are compared to near-field optical images recorded by operating a photon scanning tunneling microscope. From the near-field images recorded o…

In-plane remote photoluminescence excitation of carbon nanotube by propagating surface plasmon

International audience; In this work, we demonstrate propagating surface plasmon polariton (SPP) coupled photoluminescence (PL) excitation of single-walled carbon nanotube (SWNT). SPPs were launched at a few micrometers from individually marked SWNT, and plasmon-coupled PL was recorded to determine the efficiency of this remote in-plane addressing scheme. The efficiency depends upon the following factors: (i) longitudinal and transverse distances between the SPP launching site and the location of the SWNT and (ii) orientation of the SWNT with respect to the plasmon propagation wave vector (k(SPP)). Our experiment explores the possible integration of carbon nanotubes as a plasmon sensor in p…

Quantitative analysis of localized surface plasmons based on molecular probing

International audience; We report on the quantitative characterization of the plasmonic optical near-field of a single silver nanoparticle. Our approach relies on nanoscale molecular molding of the confined electromagnetic field by photoactivated molecules. We were able to directly image the dipolar profile of the near-field distribution with a resolution better than 10 nm and to quantify the near-field depth and its enhancement factor. A single nanoparticle spectral signature was also assessed. This quantitative characterization constitutes a prerequisite for developing nanophotonic applications.

Single-Crystal vs Polycrystalline Gold: A Non-linear-Optics Analysis

Standard gold in the field of plasmonics is obtained by evaporation or sputtering and therefore is polycrystalline. Yet, this gold presents numbers of drawbacks such as roughness, grains and ill-defined electronic band diagrams in addition to the lack of reproducibility from one instrument to another. It is, thus, beneficial to turn to a metal production that can enable well-defined and controlled gold parameters. To that end, we have explored the wet synthesis of gold nanoplates which represents a simple and robust means of obtaining single-crystal gold (Guo Z, Zhang Y, DuanMu Y, Xu L, Xie S, Gu N, Colloids Surf A 278:33–38, 2006). The synthesized nanoplates are from 50 to less than 100 nm…

Determinant role of the edges in defining surface plasmon propagation in stripe waveguides and tapered concentrators

International audience; In this paper, we experimentally show the effect of waveguide discontinuity on the propagation of the surface plasmon in metal stripes and tapered terminations. Dual-plane leakage microscopy and near-field microscopy were performed on Au stripes with varied widths to imag29e the surface plasmon intensity distribution in real and reciprocal spaces. We unambiguously demonstrate that edge diffraction is the limiting process determining the cutoff conditions of the surface plasmon mode. Finally, we determine the optimal tapered geometry leading to the highest transmission.

Optical gain, spontaneous and stimulated emission of surface plasmon polaritons in confined plasmonic waveguide

International audience; We develop a theoretical model to compute the local density of states in a confined plasmonic waveguide. Based on this model, we derive a simple formula with a clear physical interpretation for the lifetime modification of emitters embedded in the waveguide. The gain distribution within the active medium is then computed following the formalism developed in a recent work [Phys. Rev. B 78, 161401 (2008)], by taking rigorously into account the pump irradiance and emitters lifetime modifications in the system. We finally apply this formalism to describe gain–assisted propagation in a dielectric–loaded surface plasmon polariton waveguide.

Measuring the differential scattering cross-section of gold nanoparticles - art. no. 70321E

International audience; In this paper we present an experimental apparatus capable of measuring the differential scattering cross sections of individual nanoparticles and arrangement of nanoparticles. We show that the mapping a partial differential scattering cross section, qualitative information about the electromagnetic local density of states dominated by evanescent modes scattered by the structure can be obtained.

Evaluating plasmonic transport in current-carrying silver nanowires

cited By 1; International audience; Plasmonics is an emerging technology capable of simultaneously transporting a plasmonic signal and an electronic signal on the same information support1,2,3. In this context, metal nanowires are especially desirable for realizing dense routing networks4. A prerequisite to operate such shared nanowire-based platform relies on our ability to electrically contact individual metal nanowires and efficiently excite surface plasmon polaritons5 in this information support. In this article, we describe a protocol to bring electrical terminals to chemically-synthesized silver nanowires6 randomly distributed on a glass substrate7. The positions of the nanowire ends …

Electron-induced limitation of surface plasmon propagation in silver nanowires

Plasmonic circuitry is considered as a promising solution-effective technology for miniaturizing and integrating the next generation of optical nano-devices. A key element is the shared metal network between electrical and optical information enabling an efficient hetero-integration of an electronic control layer and a plasmonic data link. Here, we investigate to what extend surface plasmons and current-carrying electrons interfere in such a shared circuitry. By synchronously recording surface plasmon propagation and electrical output characteristics of single chemically-synthesized silver nanowires we determine the limiting factors hindering the co-propagation of electrical current and sur…

Apertureless scanning near-field optical microscopy: a comparison between homodyne and heterodyne approaches

International audience; In coherent homodyne apertureless scanning near-field optical microscopy (ASNOM) the background field cannot be fully suppressed because of the interference between the different collected fields, making the images difficult to interpret. We show that implementing the heterodyne version of ASNOM allows one to overcome this issue. We present a comparison between homodyne and heterodyne ASNOM through near-field analysis of gold nanowells, integrated waveguides, and a single evanescent wave generated by total internal reflection. The heterodyne approach allows for the control of the interferometric effect with the background light. In particular, the undesirable backgro…

Single-molecule controlled emission in planar plasmonic cavities

International audience; We study the fluorescence emission from single dye molecules in coplanar plasmonic cavities composed of a thin gold film surrounded by two in-plane surface plasmon Bragg mirrors. We first discuss the effect of the presence of Bragg mirrors on the radiation diagram of surface plasmon coupled emission. Then, we investigate the role of the planar cavity size by single-molecule fluorescence lifetime imaging. Experimental data are compared to numerical simulations of the decay rates calculated as a function of the molecule orientation and position within the cavity. The creation of new decay channels by coupling to the cavity modes is also discussed. We measure a plasmoni…

Integrated plasmonic waveguides: A mode solver based on density of states formulation

International audience; We express the density of states (DOS) near guided resonances of plasmonic waveguides by using multiple-scattering theory. In direct analogy with the case of localized electronic defect states in condensed matter, we demonstrate that optical DOS variations follow a lorentzian profile near guided modes resonances. The lorentzian shape gives quantitative information on the guided modes (effective index, propagation length, and polarization state). We numerically investigate both leaky and bound (lossy) modes supported by dielectric-loaded surface-plasmon-polariton waveguides.

Error signal artifact in apertureless scanning near-fiel microcospy

International audience

Fluorescence relaxation in the near-field of a mesoscopic metallic particle : distance dependence and role of plasmon modes

International audience; We analytically and numerically analyze the fluorescence decay rate of a quantum emitter placed in the vicinity of a spherical metallic particle of mesoscopic size (i.e with dimensions comparable to the emission wavelength). We discuss the efficiency of the radiative decay rate and non–radiative coupling to the particle as well as their distance dependence. The electromagnetic coupling mechanisms between the emitter and the particle are investigated by analyzing the role of the plasmon modes and their nature (dipole, multipole or interface mode). We demonstrate that near-field coupling can be expressed in a simple form verifying the optical theorem for each particle …

Dielectric-loaded surface plasmon polariton waveguides: Figures of merit and mode characterization by image and Fourier plane leakage microscopy

International audience; Waveguiding of surface plasmon polaritons by dielectric-loaded metal structures is studied in detail by combining numerical simulations and leakage radiation microscopy. These types of waveguides are first numerically investigated using the effective index model and the differential method. We analyzed systematically the influence of the ridge width and thickness of the waveguide on the properties of the surface plasmon guided modes. In particular we investigated the confinement factor of the modes and their associated propagation lengths. These two parameters can be optimized by adjusting the thickness of the dielectric layer. Waveguides loaded with thick and thin d…

Momentum-space spectroscopy for advanced analysis of dielectric-loaded surface plasmon polariton coupled and bent waveguides

We perform advanced radiation leakage microscopy of routing dielectric-loaded plasmonic waveguiding structures. By direct plane imaging and momentum-space spectroscopy, we analyze the energy transfer between coupled waveguides as a function of gap distance and reveal the momentum distribution of curved geometries. Specifically, we observed a clear degeneracy lift of the effective indices for strongly interacting waveguides in agreement with coupled-mode theory. We use momentum-space representations to discuss the effect of curvature on dielectric-loaded waveguides. The experimental images are successfully reproduced by a numerical and an analytical model of the mode propagating in a curved …

Near-field properties of plasmonic nanostructures with high aspect ratio

International audience; Using the Green's dyad technique based on cuboidal meshing, we compute the electromagnetic field scattered by metal nanorods with high aspect ratio. We investigate the effect of the meshing shape on the numerical simulations. We observe that discretizing the object with cells with aspect ratios similar to the object's aspect ratio improves the computations, without degrading the convergency. We also compare our numerical simulations to finite element method and discuss further possible improvements.

Discrimination between Single Protein Conformations Using Dynamic SERS

In biomedicine and biophysics, the discrimination of protein conformations is of critical importance for identifying the unfolding states in the diagnosis of neurodegenerative diseases. We develop a dynamic Raman spectroscopic approach based on a statistical analysis of the time series of spectral fingerprints of single protein. We show that the unfolded state of bovine serum albumin can be identified in the time series using the fluctuations of the Raman bands of some amino acids, tryptophan, tyrosine, leucine, and histidine, acting as biomarkers. The statistical analysis induces also the sorting between physisorption and chemisorption events. This is confirmed by the spectral analysis of …

Performance of electro-optical plasmonic ring resonators at telecom wavelengths

International audience; In this work we report on the characteristics of an electro-optical dielectric-loaded surface plasmon polariton waveguide ring resonator. By doping the dielectric host matrix with an electro-optical material and designing an appropriate set of planar electrodes, we measured a 16% relative change of transmission upon application of a controlled electric field. We have analyzed the temporal response of the device and conclude that electrostriction of the host matrix is playing a dominating role in the transmission response.

Directional Second Harmonic Generation Controlled by Sub-wavelength Facets of an Organic Mesowire

Directional harmonic generation is an important property characterizing the ability of nonlinear optical antennas to diffuse the signal in well-defined region of space. Herein, we show how sub-wavelength facets of an organic molecular mesowire crystal can be utilized to systematically vary the directionality of second harmonic generation (SHG) in the forward scattering geometry. We demonstrate this capability on crystalline diamonoanthraquinone (DAAQ) mesowires with subwavelength facets. We observed that the radial angles of the SHG emission can be tuned over a range of 130 degrees. This angular variation arises due to spatially distributed nonlinear dipoles in the focal volume of the excit…

Nanophotopolymerization Triggered by the Enhanced Optical Near Field of Metallic Nanoparticles

International audience; A novel approach is reported for imaging and quantifying both the depth and the strength of the optical near-field, of a single colloidal metal nanoparticle, associated with localized surface plasmons. It will be emphasized that this technique relies on a nanoscale molecular molding of the confined electromagnetic field of metal colloids, irradiated at their resonance, by a photo-activated polymer, which enabled us to directly image the dipolar profile of the near-field distribution with an unprecedented resolution, better than 10 nm. Moreover, the approach used enabled one to quantify the near-field enhancement factor. This approach has overcome all the difficulties…

Launching propagating surface plasmon polaritons by a single carbon nanotube dipolar emitter.

International audience; We report on the excitation of propagating surface plasmon polaritons in thin metal films by a single emitter. Upon excitation in the visible regime, individual semiconducting single-walled carbon nanotubes are shown to act as directional near-infrared point dipole sources launching propagating surface plasmons mainly along the direction of the nanotube axis. Plasmon excitation and propagation is monitored in Fourier and real space by leakage radiation microscopy and is modeled by rigorous theoretical calculations. Coupling to plasmons almost completely reshapes the emission of nanotubes both spatially and with respect to polarization as compared to photoluminescence…

A coupled lossy local-mode theory description of a plasmonic tip

International audience; We investigate power propagation in a metal-coated tapered optical fiber. We analyze in detail the conversion from the fiber core guided mode to a surface plasmon polariton (SPP) confined at the tip apex. To this aim, we adapt coupled local-mode theory to include lossy modes. Two distinct regimes are identified. In the case of thin metal coating, a strong coupling regime occurs between a core guided mode and a SPP with good conversion efficiency. In the case of thick metal coating, a very weak coupling occurs. Finally, energy confinement and the role of Joule losses are discussed in the near-infrared and visible ranges. Moreover, the coupled equations derived for loc…

Purcell factor for a point-like dipolar emitter coupled to a two-dimensional plasmonic waveguide

International audience; We theoretically investigate the spontaneous emission of a point-like dipolar emitter located near a two-dimensional plasmonic waveguide of arbitrary form. We invoke an explicit link with the density of modes of the waveguide describing the electromagnetic channels into which the emitter can couple. We obtain a closed form expression for the coupling to propagative plasmon, extending thus the Purcell factor to plasmonic configurations. Radiative and nonradiative contributions to the spontaneous emission are also discussed in detail.

Excitation of plasmonic nanoantennas by nonresonant and resonant electron tunnelling.

A rigorous theory of photon emission accompanied inelastic tunnelling inside the gap of plasmonic nanoantennas has been developed. The disappointingly low efficiency of the electrical excitation of surface plasmon polaritons in these structures can be increased by orders of magnitude when a resonant tunnelling structure is incorporated inside the gap. Resonant tunnelling assisted surface plasmon emitter may become a key element in future electrically-driven nanoplasmonic circuits.

Imaging Surface Plasmons

Controlling surface plasmons is at the heart of plasmonics. Advances in this field are to a large extent triggered by our ability to visualize surface plasmons in their different forms. In this chapter, we provide a review of the different techniques capable of imaging and visualizing surface plasmons. We have divided these techniques in three distinct families: proximal probe techniques, far-field microscopies, and electron imaging. We review here their principal characteristics, advantages, and limitations and illustrate the discussion with images taken from the literature.

Effect of quantized conductivity on the anomalous photon emission radiated from atomic-size point contacts

We observe anomalous visible to near-infrared electromagnetic radiation emitted from electrically driven atomic-size point contacts. We show that the number of photons released strongly depends on the quantized conductance steps of the contact. Counter-intuitively, the light intensity features an exponential decay dependence with the injected electrical power. We propose an analytical model for the light emission considering an out-of-equilibrium electron distribution. We treat photon emission as bremsstrahlung process resulting from hot electrons colliding with the metal boundary and a find qualitative accord with the experimental data.

Efficient surface plasmon field confinement in one-dimensional crystal line-defect waveguides

International audience; The authors operate a near-field optical microscope to investigate surface plasmon polariton (SPP) propagation along linear waveguides opened into one-dimensional (1D) plasmonic crystals, i.e., crystals featuring a single lattice plane orientation. They show that efficient SPP field confinement can be achieved by this type of waveguide although no band gap exists in the direction perpendicular to the waveguide axis. From computed wave-vector diagrams, they show that 1D plasmonic crystals can open a wide range of prohibited propagation directions preventing from a significant coupling of the waveguide SPP modes with the crystal Bloch modes. Finally, the authors demons…

Electromagnetic Singularities and Resonances in Near-Field Optical Probes

Over the last two decades scanning near-field optical microscopy (SNOM) has demonstrated its ability to provide optical resolution significantly better than the diffraction limit (<20 nm). The general principle of SNOM relies on the approach of a nanometer-sized object in the optical near-field of a sample to be studied. This nano-object (NO) is usually the extremity of a probe. Regardless of the nature of the observed SNOM signal (inelastic scattering, fluorescence, etc.), the detection of the light is achieved in the far-field regime where the NO acts as a mediator between the optical near-field and the detector. Figure 1 is a schematic illustration of the SNOM principle.

Colloidal Quantum Dot Integrated Light Sources for Plasmon Mediated Photonic Waveguide Excitation

We operate micron-sized CdSe/CdS core–shell quantum dot (QD) clusters deposited onto gold patches as integrated light sources for the excitation of photonic waveguides. The surface plasmon mode launched by the QD fluorescence at the top interface of the gold patches are efficiently coupled to photonic modes sustained by titanium dioxide ridge waveguides. We show that, despite a large effective index difference, the plasmonic and the photonic modes can couple with a very high efficiency provided the vertical offset between the two kinds of waveguides is carefully controlled. Based on the effective index contrast of the plasmonic and the photonic modes, we engineer in-plane integrated hybrid …

Electrostatic Control over Optically Pumped Hot Electrons in Optical Gap Antennas

International audience; We investigate the influence of a static electric field on the incoherent nonlinear response of an unloaded electrically contacted nanoscale optical gap antenna. Upon excitation by a tightly focused near-infrared femtosecond laser beam, a transient elevated temperature of the electronic distribution results in a broadband emission of nonlinear photoluminescence (N-PL). We demonstrate a modulation of the yield at which driving photons are frequency up-converted by means of an external control of the electronic surface charge density. We show that the electron temperature and consequently the N-PL intensity can be enhanced or reduced depending on the command polarity a…

Influence of an Electron Beam Exposure on the Surface Plasmon Resonance of Gold Nanoparticles

Electron beam imaging is a common technique used for characterizing the morphology of plasmonic nanostructures. During the imaging process, the electron beam interacts with traces of organic material in the chamber and produces a well-know layer of amorphous carbon over the specimen under investigation. In this paper, we investigate the effect of this carbon adsorbate on the spectral position of the surface plasmon in individual gold nanoparticles as a function of electron exposure dose. We find an optimum dose for which the plasmonic response of the nanoparticle is not affected by the imaging process. The final publication is available at link.springer.com

Influence of the Number of Nanoparticles on the Enhancement Properties of Surface-Enhanced Raman Scattering Active Area: Sensitivity versus Repeatability

In the present work, the combination of chemical immobilization with electron beam lithography enables the production of sensitive and reproducible SERS-active areas composed of stochastic arrangements of gold nanoparticles. The number of nanoparticles was varied from 2 to 500. Thereby a systematic analysis of these SERS-active areas allows us to study SERS efficiency as a function of the number of nanoparticles. We found that the experimental parameters are critical, in particular the size of the SERS-active area must be comparable to the effective area of excitation to obtained reproducible SERS measurements. The sensitivity has also been studied by deducing the number of NPs that generat…

Electrical excitation of surface plasmons

We exploit a plasmon mediated two-step momentum down-conversion scheme to convert low-energy tunneling electrons into propagating photons. Surface plasmon polaritons (SPPs) propagating along an extended gold nanowire are excited on one end by low-energy electron tunneling and are then converted to free-propagating photons at the other end. The separation of excitation and outcoupling proves that tunneling electrons excite gap plasmons that subsequently couple to propagating plasmons. Our work shows that electron tunneling provides a nonoptical, voltage-controlled, and low-energy pathway for launching SPPs in nanostructures, such as plasmonic waveguides.

Near-field beam displacement at surface plasmon resonance

International audience; A finite-size beam exciting a surface plasmon polariton (SPP) in a prism coupling configuration experiences an in-plane displacement that can be used for the characterization of plasmonic components by means of near-field optical microscopy. We first demonstrate experimentally the existence of this displacement by taking near-field images of finite-width metal strips. Next, the properties of this shift are analyzed in detail. We investigate the dynamic of the near-field shift for an incident Gaussian beam as a function of illumination conditions. For beams with a narrow spectrum, we propose a straightforward derivation showing that the displacement depends on the ave…

Hot electrons and nonlinear optical nanoantennas

The large field enhancement generated at the surface of a resonant plasmonic nanoparticle, or optical antennas, is the key mechanism that eventually led to the development of nonlinear plasmonics [1-2]. While the resonance may boost the nonlinear yield of an adjacent structure or surrounding medium, it was soon realized that optical antennas possess nonlinear coefficients comparable or exceeding those of standard nonlinear optical materials [3]. We discuss here two nonlinear optical processes — incoherent multi-photon luminescence (MPL) and coherent second-harmonic generation (SHG) — emitted from gold rod optical antennas upon local illumination with a tightly focused femtosecond near-infra…

Thermo-electric detection of waveguided surface plasmon propagation

International audience; The thermo-electric detection of a waveguided surface plasmon traveling along one electrode of an in-plane integrated thermocouple is demonstrated. By using a particular design of the thermocouple, the thermo-electric signal due to the losses of the plasmon mode can be separated from the non-resonant heating of the waveguide. The thermo-electric signal associated with the plasmon propagation is proportional to the power coupled into the waveguided mode and exhibits a maximum at a distance from the excitation site depending on both the heat transfer coefficient of the system and the plasmon mode damping distance.

Tuning of an Optical Dimer Nanoantenna by Electrically Controlling Its Load Impedance

International audience; Optical antennas are elementary units used to direct optical radiation to the nanoscale. Here we demonstrate an active control over individual antenna performances by an external electrical trigger. We find that by an in-plane command of an anisotropic load medium, the electromagnetic interaction between individual elements constituting an optical antenna can be controlled, resulting in a strong polarization and tuning response. An active command of the antenna is a prerequisite for directing light wave through the utilization of such a device.

Photon bunching of the nonlinear photoluminescence emitted by plasmonics metals

International audience; In this report, we investigate the statistical temporal distribution of nonlinear upconverted photoluminescence emitted by gold and silver nanostructures excited by focused near-infrared laser pulses. We systematically observe a clear signature of photon bunching regardless of the nano-object's geometry, material's crystalline arrangement, and electronic band structure. The similarity of the data obtained across very different plasmonic objects confirms that these types of nonlinear radiation share a common chaotic origin and result from a collection of emitters. The correlation of photons at a picosecond time scale released by nanoscale nonlinear sources of broadban…

Spontaneous hot-electron light emission from electron-fed optical antennas

Nanoscale electronics and photonics are among the most promising research areas providing functional nano-components for data transfer and signal processing. By adopting metal-based optical antennas as a disruptive technological vehicle, we demonstrate that these two device-generating technologies can be interfaced to create an electronically-driven self-emitting unit. This nanoscale plasmonic transmitter operates by injecting electrons in a contacted tunneling antenna feedgap. Under certain operating conditions, we show that the antenna enters a highly nonlinear regime in which the energy of the emitted photons exceeds the quantum limit imposed by the applied bias. We propose a model based…

Surface plasmon interference excited by tightly focused laser beams

International audience; We show that interfering surface plasmon polaritons can be excited with a focused laser beam at normal incidence to a plane metal film. No protrusions or holes are needed in this excitation scheme. Depending on the axial position of the focus, the intensity distribution on the metal surface is either dominated by interferences between counterpropagating plasmons or by a two-lobe pattern characteristic of localized surface plasmon excitation. Our experiments can be accurately explained by use of the angular spectrum representation and provide a simple means for locally exciting standing surface plasmon polaritons.

Coherent control in single plasmonic nanostructures

Coherent control in plasmonic nanostructures is a door to space-time confinement of optical excitation and femtosecond super-resolution spectroscopy. Towards this goal, here we demonstrate femtosecond pulse-shaping of single gold nanostructure and local phase compensation.

Plasmon-based free-radical photopolymerization : effect of diffusion on nanolithography processes

This Article interrogates the mechanisms responsible for nanoscale photopolymerization induced by confined and enhanced electromagnetic fields. Surface plasmon dipolar resonance of individual Ag nanoparticles was used as an optical near-field source to locally trigger the reaction of a photopolymerizable formulation. Laser excitation of the nanoparticles embedded in the formulation reproducibly generates polymer features with typical dimensions ranging from 2 nm to a few tens of nanometer. We have determined the physicochemical parameters and mechanisms controlling the spatial extent of the photopolymerization process. We found that the diffusion of the dye is the main process limiting the …

Off-Resonant Optical Excitation of Gold Nanorods: Nanoscale Imprint of Polarization Surface Charge Distribution

International audience; We report on the nanoscale optical characterization of gold nanorods irradiated out of their plasmonic resonance. Our approach is based on the reticulation of a photopolymerizable formulation locally triggered by enhanced electromagnetic fields. The tiny local field enhancement stems from the surface polarization charges associated with the electric field discontinuity at the metal/dielectric interface. This allows us to get a nanoscale signature of the spatial distribution of the surface charge density in metallic nanoparticles irradiated off-resonance.

Quelle est la couleur de l’or ?

International audience; A priori, la question peut surprendre ; son reflet doré est si caractéristique. Pourtant, ce métal précieux peut diffuser une réponse chromatique variée si on l’observe sous une forme nano-structurée. Mieux, si on l’éclaire avec une impulsion lumineuse ultra-brève, l’or génère une variété de phénomènes non-linéaires qui enrichissent spectralement la palette de longueurs d’onde émise par le métal.

NEAR-FIELD OPTICAL EXCITATION AND DETECTION OF SURFACE PLASMONS

Resonance quality, radiative/ohmic losses and modal volume of Mie plasmons

International audience; Molecular sytems are efficiently coupled to metal nanoparticles via the excitation of localized surface plasmons-polaritons (SPPs). The coupling strength between SPP and emitters can be estimated from the ratio Q/V where Q and V refer to the mode quality factor and effective volume, respectively. In this letter, we investigate in details the properties of Mie plasmons supported by a metallic nanosphere (Q-factor, radiative and ohmic losses, modal volume). We particularly focus on the difficulty to unambiguously define the modal volumes of localized SPPs. This leads us to propose two definitions; the first one is based on Purcell factor for a dipolar emitter in close …

Far-field imaging of the electromagnetic local density of optical states.

International audience; We introduce a new experimental method to measure the local electromagnetic density of states (LDOS) by integrating the differential scattering cross section. The signal detected essentially reflects the intrinsic scattering response of the photonic structures and renders the partial LDOS dominated by evanescent modes. We give a theoretical understanding of the LDOS image formation and show a qualitative agreement between experimental images and theoretical maps. This approach can be practically applied to the direct measurement of an optical antenna's scattering efficiency and can provide valuable information for designing optimum structures utilized in radiative de…

Reversible Strong Coupling in Silver Nanoparticle Arrays Using Photochromic Molecules

International audience; In this Letter, we demonstrate a reversible strong coupling regime between a dipolar surface plasmon resonance and a molecular excited state. This reversible state is experimentally observed on silver nanoparticle arrays embedded in a polymer film containing photochromic molecules. Extinction measurements reveal a clear Rabi splitting of 294 meV, corresponding to ∼13% of the molecular transition energy. We derived an analytical model to confirm our observations, and we emphasize the importance of spectrally matching the polymer absorption with the plasmonic resonance to observe coupled states. Finally, the reversibility of this coupling is illustrated by cycling the …

Sorting of Single Biomolecules based on Fourier Polar Representation of Surface Enhanced Raman Spectra

AbstractSurface enhanced Raman scattering (SERS) spectroscopy becomes increasingly used in biosensors for its capacity to detect and identify single molecules. In practice, a large number of SERS spectra are acquired and reliable ranking methods are thus essential for analysing all these data. Supervised classification strategies, which are the most effective methods, are usually applied but they require pre-determined models or classes. In this work, we propose to sort SERS spectra in unknown groups with an alternative strategy called Fourier polar representation. This non-fitting method based on simple Fourier sine and cosine transforms produces a fast and graphical representation for sor…

Gain, detuning, and radiation patterns of nanoparticle optical antennas

International audience; For their capability to localize and redirect electromagnetic field, metal nanoparticles have been recently viewed as efficient nanoantenna operating in the optical regime. In this article, we experimentally investigated the optical responses of coupled gold antenna pairs and measured the critical parameters defining antenna characteristics: resonant frequencies and bandwidths, detuning and gains, and radiation patterns.

Discerning the Origins of the Amplitude Fluctuations in Dynamic Raman Nanospectroscopy

International audience; We introduce a novel experimental and analytical method for discerning rare surface-enhanced Raman scattering (SERS) events observable at the nanoscale. We show that the kinetics of the Raman activity recorded on an isolated nanostructure is punctuated by intense and rare events of large amplitude and spectral variations. The fluctuations of thousands of SERS spectra were analyzed statistically in terms of power density functions, and the occurrence of the rare events was quantified by a wavenumber statistics. Our analysis enables one to extract valuable and unique spectroscopic signature of Raman variations usually hidden in time-average or space-average measurement…

Silencing and enhancement of second-harmonic generation in optical gap antennas

International audience; Amplifying local electromagnetic fields by engineering optical interactions between individual constituents of an optical antenna is considered fundamental for efficient nonlinear wavelength conversion in nanometer-scale devices. In contrast to this general statement we show that high field enhancement does not necessarily lead to an optimized nonlinear activity. In particular, we demonstrate that second-harmonic responses generated at strongly interacting optical gap antennas can be significantly suppressed. Numerical simulations are confirming silencing of second-harmonic in these coupled systems despite the existence of local field amplification. We then propose a…

Wave-vector analysis of plasmon-assisted distributed nonlinear photoluminescence along Au nanowires

We report a quantitative analysis of the wavevector diagram emitted by nonlinear photoluminescence generated by a tightly focused pulsed laser beam and distributed along Au nanowire via the mediation of surface plasmon polaritions. The nonlinear photoluminescence is locally excited at key locations along the nanowire in order to understand the different contributions constituting the emission pattern measured in a conjugate Fourier plane of the microscope. Polarization-resolved measurements reveal that the nanowire preferentially emits nonlinear photoluminescence polarized transverse to the long axis at close to the detection limit wavevectors with a small azimuthal spread in comparison to …

Pre-determining the location of electromigrated gaps by nonlinear optical imaging

In this paper we describe a nonlinear imaging method employed to spatially map the occurrence of constrictions occurring on an electrically-stressed gold nanowire. The approach consists at measuring the influence of a tightly focused ultrafast pulsed laser on the electronic transport in the nanowire. We found that structural defects distributed along the nanowire are efficient nonlinear optical sources of radiation and that the differential conductance is significantly decreased when the laser is incident on such electrically-induced morphological changes. This imaging technique is applied to pre-determined the location of the electrical failure before it occurs.

All-optical and electro-optical active plasmonic telecom components

Active plasmonics is an attractive emerging field in which the ability to control the surface plasmon polariton (SPP) propagation finds many applications such as realization of fully functional integrated photonic circuitry. We demonstrate both numerically and experimentally switching of the SPP transmission based on two different approaches namely the all-optical and electro-optical at telecom wavelengths. The plasmonic component consists of a compact and efficient SPP switch utilizing highly sensitive ring resonator which has high sensitivity to the refractive index changes. Fabrication was done via e-beam lithography utilizing advanced proximity corrections. The compenents were character…

Excitation of a one-dimensional evanescent wave by conical edge diffraction of surface plasmon

International audience; The experimental observation of a one-dimensional evanescent wave supported by a 90◦ metal edge is reported. Through a measurement of in-plane momenta, we clearly demonstrate the dimensional character of this surface wave and show that it is non-radiative in the superstrate. Excitation conditions, lateral extension and polarization properties of this wave are discussed. Finally, we explore the effect of the surrounding dielectric medium and demonstrate that a single edge can sustain distinct excitations.

Modal and wavelength conversions in plasmonic nanowires

We show that plasmonic nanowire-nanoparticle systems can perform nonlinear wavelength and modal conversions and potentially serve as building blocks for signal multiplexing and novel trafficking modalities. When a surface plasmon excited by a pulsed laser beam propagates in a nanowire, it generates a localized broadband nonlinear continuum at the nanowire surface as well as at active locations defined by sites where nanoparticles are absorbed (enhancement sites). The local response may couple to new sets of propagating modes enabling a complex routing of optical signals through modal and spectral conversions. Different aspects influencing the optical signal conversions are presented, includ…

Differential method for modelling dielectric-loaded surface plasmon polariton waveguides

International audience; This paper demonstrates the efficiency of the differential method, a conventional grating theory, to investigate dielectric loaded surface plasmon polariton waveguides (DLSPPWs), known to be a potential solution for optical interconnects. The method is used to obtain the mode effective indices (both real and imaginary parts) and the mode profiles. The results obtained with the differential method are found to be in good agreement with those provided by the effective index method or finite elements. The versatility of the differential method is demonstrated by considering complex configurations such as trapezoidal waveguides or DLSPPWs lying on a finite width metal st…

Coupling of a dipolar emitter into one-dimensional surface plasmon.

Quantum plasmonics relies on a new paradigm for light-matter interaction. It benefits from strong confinement of surface plasmon polaritons (SPP) that ensures efficient coupling at a deep subwavelength scale, instead of working with a long lifetime cavity polariton that increases the duration of interaction. The large bandwidth and the strong confinement of one dimensional SPP enable controlled manipulation of a nearby quantum emitter. This paves the way to ultrafast nanooptical devices. However, the large SPP bandwidth originates from strong losses so that a clear understanding of the coupling process is needed. In this report, we investigate in details the coupling between a single emitte…

Electrical excitation of surface plasmons by an individual carbon nanotube transistor.

We demonstrate here the realization of an integrated, electrically driven, source of surface plasmon polaritons. Light-emitting individual single-walled carbon nanotube field effect transistors were fabricated in a plasmonic-ready platform. The devices were operated at ambient conditions to act as an electroluminescence source localized near the contacting gold electrodes. We show that photon emission from the semiconducting channel can couple to propagating surface plasmons developing in the electrical terminals. Our results show that a common functional element can be operated for two different platforms emphasizing thus the high degree of compatibility between state-of-the-art nano-optoe…

Selective excitation of bright and dark plasmonic resonances of single gold nanorods.

Plasmonic dark modes are pure near-field resonances since their dipole moments are vanishing in far field. These modes are particularly interesting to enhance nonlinear light-matter interaction at the nanometer scale because radiative losses are mitigated therefore increasing the intrinsic lifetime of the resonances. However, the excitation of dark modes by standard far field approaches is generally inefficient because the symmetry of the electromagnetic near-field distribution has a poor overlap with the excitation field. Here, we demonstrate the selective optical excitation of bright and dark plasmonic modes of single gold nanorods by spatial phase-shaping the excitation beam. Using two-p…

Polymer-metal waveguides characterization by Fourier plane leakage radiation microscopy

International audience; The guiding properties of polymer waveguides on a thin gold film are investigated in the optical regime. The details of propagation in the waveguides are studied simultaneously in the object and Fourier planes, providing direct measurement of both the real and imaginary parts of the effective index of the guided mode. A fair agreement between theoretical analysis provided by the differential method and experimental leakage radiation microscopy data is shown. All these tools bring valuable information for designing and understanding such devices. (C) 2007 American Institute of Physics.

Imaging Symmetry-Selected Corner Plasmon Modes in Penta-Twinned Crystalline Ag Nanowires

International audience; Using dual-plane leakage radiation microscopy, we investigate plasmon propagation in individual penta-twinned crystalline silver nanowires. By measuring the wavevector content of the light emitted in the substrate, we unambiguously determine the effective index and the losses of the mode propagating in these structures. The experimental results, in particular, the unexpectedly low effective index, reveal the direct influence of the nanowire crystallinity and pentagonal structure on the observed plasmon modes. By analogy with molecular orbitals of similar symmetry, the plasmon modes are also determined numerically in good agreement with the observed values. We further…

Spatial Distribution of the Nonlinear Photoluminescence in Au Nanowires

When gold nanowires are excited with a tightly focused femtosecond laser a distributed nonlinear photoluminescence (N-PL) develops throughout the entire structure. A complete spaced-resolved analysis of the spectral signature of the nanowire nonlinear response is carried out to understand the origin of the distributed nonlinear response. We discuss various mechanisms to explain the experimental data and unambiguously demonstrate that the spatial and spectral extension of the N-PL in the nanowire are mainly dictated by the propagation of a surface plasmon excited at the pump wavelength. We also present experimental signature of near-field excitation of a broadband continuum of surface plasmo…

Surface plasmon routing in dielectric-loaded surface plasmon polariton waveguides - art. no. 70330S

International audience; Waveguiding by dielectric-loaded surface plasmon-polaritons (DLSPP) structures are numerically and experimentally investigated. We used the effective index model to understand the influence of basic waveguide parameters such as width and thickness on the properties of the surface plasmon guided modes. A waveguide was fabricated and experimentally studied. The effective indices of the modes supported by the waveguide and their propagation length are evaluated by leakage radiation microscopy in both the Fourier and imaging planes. Several excitation schemes were tested including surface plasmon coupling by diascopic or episcopic illumination as well as defect-mediated …

Optical absorption of torus-shaped metal nanoparticles in the visible range

Received 22 November 2007; published 19 December 2007We theoretically and experimentally investigated the optical response of a thin metal nanotorus in the visiblerange. The close formulas describing the extinction cross sections of a torus are obtained in the nonretardedapproximation. We demonstrate a good agreement between numerical simulations and experimental data. Ourfindings show that the main resonance is highly sensitive to the external medium and the geometrical param-eters of the particle.DOI: 10.1103/PhysRevB.76.245422 PACS number s : 78.67.Bf, 73.20.Mf, 78.20.Ci

Purcell factor for 3D- dipolar emitter coupling to 2D- plasmonic waveguides

We theoretically investigate spontaneous emission of a quantum (3D) dipolar emitter located near a (2D) plasmonic waveguide of arbitrary form. The channels into which emitter couples (plasmon, scattering, electron-hole pairs creation) are well identified.

si-movie1.avi

The video describes the SHG signal from an organic meso wire under laser illumination. We show the generation of SHG from different facets of the wire by moving the illumination spot transversly accross the mesowire axis.

si-movie1.avi

The video describes the SHG signal from an organic meso wire under laser illumination. We show the generation of SHG from different facets of the wire by moving the illumination spot transversly accross the mesowire axis.