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We employ tip-enhanced infrared near-field microscopy to study the plasmonic properties of epitaxial quasi-free-standing monolayer graphene on silicon carbide. The near-field images reveal propagating graphene plasmons, as well as a strong plasmon reflection at gaps in the graphene layer, which appear at the steps between the SiC terraces. When the step height is around 1.5 nm, which is two orders of magnitude smaller than the plasmon wavelength, the reflection signal reaches 20% of its value at graphene edges, and it approaches 50% for step heights as small as 5 nm. This intriguing observation is corroborated by numerical simulations and explained by the accumulation of a line charge at the graphene termination. The associated electromagnetic fields at the graphene termination decay within a few nanometers, thus preventing efficient plasmon transmission across nanoscale gaps. Our work suggests that plasmon propagation in graphene-based circuits can be tailored using extremely compact nanostructures, such as ultranarrow gaps. It also demonstrates that tip-enhanced near-field microscopy is a powerful contactless tool to examine nanoscale defects in graphene.

When exposing small particles on a substrate to a light plane wave, the scattered optical near field is spatially modulated and highly complex. We show, for the particular case of dielectric microspheres, that it is possible to image these optical near-field distributions in a quantitative way. By placing a single microsphere on a thin film of the photosensitive phase change material Ge(2)Sb(5)Te(5) and exposing it to a single short laser pulse, the spatial intensity modulation of the near field is imprinted into the film as a pattern of different material phases. The resulting patterns are investigated by using optical as well as high-resolution scanning electron microscopy. Quantitative information on the local optical near field at each location is obtained by calibrating the material response to pulsed laser irradiation. We discuss the influence of polarization and angle of incidence of the laser beam as well as particle size on the field distribution. The experimental results are in good quantitative agreement with a model based on a rigorous solution of Maxwell's equations. Our results have potential application to near-field optical lithography and experimental determination of near fields in complex nanostructures.

We investigate the frictional forces due to quantum fluctuations acting on a small sphere rotating near a surface. At zero temperature, we find the frictional force near a surface to be several orders of magnitude larger than that for the sphere rotating in vacuum. For metallic materials with typical conductivity, quantum friction is maximized by matching the frequency of rotation with the conductivity. Materials with poor conductivity are favored to obtain large quantum frictions. For semiconductor materials that are able to support surface plasmon polaritons, quantum friction can be further enhanced by several orders of magnitude due to the excitation of surface plasmon polaritons.

Imaging localized plasmon modes in noble-metal nanoparticles is of fundamental importance for applications such as ultrasensitive molecular detection. Here, we demonstrate the combined use of optical dark-field microscopy (DFM), cathodoluminescence (CL), and electron energy-loss spectroscopy (EELS) to study localized surface plasmons on individual gold nanodecahedra. By exciting surface plasmons with either external light or an electron beam, we experimentally resolve a prominent dipole-active plasmon band in the far-field radiation acquired via DFM and CL, whereas EELS reveals an additional plasmon mode associated with a weak dipole moment. We present measured spectra and intensity maps of plasmon modes in individual nanodecahedra in excellent agreement with boundary-element method simulations, including the effect of the substrate. A simple tight-binding model is formulated to successfully explain the rich plasmon structure in these particles encompasing bright and dark modes, which we predict to be fully observable in less lossy silver decahedra. Our work provides useful insight into the complex nature of plasmon resonances in nanoparticles with pentagonal symmetry.

The ability to manipulate optical fields and the energy flow of light is central to modern information and communication technologies, as well as quantum information processing schemes. However, because photons do not possess charge, a way of controlling them efficiently by electrical means has so far proved elusive. A promising way to achieve electric control of light could be through plasmon polaritons—coupled excitations of photons and charge carriers—in graphene. In this two-dimensional sheet of carbon atoms, it is expected that plasmon polaritons and their associated optical fields can readily be tuned electrically by varying the graphene carrier density. Although evidence of optical graphene plasmon resonances has recently been obtained spectroscopically, no experiments so far have directly resolved propagating plasmons in real space. Here we launch and detect propagating optical plasmons in tapered graphene nanostructures using near-field scattering microscopy with infrared excitation light. We provide real-space images of plasmon fields, and find that the extracted plasmon wavelength is very short—more than 40 times smaller than the wavelength of illumination. We exploit this strong optical field confinement to turn a graphene nanostructure into a tunable resonant plasmonic cavity with extremely small mode volume. The cavity resonance is controlled in situ by gating the graphene, and in particular, complete switching on and off of the plasmon modes is demonstrated, thus paving the way towards graphene-based optical transistors. This successful alliance between nanoelectronics and nano-optics enables the development of active subwavelength-scale optics and a plethora of nano-optoelectronic devices and functionalities, such as tunable metamaterials, nanoscale optical processing, and strongly enhanced light–matter interactions for quantum devices and biosensing applications.

We report on the identification of surface plasmons in individual gold dumbbell-shaped nanoparticles (AuDBs), as well as AuDBs coated with silver. We use spatially resolved electron energy-loss spectroscopy in a scanning electron microscope, which allows us to map plasmon-energy and intensity spatial distributions. Two dominant plasmon resonances are experimentally resolved in both AuDBs and silver-coated AuDBs. The intensity of these features is peaked either at the tips or at the sides of the nanoparticles. We present boundary element method simulations in good agreement with the experiment, allowing us to elucidate the nature of such modes. While the lower-energy, tip-focused plasmon is of longitudinal character for all dumbbells under consideration, the second side-bound plasmon has a more involved symmetry, starting as a longitudinal quadrupole in homogeneous AuDBs and picking up transversal components when silver coating is added. The longitudinal dipolar mode energy is found to blue-shift upon coating with silver. We find that the substrate produces sizable shifts in the plasmons of silver-coated AuDBs. Our analysis portraits a complex plasmonic scenario in metal nanoparticles coated with silver, including a transition from the original homogeneous gold dumbbell plasmons to the modes of homogeneous silver rods. We believe that these findings can have potential application to plasmon engineering.

The availability of macroscopic, nearly periodic structures known as eutectics opens a new path for controlling light at wavelength scales determined by the geometrical parameters of these materials and the intrinsic properties of their component phases. Here, we analyze the optical waveguiding properties of eutectic mixtures of alkali halides, formed by close-packed arrangements of aligned cylindrical inclusions. The wavelengths of phonon polaritons in these constituents are conveniently situated in the infrared and are slightly larger than the diameter and separation of the inclusions, typically consisting on single-crystal wires down to submicrometer diameter. We first discuss the gap mode and the guiding properties of metallic cylindrical waveguides in the visible and near-infrared, and in particular we investigate the transition between cylinder touching and non-touching regimes. Then, we demonstrate that these properties can be extended to the mid infrared by means of phonon polaritons. Finally, we analyze the guiding properties of an actual eutectic. For typical eutectic dimensions, we conclude that crosstalk between neighboring cylindrical wires is small, thus providing a promising platform for signal propagation and image analysis in the mid infrared.

We study a class of acoustic metamaterials formed by layers of perforated plates and producing negative refraction and backward propagation of sound. A slab of such material is shown to act as a perfect acoustic lens, yielding images with subwavelength resolution over large distances. Our study constitutes a nontrivial extension of similar concepts from optics to acoustics, capable of sustaining negative refraction over extended angular ranges, with potential application to enhanced imaging for medical and detection purposes, acoustofluidics, and sonochemistry.

Graphene plasmons are emerging as an alternative solution to noble metal plasmons, adding the advantages of tunability via electrostatic doping and long lifetimes. These excitations have been so far described using classical electrodynamics, with the carbon layer represented by a local conductivity. However, the question remains, how accurately is such a classical description representing graphene? What is the minimum size for which nonlocal and quantum finite-size effects can be ignored in the plasmons of small graphene structures? Here, we provide a clear answer to these questions by performing first-principles calculations of the optical response of doped nanostructured graphene obtained from a tight-binding model for the electronic structure and the random-phase approximation for the dielectric response. The resulting plasmon energies are in good agreement with classical local electromagnetic theory down to ∼10 nm sizes, below which plasmons split into several resonances that emphasize the molecular character of the carbon structures and the quantum nature of their optical excitations. Additionally, finite-size effects produce substantial plasmon broadening compared to homogeneous graphene up to sizes well above 20 nm in nanodisks and 10 nm in nanoribbons. The atomic structure of edge terminations is shown to be critical, with zigzag edges contributing to plasmon broadening significantly more than armchair edges. This study demonstrates the ability of graphene nanostructures to host well-defined plasmons down to sizes below 10 nm, and it delineates a roadmap for understanding their main characteristics, including the role of finite size and nonlocality, thus providing a solid background for the emerging field of graphene nanoplasmonics.

Among the many extraordinary properties of graphene, its optical response allows one to easily tune its interaction with nearby molecules via electrostatic doping. The large confinement displayed by plasmons in graphene nanodisks makes it possible to reach the strong-coupling regime with a nearby quantum emitter, such as a quantum dot or a molecule. In this limit, the quantum emitter can introduce a significant plasmon-plasmon interaction, which gives rise to a plasmon blockade effect. This produces, in turn, strongly nonlinear absorption cross sections and modified statistics of the bosonic plasmon mode. We characterize these phenomena by studying the equal-time second-order correlation function g((2))(0), which plunges below a value of 1, thus revealing the existence of nonclassical plasmon states. The plasmon-emitter coupling, and therefore the plasmon blockade, can be efficiently controlled by tuning the doping level of the graphene nanodisks. The proposed system emerges as a new promising platform to realize quantum plasmonic devices capable of commuting optical signals at the single-photon/plasmon level.

We demonstrate that 100% light absorption can take place in a single patterned sheet of doped graphene. General analysis shows that a planar array of small particles with losses exhibits full absorption under critical-coupling conditions provided the cross section of each individual particle is comparable to the area of the lattice unit cell. Specifically, arrays of doped graphene nanodisks display full absorption when supported on a substrate under total internal reflection and also when lying on a dielectric layer coating a metal. Our results are relevant for infrared light detectors and sources, which can be made tunable via electrostatic doping of graphene.

We propose a drastically new method for generating single photons in a deterministic way by interaction of electron beams with optical waveguides. We find a single swift electron to produce a guided photon with large probability. The change in energy and propagation direction of the electron reveals the creation of a photon, with the photon energy directly read from the energy-loss spectrum or the beam displacement. Our study demonstrates the viability of deterministically creating single guided photons using electron beams with better than picosecond time uncertainty, thus opening a new avenue for making room temperature, heralded frequency-tunable sources affordable for scientific and commercial developments.

Except for heating losses in metal, propagating plasmons also suffer a lot from radiation losses. In this paper, electron beams are proposed as a way to excite higher-order, multipolar plasmons, which would otherwise not be excited by light, as a way to reduce radiation losses. Specifically, electron excited guided plasmons in a coupled nanoparticle chain and a symmetrical four-wire waveguide are separately discussed. In the coupled nanoparticle chain, the plasmon mode formed by quadrupolar polarized particles with low radiation is efficiently coupled by electron beams. Meanwhile, in the four-wire waveguide, the excited plasmons with zero momentum in the cross-section of each wire possess longer propagating distance than other higher-order plasmons.

Graphene plasmons provide a suitable alternative to noble-metal plasmons because they exhibit much tighter confinement and relatively long propagation distances, with the advantage of being highly tunable via electrostatic gating. Here, we propose to use graphene plasmons as a platform for strongly enhanced light-matter interactions. Specifically, we predict unprecedented high decay rates of quantum emitters in the proximity of a carbon sheet, observable vacuum Rabi splittings, and extinction cross sections exceeding the geometrical area in graphene nanoribbons and nanodisks. Our theoretical results provide the basis for the emerging and potentially far-reaching field of graphene plasmonics, offering an ideal platform for cavity quantum electrodynamics, and supporting the possibility of single-molecule, single-plasmon devices.

We study the plasmons confined at the gap between silver nanospheres and silver planar surfaces by means of angle- and space-resolved spectral cathodoluminescence. Plasmons in individual nanoparticles are excited by an electron beam, giving rise to light emission that is analyzed as a function of photon-energy, emission direction, and position of the beam spot. Gap plasmons are significantly red shifted due to the interaction between the particles and the metal substrate, and they are preferentially excited by positioning the beam close to the sphere centers, which results in an angular emission pattern similar to that of a dipole oriented along the surface normal. In contrast, weaker emission features are observed at higher-energies when the beam is grazing to the spheres, corresponding to the excitation of Mie plasmons like those of isolated particles, which display an angular pattern approximately mimicking a dipole parallel to the surface. Our measurements are in excellent agreement with simulations, thus providing useful insight into gap plasmons arising from the interaction between metal particles and metal substrates that are relevant for molecular sensing applications.

We present resonant dielectric structures exhibiting arbitrarily large optical field enhancement, only limited by fabrication imperfections. Three different arrangements are investigated, based upon dielectric waveguides, dielectric particle arrays, and a combination of these two structures. Experimental confirmation of enhancement in a waveguide resonator is achieved by measuring the luminescence of quantum dots dispersed in the hot optical region of the structure. The performance of these systems can be readily controlled by simply changing geometrical parameters, which allows obtaining remarkable values of the intensity enhancement approaching 105 relative to the incident intensity over large volumes under feasible experimental conditions. This opens new avenues for all-optical switching and biosensing.

A pair of coupled gold nanorods excited by a beam of free electrons acts as a transmitting Hertzian antenna in the optical part of the spectrum. Significantly enhanced resonant emission is observed from the antenna when the electron beam is injected around the junction between the rods, where the local density of electromagnetic states is elevated.

We study the resonant modes of nanoscale disk resonators sustaining metal-insulator-metal (MIM) plasmons and demonstrate the versatility of these cavities to achieve ultrasmall cavity mode volume. Ag/SiO2/Ag MIM structures were made by thin-film deposition and focused ion beam milling with cavity diameters that ranged from d = 65-2000 nm. High-resolution two-dimensional cavity-mode field distributions were determined using cathodoluminescence imaging spectroscopy and are in good agreement with boundary element calculations. For the smallest cavities (d = 65-140 nm), the lowest order mode (m = 1, n = 1) is observed in the visible spectral range. This mode is of similar nature as the one in plasmonic particle dimers, establishing a natural connection between localized and traveling plasmon cavities. A cavity quality factor of Q = 16 is observed for the 105 nm diameter cavity, accompanied by a mode volume as small as 0.00033lamda(0)(3). The corresponding Purcell factor is 900, making these ultrasmall disk resonators ideal candidates for studies of enhanced spontaneous emission and lasing.

We introduce a theory to describe the interaction of swift electrons with strong evanescent light fields. This allows us to explain recent experimental results of multiple energy losses and gains for electrons passing near illuminated nanostructures. A complex evolution of the electron state over attosecond time scales is unveiled, giving rise to non-Poissonian distributions of multiphoton features in the electron spectra. Prospects for application to nanoscale-resolved transmission electron microscopy and spectroscopy are discussed.

We introduce a numerical technique to investigate the temperature distribution in arbitrarily complex plasmonic systems subject to external illumination. We perform both electromagnetic and thermodynamic calculations based upon a time-efficient boundary element method. Two kinds of plasmonic systems are investigated in order to illustrate the potential of such a technique. First, we focus on individual particles with various morphologies. In analogy with electrostatics, we introduce the concept of thermal capacitance. This geometry-dependent quantity allows us to assess the temperature increase inside a plasmonic particle from the sole knowledge of its absorption cross section. We present universal thermal-capacitance curves for ellipsoids, rods, disks, and rings. Additionally, we investigate assemblies of nanoparticles in close proximity and show that, despite its diffusive nature, the temperature distribution can be made highly non-uniform even at the nanoscale using plasmonic systems. A significant degree of nanoscale control over the individual temperatures of neighboring particles is demonstrated, depending on the external light wavelength and direction of incidence. We illustrate this concept with simulations of gold sphere dimers and chains in water. Our work opens new possibilities for selectively controlling processes such as local melting for dynamic patterning of textured materials, chemical and metabolic thermal activation, and heat delivery for producing mechanical motion with spatial precision in the nanoscale.

The confinement of surface-state electrons by a complex supramolecular network is studied with low-temperature scanning tunneling microscopy and rationalized by electronic structure calculations using a boundary element method. We focus on the self-assembly of dicarbonitrile-sexiphenyl molecules on Ag(111) creating an open kagomé topology tessellating the surface into pores with different size and symmetry. This superlattice imposes a distinct surface electronic structure modulation, as observed by tunneling spectroscopy and thus acts as a dichotomous array of quantum corrals. The inhomogenous lateral electronic density distribution in the chiral cavities is reproduced by an effective pseudopotential model. Our results demonstrate the engineering of ensembles of elaborate quantum resonance states by molecular self-assembly at surfaces.

We resolve the resonant whispering gallery modes of plasmonic subwavelength ring cavities defined by circular grooves patterned into a gold surface. An interesting interplay is observed between subwavelength confinement and guiding along the groove. Full spatial and spectroscopic information is directly obtained using cathodoluminescence, including details of the nanoscale intensity distribution (spatial resolution 11 +/- 8 nm). Excellent agreement between measurements and rigorous electromagnetic theory is obtained, thus allowing us to assess the symmetry, ordering, degree of confinement, and near-field enhancement of the modes with unprecedented detail.

The reflection of surface plasmon polaritons by deep linear grooves structured into gold surfaces is investigated with numerical finite-difference-in-time-domain as well as boundary-element-method calculations. Groove widths of 25 and 100 nm are studied, with depths as large as 500 nm. The reflection depends strongly on wavelength, groove depth, and width. By systematically varying these parameters and studying the field profiles in the grooves as well as mode dispersion, we relate the resonances of the reflectivity to resonant coupling of propagating planar plasmon modes to cavity modes inside the grooves. By careful design of the groove width and depth the reflectivity can be tuned to values up to at least 30% for either a narrow or wide band of wavelengths.

We study the angle and frequency dependence of sound transmission through water-immersed perforated aluminum plates. Three types of resonances are found to govern the acoustic properties of the plates: lattice resonances in periodic arrays, Fabry-Perot modes of the hole cavities, and elastic Lamb modes. The last two of them are still present in random arrays and have no parallel in optical transmission through holes. These modes are identified by comparing experiment with various levels of theoretical analysis, including full solution of the elasto-acoustic wave equations. We observe strong mixture of different transmission mechanisms, giving rise to unique acoustic behavior and opening new perspectives for exotic wave phenomena.

SERS permits identifying the nature of molecules in extremely low concentrations, but it is hindered by poor enhancement or low reproducibility. We demonstrate controllable approximately 10(10) signal amplification reaching the zeptomol detection limit for a nonresonant molecule by sandwiching the analyte between the tips of star-shaped gold nanoparticles and a planar gold surface using a simple synthetic procedure. This unprecedented control over light-intensity amplification opens a new avenue toward high-yield, fully reproducible, SERS-based, zeptomol detection and holds promise for nonlinear optics applications at the single-particle level.

We report highly efficient generation of propagating plasmons by electron beams in planar films, planar dielectric cavities, metallic wires, and nanoparticle waveguides. Electron-induced plasmon excitation is investigated in (1) gold thin films, both free-standing or supported on a silica substrate, (2) gold-silica-gold planar cavities, (3) gold nanowires, and (4) gold nanoparticle arrays. We obtain excitation yields as high as 10(- 2) plasmons per incoming electron over the visible and near-infrared range. Symmetric and antisymmetric plasmon modes are found to be more easily excited in thick and thin films, respectively, and in particular leaky plasmons in supported films are shown to be excited with very large probability exceeding one plasmon per electron. Generation of guided plasmons in metallic particle arrays is also proved to be attainable by aiming the electron at one end of the waveguide. The temporal evolution and spectral distribution of excited plasmons are discussed as well. Our results provide full support for the application of electron bombardment to excite propagating plasmons with high efficiency, thus solving the standing problem of plasmon generation at designated locations.

The rich structure of bright and dark surface-plasmon modes localized in individual and coupled gold nanoparticles is unveiled by electron-energy-loss spectroscopy performed in a scanning transmission electron microscope. Spatially resolved maps of surface-plasmon modes in the approximately 1.5-2.5 eV range (wavelengths approximately 500-800 nm), collected for individual nanorods, coupled nanorod dimers, and touching nanosphere dimers, are in excellent agreement with theory. Surface-plasmon maps constructed from the spatially and spectrally resolved energy-loss signals are shown to mimic rather well the near fields calculated for external illumination in the case of bright surface-plasmon modes (i.e., those coupling to external light). Dark surface-plasmon modes that cannot be excited by optical means are also found, and our electron probing technique provides further insight into their corresponding spatial distribution and symmetry, which are not accessible to any other existing techniques. Our results initiate the study of a whole set of new dark surface-plasmon modes that should become a source of new applications in sensing and microscopy but have escaped experimental scrutiny so far.

This tutorial review presents an overview of theoretical methods for predicting and understanding the optical response of gold nanoparticles. A critical comparison is provided, assisting the reader in making a rational choice for each particular problem, while analytical models provide insights into the effects of retardation in large particles and non-locality in small particles. Far- and near-field spectra are discussed, and the relevance of the latter in surface-enhanced Raman spectroscopy and electron energy-loss spectroscopy is emphasized.

We study the amplitude and phase signals detected in infrared scattering-type near field optical microscopy (s-SNOM) when probing a thin sample layer on a substrate. We theoretically describe this situation by solving the electromagnetic scattering of a dipole near a planar sample consisting of a substrate covered by thin layers. We perform calculations to describe the effect of both weakly (Si and SiO(2)) and strongly (Au) reflecting substrates on the spectral s-SNOM signal of a thin PMMA layer. We theoretically predict, and experimentally confirm an enhancement effect in the polymer vibrational spectrum when placed on strongly reflecting substrates. We also calculate the scattered fields for a resonant tip-substrate interaction, obtaining a dramatic enhancement of the signal amplitude and spectroscopic contrast of the sample layer, together with a change of the spectral line shape. The enhanced contrast opens the possibility to perform ultra-sensitive near field infrared spectroscopy of monolayers and biomolecules.

We study the light scattering and surface plasmon resonances of Au nanorods that are commonly used as optical nanoantennas in analogy to dipole radio antennas for chemical and biodetection field-enhanced spectroscopies and scanned-probe microscopies. With the use of the boundary element method, we calculate the nanorod near-field and far-field response to show how the nanorod shape and dimensions determine its optical response. A full mapping of the size (length and radius) dependence for Au nanorods is obtained. The dipolar plasmon resonance wavelength lambda shows a nearly linear dependence on total rod length L out to the largest lengths that we study. However, L is always substantially less than lambda/2, indicating the difference between optical nanoantennas and long-wavelength traditional lambda/2 antennas. Although it is often assumed that the plasmon wavelength scales with the nanorod aspect ratio, we find that this scaling does not apply except in the extreme limit of very small, spherical nanoparticles. The plasmon response depends critically on both the rod length and radius. Large (500 nm) differences in resonance wavelength are found for structures with different sizes but with the same aspect ratio. In addition, the plasmon resonance deduced from the near-field enhancement can be significantly red-shifted due to retardation from the resonance in far-field scattering. Large differences in near-field and far-field response, together with the breakdown of the simple scaling law must be accounted for in the choice and design of metallic lambda/2 nanoantennas. We provide a general, practical map of the resonances for use in locating the desired response for gold nanoantennas.

We report the observation of plasmonic modes of annular resonators in nanofabricated Ag and Au surfaces that are imaged by spectrally resolved cathodoluminescence. A highly focused 30 keV electron beam is used to excite localized surface plasmons that couple to collective resonant modes of the nanoresonators. We demonstrate unprecedented resolution of plasmonic mode excitation and by combining these observations with full-field simulations find that cathodoluminescence in plasmonic nanostructures is most efficiently excited at positions corresponding to antinodes in the modal electric field intensity.

The plasmon analog of the self-imaging Talbot effect is described and theoretically analyzed. Rich plasmon carpets containing hot spots are shown to be produced by a row of periodically-spaced surface features. A row of holes drilled in a metal film and illuminated from the back side is discussed as a realizable implementation of this concept. Self-images of the row are produced, separated from the original one by distances up to several hundreds of wavelengths in the examples under consideration. The size of the image focal spots is close to half a wavelength and the spot positions can be controlled by changing the incidence direction of external illumination, suggesting the possibility of using this effect (and its extension to non-periodic surface features) for far-field patterning and for long-distance plasmon-based interconnects in plasmonic circuits, energy transfer, and related phenomena.

Adaptive shaping of the phase and amplitude of femtosecond laser pulses has been developed into an efficient tool for the directed manipulation of interference phenomena, thus providing coherent control over various quantum-mechanical systems. Temporal resolution in the femtosecond or even attosecond range has been demonstrated, but spatial resolution is limited by diffraction to approximately half the wavelength of the light field (that is, several hundred nanometres). Theory has indicated that the spatial limitation to coherent control can be overcome with the illumination of nanostructures: the spatial near-field distribution was shown to depend on the linear chirp of an irradiating laser pulse. An extension of this idea to adaptive control, combining multiparameter pulse shaping with a learning algorithm, demonstrated the generation of user-specified optical near-field distributions in an optimal and flexible fashion. Shaping of the polarization of the laser pulse provides a particularly efficient and versatile nano-optical manipulation method. Here we demonstrate the feasibility of this concept experimentally, by tailoring the optical near field in the vicinity of silver nanostructures through adaptive polarization shaping of femtosecond laser pulses and then probing the lateral field distribution by two-photon photoemission electron microscopy. In this combination of adaptive control and nano-optics, we achieve subwavelength dynamic localization of electromagnetic intensity on the nanometre scale and thus overcome the spatial restrictions of conventional optics. This experimental realization of theoretical suggestions opens a number of perspectives in coherent control, nano-optics, nonlinear spectroscopy, and other research fields in which optical investigations are carried out with spatial or temporal resolution.

The diffractive properties of gold films with a periodic lattice of sub-micron voids beneath the surface are investigated. It has been shown that nanoporous metal surfaces exhibit frequency-selective non-dispersive diffraction enhanced by Mie plasmons in nanovoids, which leads to absolute angular tolerance of the diffracted beam intensity that can be useful for a variety of applications covering angle-tolerant optical filters, deflectors, absorbers, and beam splitters. Diffraction spectra are measured and calculated to support these conclusions, showing good qualitative agreement.

The response of gold nanoparticle dimers is studied theoretically near and beyond the limit where the particles are touching. As the particles approach each other, a dominant dipole feature is observed that is pushed into the infrared due to interparticle coupling and that is associated with a large pileup of induced charge in the interparticle gap. The redshift becomes singular as the particle separation decreases. The response weakens for very small separation when the coupling across the interparticle gap becomes so strong that dipolar oscillations across the pair are inhibited. Lowerwavelength, higher-order modes show a similar separation dependence in nearly touching dimers. After touching, singular behavior is observed through the emergence of a new infrared absorption peak, also accompanied by huge charge pileup at the interparticle junction, if initial interparticle-contact is made at a single point. This new mode is distinctly different from the lowest mode of the separated dimer. When the junction is made by contact between flat surfaces, charge at the junction is neutralized and mode evolution is continuous through contact. The calculated singular response explains recent experiments on metallic nanoparticle dimers and is relevant in the design of nanoparticle-based sensors and plasmon circuits.

A modified seeded growth process has been used for the controlled synthesis of quasispherical, CTAB-stabilized gold nanoparticles from 12 up to 180 nm with narrow size distributions. The UV-visible spectra of the aqueous colloids show distinct bands corresponding to dipole and quadrupole plasmon modes, for diameters above 100 nm, in close agreement with predictions based on Mie theory. The assignment of the modes is demonstrated by calculation of near field enhancement maps based on the boundary element method. Apart from other applications, since absorption is drastically reduced above 600 nm, while scattering is largely increased, these particles open new possibilities for construction of highly efficient photonic structures.

We study the optical plasmonic properties of metal surfaces which have a periodic lattice of voids buried immediately beneath their flat upper surface. Light reflection spectra calculated in the framework of a self-consistent electromagnetic multiple-scattering layer-KKR approach exhibit two types of plasmon resonances originating from the excitation of different plasmon modes: surface plasmon-polaritons propagating on the planar surface of metal and Mie plasmons localized in the buried voids. Coupling between these two types of plasma oscillation leads to an enhancement of the surface plasmon-polariton resonances even for close-packed void lattices. Our theoretical model quantitatively agrees with experimental results, demonstrating that planar surfaces can exhibit strong plasmonic field enhancements.

Femtosecond laser pulse shaping techniques have been restricted to propagating transverse electromagnetic waves. We present a scheme for pulse shaping of optical near fields based on the excitation of longitudinal electromagnetic fields with polarization-shaped light pulses. By solving Maxwell's equations for a model nanostructure, i.e., a scanning tunneling microscope tip, with help from the boundary-element method, we demonstrate that the electric field vector oscillates in a complex yet controllable fashion in three dimensions. Many applications are envisioned because literally another dimension in the optimal control of light-matter interaction is accessible.