Abstract. Nanoantennas for visible and infrared radiation can strongly enhance the interaction of light with nanoscale matter by their ability to efficiently link propagating and spatially localized optical fields. This ability unlocks an enormous potential for applications ranging from nanoscale optical microscopy and spectroscopy over solar energy conversion, integrated optical nanocircuitry, opto-electronics and density-ofstates engineering to ultra-sensing as well as enhancement of optical nonlinearities. Here we review the current understanding of metallic optical antennas based on the background of both well-developed radiowave antenna engineering and plasmonics. In particular, we discuss the role of plasmonic resonances on the performance of nanoantennas and address the influence of geometrical parameters imposed by nanofabrication. Finally, we give a brief account of the current status of the field and the major established and emerging lines of investigation in this vivid area of research.

Deep subwavelength integration of high-definition plasmonic nanostructures is of key importance in the development of future optical nanocircuitry for high-speed communication, quantum computation and lab-on-a-chip applications. To date, the experimental realization of proposed extended plasmonic networks consisting of multiple functional elements remains challenging, mainly because of the multi-crystallinity of commonly used thermally evaporated gold layers. This can produce structural imperfections in individual circuit elements that drastically reduce the yield of functional integrated nanocircuits. In this paper we demonstrate the use of large (>100 μm(2)) but thin (<80 nm) chemically grown single-crystalline gold flakes that, after immobilization, serve as an ideal basis for focused ion beam milling and other top-down nanofabrication techniques on any desired substrate. Using this methodology we obtain high-definition ultrasmooth gold nanostructures with superior optical properties and reproducible nano-sized features over micrometre-length scales. Our approach provides a possible solution to overcome the current fabrication bottleneck and realize high-definition plasmonic nanocircuitry.

ABSTRACT:Boosting nonlinear frequency conversion in extremely confined volumes remains a key challenge in nano-optics, nanomedicine, photocatalysis, and background-free biosensing. To this aim, field enhancements in plasmonic nanostructures are often exploited to effectively compensate for the lack of phase-matching at the nanoscale. Second harmonic generation (SHG) is, however, strongly quenched by the high degree of symmetry in plasmonic materials at the atomic scale and in nanoantenna designs.Here, we devise a plasmonic nanoantenna lacking axial symmetry, which exhibits spatial and frequency mode overlap at both the excitation and the SHG wavelengths. The effective combination of these features in a single device allows obtaining unprecedented SHG conversion efficiency. Our results shed new light on the optimization of SHG at the nanoscale, paving the way to new classes of nanoscale coherent light sources and molecular sensing devices based on nonlinear plasmonic platforms.

An experimentally realizable prototype nanophotonic circuit consisting of a receiving and an emitting nano antenna connected by a two-wire optical transmission line is studied using finite-difference time-and frequency-domain simulations. To optimize the coupling between nanophotonic circuit elements we apply impedance matching concepts in analogy to radio frequency technology. We show that the degree of impedance matching, and in particular the impedance of the transmitting nano antenna, can be inferred from the experimentally accessible standing wave pattern on the transmission line. We demonstrate the possibility of matching the nano antenna impedance to the transmission line characteristic impedance by variations of the antenna length and width realizable by modern microfabrication techniques. The radiation efficiency of the transmitting antenna also depends on its geometry but is independent of the degree of impedance matching. Our systems approach to nanophotonics provides the basis for realizing general nanophotonic circuits and a large variety of derived novel devices. 3 IntroductionMiniaturization and packaging density of integrated optics based on dielectrics is limited by the wavelength scale modal profiles of guided modes. 1 In contrast, plasmonic modes on noble metal nanostructures offer strong subwavelength confinement and therefore promise the realization of nanometer-scale integrated optical circuitry. 2,3 A truly subwavelength integrated photonic circuit based on plasmonic nano structures will generally consist of (i) a set of optical antennas 4,5,6,7 to efficiently excite specific local modes by far-field radiation, (ii) a very small footprint network of optical transmission lines 8 (OTLs) to distribute and manipulate plasmonic excitations, 9,10,11,12,13,14,15,16 and (iii) another set of optical antennas to efficiently convert local modes into propagating photons. The properties of metal nanoparticle chains, 17,18 metal nanowires, 19,20 line defects in plasmonic photonic crystals, 21 as well as gaps 22,23,24, and v-shaped grooves 9,25,26 in extended metal films have been explored as subwavelength waveguides for light.Efficient launching of specific guided modes on such structures is difficult since it requires matching of both, the small mode extension and the k-vector. It has been shown recently that efficient coupling between far-field photons and subwavelength spatial domains can be achieved using resonant optical antennas. 5,7,27,28,29,30,31 However, so far optical antennas have mostly been studied as isolated elements. Here we consider optical antennas as integral parts of an experimentally realizable integrated nanophotonic circuit where they act as efficient interfacing elements between propagating photons and guided modes of a plasmonic two-wire transmission line. We show by simulations that the principles of classical transmission line theory, e.g. impedance matching, 32 between the two-wire OTL and dipole antennas are fully applicable at optical frequencies. We further suggest tha...

The number of eigenmodes in plasmonic nanostructures increases with complexity due to mode hybridization, raising the need for efficient mode characterization and selection. Here we experimentally demonstrate direct imaging and selective excitation of the "bonding" and "antibonding" plasmon mode in symmetric dipole nanoantennas using confocal two-photon photoluminescence mapping. Excitation of a high-qualityfactor antibonding resonance manifests itself as a two-lobed pattern instead of the single spot observed for the broad "bonding" resonance, in accordance with numerical simulations. The two-lobed pattern is observed due to the fact that excitation of the antibonding mode is forbidden for symmetric excitation at the feedgap, while concomitantly the mode energy splitting is large enough to suppress excitation of the "bonding" mode. The controlled excitation of modes in strongly coupled plasmonic nanostructures is mandatory for efficient sensors, in coherent control as well as for implementing well-defined functionalities in complex plasmonic devices. IntroductionPlasmonic nanostructures consisting of particular arrangements of closely spaced resonant particles are of great interest since they offer a variety of eigenmodes that evolve due to mode hybridization [1]. Characterization and well-defined excitation of such eigenmodes is important in order to achieve welldefined functionality in devices [2,3] and to successfully apply techniques of coherent control [4][5][6][7]. Nanoantennas consisting of two strongly coupled particles can serve as a model system to study the impact of mode selectivity [6,8,9]. Upon illumination nanoantennas confine and enhance optical fields [10,11] and can therefore be used to tailor the interaction of light with nanomatter [12]. Various applications of nanoantennas have been proposed and experimentally demonstrated, including enhanced single-emitter fluorescence [13][14][15], enhanced Raman scattering [16,17], near-field polarization engineering [18][19][20], high-harmonic generation [21,22], as well as applications in integrated optical nanocircuitry [23,24]. The longitudinal resonances of a symmetric dipole antenna can be understood in terms of hybridization of the longitudinal resonances of individual antenna arms, caused by the coupling over the narrow feedgap [25,26]. Such coupling causes a mode splitting into a lower-energy "bonding" mode and a higher-energy "antibonding" mode, respectively (Fig. 1). Limited by the uncertainty of conventional nanofabrication, it is often difficult to fabricate antenna arrays with a reproducible gap size below 20 nm, which is necessary to achieve significant energy splitting between the bonding and the antibonding mode. As a result, the existence of the antibonding antenna resonance has hardly been considered, although it may offer interesting opportunities, such as impedance tunability, a high quality factor due to its weakly radiative nature, the launching of propagating plasmon modes with increased propagation lengths [27] and spatial select...

Midinfrared plasmonic sensing allows the direct targeting of unique vibrational fingerprints of molecules. While gold has been used almost exclusively so far, recent research has focused on semiconductors with the potential to revolutionize plasmonic devices. We fabricate antennas out of heavily doped Ge films epitaxially grown on Si wafers and demonstrate up to 2 orders of magnitude signal enhancement for the molecules located in the antenna hot spots compared to those located on a bare silicon substrate. Our results set a new path toward integration of plasmonic sensors with the ubiquitous CMOS platform.

2The interaction of light and matter, i.e. absorption and emission of photons, can be considerably enhanced in the presence of strongly localized and therefore highly intense optical near fields 1 .Plasmonic antennas consisting of pairs of closely spaced metal nano particles have gained much attention in this context since they provide the possibility to strongly concentrate optical fields into the gap between the two metal particles [2][3][4] . Pairs of closely spaced metal nanoparticles supporting plasmonic gap resonances consequently find broad applications, e.g. in single-emitter surfaceenhanced spectroscopy 5,6 , quantum optics 7 , extreme nonlinear optics 8-10 , optical trapping 11 , metamaterials 12, 13 and molecular opto-electronics 14 .The success of metal-insulator-metal structures is based on two fundamental properties of their anti-symmetric electromagnetic gap modes. (i) As a direct consequence of the boundary conditions, the dominating field components normal to the metal-dielectric interfaces are sizable only inside the dielectric gap. This means that for anti-symmetric gap modes the achievable field confinement is not limited by the skin depth of the metal, but is solely determined by the actual size of the gap. (ii) Since the free electrons of the metal respond resonantly to an external optical frequency field, enormous surface charge accumulations, accompanied by ultra-intense optical near fields, will occur. In addition, with decreasing gap width, stronger attractive coulomb forces 4 across the gap lead to further surface-charge accumulation and a concomitantly increased near-field intensity enhancement. We therefore conclude that an experimental realization of atomic-scale concentration of electromagnetic fields at visible frequencies is possible but it requires atomic-scale shape control of the field-confining structure, i.e. the gap, as well as a careful assignment and selection of suitable optical modes.Here we achieve atomic-scale confinement of electromagnetic fields at visible frequencies by combining for the first time both atomic-scale shape control of the field confining structure 15 as well as a careful selection and assignment of suitable optical modes [16][17][18] . We study single-crystalline nanorods which self-assemble into side-by-side aligned dimers with gap widths below 0.5 nm. Sideby-side aligned nanorod dimers possess various distinguishable symmetric and anti-symmetric 3 modes in the visible range 19 . In contrast to previous work 20-22 we demonstrate full control over symmetric and anti-symmetric optical modes by means of white-light scattering experiments. We experimentally demonstrate the presence of atomic-scale light confinement in these structures by observing an extreme > 800 meV hybridization splitting of corresponding symmetric and antisymmetric dimer modes. Our results open new perspectives for atomically-resolved spectroscopic imaging, deeply nonlinear optics and attosecond physics, cavity optomechanics and ultra-sensing as well as quantum optics.To obtain nano...

The surface wetting of five biopolymers, used as coating materials for a plastic film, was monitored over a span of 8 min by means of the optical contact angle technique. Because most of the total variation was observed to occur during the first 60 s, we decided to focus on this curtailed temporal window. Initial contact angle values (θ(0)) ranged from ∼91° for chitosan to ∼30° for pullulan. However, the water drop profile began to change immediately following drop deposition for all biocoatings, confirming that the concept of water contact angle equilibrium is not applicable to most biopolymers. First, a three-parameter decay equation [θ(t) = θ(0) exp(kt(n))] was fit to the experimental contact angle data to describe the kinetics of the contact angle change for each biocoating. Interestingly, the k constant correlated well with the contact angle evolution rate and the n exponent seemed to be somehow linked to the physicochemical phenomena underlying the overall kinetics process. Second, to achieve a reliable description of droplet evolution, the contact angle (CA) analysis was coupled with image analysis (IA) through a combined geometric/trigonometric approach. Absorption and spreading were the key factors governing the overall mechanism of surface wetting during the 60 s analysis, although the individual quantification of both phenomena demonstrated that spreading provided the largest contribution for all biopolymers, with the only exception of gelatin, which showed two quasi-equivalent and counterbalancing effects. The possible correlation between these two phenomena and the topography of the biopolymer surfaces are then discussed on the basis of atomic force microscopy analyses.