Antonio I. Fernández-Domínguez

Plasmonic Nanoantennas: Fundamentals and Their Use in Controlling the Radiative Properties of Nanoemitters

When light interacts with a metal nanoparticle (NP), its conduction electrons can be driven by the incident electric field in collective oscillations known as localized surface plasmon resonances (LSPRs). These give rise to a drastic alteration of the incident radiation pattern and to striking effects such as the subwavelength localization of electromagnetic (EM) energy, the formation of high intensity hot spots at the NP surface, or the directional scattering of light out of the structure. LSPRs can also couple to the EM fields emitted by molecules, atoms, or quantum dots placed in the vicinity of the NP, leading in turn to a strong modification of the radiative and nonradiative properties of the emitter. Since LSPRs enable an efficient transfer of EM energy from the near to the far-field of metal NPs and vice versa, we can consider plasmonic nanostructures as nanoantennas, because they operate in a similar way to radio antennas but at higher frequencies. Typically, plasmonic nanoantennas at optical frequencies are made of gold and silver due to their goodmetallic properties and low absorption. Controlling and guiding light has been one of science’s most influential achievements. It affects everyday life in many ways, such as the development of telescopes, microscopes, spectrometers, and optical fibers, to name but a few. These examples exploit the wave nature of light and are based on the reflection, refraction and diffraction of light by optical elements such as mirrors, lenses or gratings. However, the wave nature of light limits the resolution to which an object can be imaged, as well as the size of the transverse cross section of efficient guiding structures to the wavelength dimension. Plasmonic resonances in nanoantennas overcome these constraints, allowing unprecedented control of light-matter interactions within subwavelength volumes (i.e., within the nanoscale at optical frequencies). Such properties have attracted much interest lately, due to the implications they have both in fundamental research and in technological applications. Metal NPs have been used since antiquity. Due to their strong scattering properties in the visible range, they show attractive colors. One of their first applications, dating back to the Roman Empire more than 2000 years ago, was as a colorant for clothing. In art, they were used to stain window glass and ceramics. Obviously, it was not known then that the colorants being used contained metal NPs or that the spectacular colors were due to the excitation of LSPRs. The first reported intentional production of metal NPs dates from 1857, when Faraday synthesized gold colloids. However, at the time there was not much interest in understanding the physics behind the optical properties of colloids due to the impossibility of synthesizing NPs with well-controlled shapes and sizes, as well as the lack of accurate detection techniques. The first theoretical work on the scattering of light by particles smaller than the incident wavelength was carried out by Lord Rayleigh at the end of the 19th century. He analyzed the diffusion of light by diluted gases, and his theory explained physical phenomena such as the blueness of the sky, the redness of the sunset, or the yellow color of the sun. Mie took the next step forward by deriving an analytical solution to Maxwell’s equations to describe the interaction of light with spheres of arbitrary radius and composition. Subsequently, based on the results of Rayleigh and Mie, Gans considered elliptical geometries. He demonstrated that the optical response of metal NPs is

Probing the Ultimate Limits of Plasmonic Enhancement

Boundaries on Plasmonic Excitations The localization of optical fields within a metal nanostructure can achieve strengths that are orders of magnitude greater than that of the incident field. This focusing and enhancement of the optical field maybe useful in sensing, nonlinear optics, and optical scattering applications. In probing the properties of metallic nanoparticles, Ciracì et al. (p. 1072; see the cover) show that the enhancement is limited by the electronic response of the metal, which has implications for the ultimate performance of nanophotonic systems. The nonlocal dielectric response of metals places a fundamental limit on the performance of plasmonic optical devices. Metals support surface plasmons at optical wavelengths and have the ability to localize light to subwavelength regions. The field enhancements that occur in these regions set the ultimate limitations on a wide range of nonlinear and quantum optical phenomena. We found that the dominant limiting factor is not the resistive loss of the metal, but rather the intrinsic nonlocality of its dielectric response. A semiclassical model of the electronic response of a metal places strict bounds on the ultimate field enhancement. To demonstrate the accuracy of this model, we studied optical scattering from gold nanoparticles spaced a few angstroms from a gold film. The bounds derived from the models and experiments impose limitations on all nanophotonic systems.

Plasmonic light-harvesting devices over the whole visible spectrum.

On the basis of conformal transformation, a general strategy is proposed to design plasmonic nanostructures capable of an efficient harvesting of light over a broadband spectrum. The surface plasmon modes propagate toward the singularity of these structures where the group velocity vanishes and energy accumulates. A considerable field enhancement and confinement is thus expected. Radiation losses are also investigated when the structure dimension becomes comparable to the wavelength.

Nanoplasmonics: Classical down to the Nanometer Scale

We push the fabrication limit of gold nanostructures to the exciting sub-nanometer regime, in which light-matter interactions have been anticipated to be strongly affected by the quantum nature of electrons in metals. Doing so allows us to (1) evaluate the validity of classical electrodynamics to describe plasmonic effects at this length scale and (2) witness the gradual (instead of sudden) evolution of plasmon modes when two gold nanoprisms are brought into contact. Using electron energy-loss spectroscopy and transmission electron microscope imaging, we investigated nanoprisms separated by gaps of only 0.5 nm and connected by conductive bridges as narrow as 3 nm. Good agreement of our experimental results with electromagnetic calculations and LC circuit models evidence the gradual evolution of the plasmonic resonances toward the quantum coupling regime. We demonstrate that down to the nanometer length scales investigated classical electrodynamics still holds, and a full quantum description of electrodynamics phenomena in such systems might be required only when smaller gaps of a few angstroms are considered. Our results show also the gradual onset of the charge-transfer plasmon mode and the evolution of the dipolar bright mode into a 3λ/2 mode as one literally bridges the gap between two gold nanoprisms.

High-resolution mapping of electron-beam-excited plasmon modes in lithographically defined gold nanostructures.

We demonstrate the use of high-resolution electron beam lithography to fabricate complex nanocavities with nanometric spatial and positional control. The plasmon modes of these nanostructures are then mapped using electron energy-loss spectroscopy in a scanning transmission electron microsope. This powerful combination of patterning and plasmon mapping provides direct experimental verification to theoretical predictions of plasmon hybridization theory in complex metal nanostructures and allows the determination of the full mode spectrum of such cavities.

Domino plasmons for subwavelength terahertz circuitry.

A new approach for the spatial and temporal modulation of electromagnetic fields at terahertz frequencies is presented. The waveguiding elements are based on plasmonic and metamaterial notions and consist of an easy-to-manufacture periodic chain of metallic box-shaped elements protruding out of a metallic surface. It is shown that the dispersion relation of the corresponding electromagnetic modes is rather insensitive to the waveguide width, preserving tight confinement and reasonable absorption loss even when the waveguide transverse dimensions are well in the subwavelength regime. This property enables the simple implementation of key devices, such as tapers and power dividers. Additionally, directional couplers, waveguide bends, and ring resonators are characterized, demonstrating the flexibility of the proposed concept and the prospects for terahertz applications requiring high integration density.

Controlling Light Localization and Light-Matter Interactions with Nanoplasmonics

Nanoplasmonics is the emerging research field that studies light-matter interactions mediated by resonant excitations of surface plasmons in metallic nanostructures. It allows the manipulation of the flow of light and its interaction with matter at the nanoscale (10(-9) m). One of the most promising characteristics of plasmonic resonances is that they occur at frequencies corresponding to typical electronic excitations in matter. This leads to the appearance of strong interactions between localized surface plasmons and light emitters (such as molecules, dyes, or quantum dots) placed in the vicinity of metals. Recent advances in nanofabrication and the development of novel concepts in theoretical nanophotonics have opened the way to the design of structures aimed to reduce the lifetime and enhance the decay rate and quantum efficiency of available emitters. In this article, some of the most relevant experimental and theoretical achievements accomplished over the last several years are presented and analyzed.

Revealing Plasmonic Gap Modes in Particle-on-Film Systems Using Dark-Field Spectroscopy

Polarization-controlled excitation of plasmonic modes in nanometric Au particle-on-film gaps is investigated experimentally using single-particle dark-field spectroscopy. Two distinct geometries are explored: nanospheres on top of and inserted in a thin gold film. Numerical simulations reveal that the three resonances arising in the scattering spectra measured for particles on top of a film originate from highly confined gap modes at the interface. These modes feature different azimuthal characteristics, which are consistent with recent theoretical transformation optics studies. On the other hand, the scattering maxima of embedded particles are linked to dipolar modes having different orientations and damping rates. Finally, the radiation properties of the particle-film gap modes are studied through the mapping of the scattered power within different solid angle ranges.

Surface plasmons and nonlocality: a simple model.

Surface plasmons on metals can concentrate light into subnanometric volumes and on these near atomic length scales the electronic response at the metal interface is smeared out over a Thomas-Fermi screening length. This nonlocality is a barrier to a good understanding of atomic scale response to light and complicates the practical matter of computing the fields. In this Letter, we present a local analogue model and show that spatial nonlocality can be represented by replacing the nonlocal metal with a composite material, comprising a thin dielectric layer on top of a local metal. This method not only makes possible the quantitative analysis of nonlocal effects in complex plasmonic phenomena with unprecedented simplicity and physical insight, but also offers great practical advantages in their numerical treatment.

Nonlocal Effects in the Nanofocusing Performance of Plasmonic Tips

The nanofocusing performance of plasmonic tips is studied analytically and numerically. The effects of electron-electron interactions in the dielectric response of the metal are taken into account through the implementation of a nonlocal, spatially dispersive, hydrodynamic permittivity. We demonstrate that spatial dispersion only slightly modifies the device parameters which maximize its field enhancement capabilities. The interplay between nonlocality, tip bluntness, and surface roughness is explored. We show that, although spatial dispersion reduces the field enhancement taking place at the structure apex, it also diminishes the impact that geometric imperfections have on its performance.