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Nonlinear optical phenomena enable novel photonic and optoelectronic applications. Especially, metallic nanoparticles and thin films with nonlinear optical properties offer the potential for micro-optical system integration. For this purpose, new nonlinear materials need to be continuously identified, investigated, and utilized for nonlinear optical applications. While noble-metal nanoparticles, nanostructures, and thin films of silver and gold have been widely studied, iridium (Ir) nanoparticles and ultrathin films have not been investigated for nonlinear optical applications yet. Here, we present a combined theoretical and experimental study on the linear and nonlinear optical properties of iridium nanoparticles deposited via atomic layer deposition (ALD). Linear optical constants, such as the effective refractive index and extinction coefficient, were evaluated at different growth stages of nanoparticle formation. Both linear and nonlinear optical properties of these Ir ALD coatings were calculated theoretically using the Maxwell Garnett theory. The third-order susceptibility of iridium nanoparticle samples was experimentally investigated using the z-scan technique. According to the experiment, for an Ir ALD coating with 45 cycles resulting in iridium nanoparticles, the experimentally determined nonlinear third-order susceptibility is about χIr(3) = (2.4 − i2.1) × 10−17 m2/V2 at the fundamental wavelength of 700 nm. The theory fitted to the experimental results predicts a 5 × 106-fold increase around 230 nm. This strong increase is due to the proximity to the Mie resonance of iridium nanoparticles.

A theoretical approach to simulate the light scattering from multilayers of thin films with one rough surface is presented. Image processing is applied to calculate absorption for samples with different surface morphologies.

Second harmonic generation is enhanced at the surface lattice resonance in plasmonic nanoparticle arrays. We carried out a parametric investigation on two-dimensional lattices composed of gold nanobars where the centrosymmetry is broken at oblique incidence. We study the influence of the periodicity, the incidence angle and the direction of the linear input polarization on the second harmonic generation. Excitation of the surface lattice resonance either at the fundamental or second harmonic wavelength, achieved by varying the incidence angle, enhance the conversion efficiency. As a special case, we demonstrate that both the wavelengths can be simultaneously in resonance for a specific period of the lattice. In this double resonant case, maximum second harmonic power is achieved., Comment: 19 pages, 18 figures

The role played by surface lattice resonances (SLRs) in modulating the Second-Harmonic Generation (SHG) is addressed by measuring the nonlinear response of plas-monic metasurfaces for several lattice parameters.

The question of how energy resources can be efficiently used is likewise of fundamental and technological interest. In this opinion, we give a brief overview on developments of harvesting solar energy across different length scales and address some strategies to tackle economic and ecological challenges, in particular with a view to sustainability and toward a circular economy. On the mesoscopic scale, the emergence of thermodynamic laws in open quantum systems is of central importance and how they can be employed for efficient quantum thermal machines and batteries. The broad tunability of band gaps in quantum dot systems makes them attractive for hybrid photovoltaic devices. Complementary, machine learning-aided band gap engineering and the high-throughput screening of novel materials assist with improving absorption characteristics. On the device scale, hybrid concepts of optical control via metasurfaces enable a multitude of functionalities such as a directed re-emission of embedded photoluminescent materials or field enhancement effects from nanostructures. Advanced techniques in computational nanophotonics concern a topology optimization of nanostructured layers together with multiobjective optimization toward specific light management tasks. On the industrial level, modern manufacturers explore 3D printing and flexible solar cell platforms obtained from roll-to-roll technologies. The remote control of solar parks through applications via the Internet of Things opens up new strategies to expand to difficult terrain where human interaction is only required to a limited extent.

Particle layers employing conductive transition metal nitrides have been proposed as possible alternative plasmonic materials for photovoltaic applications due to their reduced losses compared to metal nanostructures. We critically compare the potential photocurrent gain from an additional layer made of nanopillars of nitrides with other material classes obtained in an optimized c-Si baseline solar cell, considering an experimental doping profile. A relative photocurrent gain enhancement of on average 5% to 10% is observed, achieving for a few scenarios around 30% gain. The local field enhancement is moderate around the resonances for nitrides which spread over the whole ultraviolet and visible range. We can characterize two types of nitrides: nitrides for which the shading effect remains a problem similar to for metals, and others which behave like dielectric scatterers with high photocurrent gain.

We have investigated the plasmonic enhancement of the radiation field at various nanostructured multilayer devices, that may be applied in surface enhanced Raman spectroscopy. We apply an image dipole method to describe the effect of surface morphology on the field enhancement in a quasistatic limit. In particular, we compare the performance of a nanostructured silver surface and a layered silver-gold hybrid device. It is found that localized surface plasmon states (LSP) provide a high field enhancement in silver-gold hybrid devices, where symmetry breaking due to surface-defects is a supporting factor. These results are compared to those obtained for multi-shell nanoparticles of spherical symmetry. Calculated enhancement factors are discussed on the background of recent experimental data., 8 pages, 6 figures

I discuss the plasmonic properties of charged fluids introducing a two-fluid model for spherical microparticles in analogy to metal particles. Additional degrees of freedom (ion mass, ion charge, concentration) allow a wide range of resonance frequencies. I include commonly neglected charge interactions thus deriving nonlocal Mie coefficients applicable for either ions or metals and demonstrate the impact of nonlocality in these different spectral regimes. Ionic microspheres and chains are studied and compared to solid metal nanoparticles.

We study strong optical coupling of metal nanoparticle arrays with dielectric substrates. Based on the Fermi Golden Rule, the particle&ndash, substrate coupling is derived in terms of the photon absorption probability assuming a local dipole field. An increase in photocurrent gain is achieved through the optical coupling. In addition, we describe light-induced, mesoscopic electron dynamics via the nonlocal hydrodynamic theory of charges. At small nanoparticle size (&lt, 20 nm), the impact of this type of spatial dispersion becomes sizable. Both absorption and scattering cross sections of the nanoparticle are significantly increased through the contribution of additional nonlocal modes. We observe a splitting of local optical modes spanning several tenths of nanometers. This is a signature of semi-classical, strong optical coupling via the dynamic Stark effect, known as Autler&ndash, Townes splitting. The photocurrent generated in this description is increased by up to 2%, which agrees better with recent experiments than compared to identical classical setups with up to 6%. Both, the expressions derived for the particle&ndash, substrate coupling and the additional hydrodynamic equation for electrons are integrated into COMSOL for our simulations.

Two-dimensional arrays of hollow nanotubes made of TiO 2 are a promising platform for sensing, spectroscopy and light harvesting applications. Their straightforward fabrication via electrochemical anodization, growing nanotube pillars of finite length from a Ti foil, allows precise tailoring of geometry and, thus, material properties. We theoretically investigate these photonic crystal structures with respect to reduction of front surface reflection, achievable field enhancement, and photonic bands. Employing the Rigorous Coupled Wave Analysis (RCWA), we study the optical response of photonic crystals made of thin-walled nanotubes relative to their bare Ti foil substrate, including under additional charge carrier doping which might occur during the growth process.

Two-dimensional arrays of hollow nanotubes made of TiO 2 are a promising platform for sensing, spectroscopy and light harvesting applications. Their straightforward fabrication via electrochemical anodization, growing nanotube pillars of finite length from a Ti foil, allows precise tailoring of geometry and, thus, material properties. We theoretically investigate these photonic crystal structures with respect to reduction of front surface reflection, achievable field enhancement, and photonic bands. Employing the Rigorous Coupled Wave Analysis (RCWA), we study the optical response of photonic crystals made of thin-walled nanotubes relative to their bare Ti foil substrate, including under additional charge carrier doping which might occur during the growth process.

We demonstrate that the direct application of numerical packets like Comsol to plasmonic effect in solar cells metallically modified in nano-scale may be strongly inaccurate if quantum corrections are neglected. The near-field coupling of surface plasmons in metallic nanoparticles deposited on the top of a solar cell with band electrons in a semiconductor substrate strongly enhances the damping of plasmons in metallic components, which is not accounted for in standard numerical packets using the Drude type dielectric function for metal (taken from measurements in bulk or in thin layers) as the prerequisite for the numerical e-m field calculus. Inclusion of the proper corrections to plasmon damping causes additional enhancement of the plasmon-induced photo-effect efficiency growth of a metalized photo-diode by ten percent, at least, in comparison to only effect induced by the electric field concentration near metallic nanoparticles. This happens to be consistent with the experimental observations which cannot be explained by only local increases of the electrical field near the curvature of metallic nanoparticles determined by a finite-element solution of the Maxwell&ndash, Fresnel boundary problem as given by a numerical system like Comsol. The proper damping rate for plasmons can be identified by application of the Fermi Golden Rule approach to the plasmon-band electron coupling. We demonstrate this effect including the material and size dependence in two types of solar cells, multi-crystalline Si and CIGS (copper-indium-gallium-diselenide) as idealized photo-diode semiconductor substrate modified by various metallic nano-particles, in comparison to the experimental data and Comsol simulation.

Photovoltaics is amongst the most important technologies for renewable energy sources, and plays a key role in the development of a society with a smaller environmental footprint. Key parameters for solar cells are their energy conversion efficiency, their operating lifetime, and the cost of the energy obtained from a photovoltaic system compared to other sources. The optimization of these aspects involves the exploitation of new materials and development of novel solar cell concepts and designs. Both theoretical modeling and characterization of such devices require a comprehensive view including all scales from the atomic to the macroscopic and industrial scale. The different length scales of the electronic and optical degrees of freedoms specifically lead to an intrinsic need for multiscale simulation, which is accentuated in many advanced photovoltaics concepts including nanostructured regions. Therefore, multiscale modeling has found particular interest in the photovoltaics community, as a tool to advance the field beyond its current limits. In this article, we review the field of multiscale techniques applied to photovoltaics, and we discuss opportunities and remaining challenges. © T. Abu Hamed et al., published by EDP Sciences, 2018., European Cooperation in Science and Technology: MP1406, The authors are grateful for the financial support by the COST Action MP1406 “MultiscaleSolar.”

We present the fabrication of TiO

Spatial interaction effects between charge carriers in ionic systems play a sizable role beyond a classical Maxwellian description. We develop a nonlocal, two-fluid, hydrodynamic theory of charges and study ionic plasmon effects, i. e. collective charge oscillations in electrolytes. Ionic spatial dispersion arises from both positive and negative charge dynamics with an impact in the (far-)infrared. Despite highly classical parameters, nonlocal quenching of up to 90% is observed for particle sizes spanning orders of magnitude. Notably, the ionic system is widely tunable via ion concentration, mass and charge, in contrast to solid metal nanoparticles. A nonlocal soft plasmonic theory for ions is relevant for biological and chemical systems bridging hard and soft matter theory and allowing the investigation of non-classical effects in electrolytes in full analogy to solid metal particles. The presented semi-classical approach allows studying plasmonic photo-catalysis introducing nonlocal aspects into electrolyte-metal interactions., Comment: 13 pages, 7 figures

We present the fabrication of TiO2 nanotube electrodes with high biocompatibility and extraordinary spectroscopic properties. Intense surface-enhanced resonance Raman signals of the heme unit of the redox enzyme Cytochromeb(5) were observed upon covalent immobilization of the protein matrix on the TiO2 surface, revealing overall preserved structural integrity and redox behavior. The enhancement factor could be rationally controlled by varying the electrode annealing temperature, reaching a record maximum value of over 70 at 475 degrees C. For the first time, such high values are reported for non-directly surface-interacting probes, for which the involvement of charge-transfer processes in signal amplification can be excluded. The origin of the surface enhancement is exclusively attributed to enhanced localized electric fields resulting from the specific optical properties of the nanotubular geometry of the electrode.

Electrolytes consist of positively and negatively charged ions even in equilibrium. Hence, plasmonic behavior can be observed in ionic systems and interaction effects between the charge carriers may play a sizable role as compared to the quantum effects observed for metal nanoparticles beyond a classical Maxwellian description. I study ionic plasmon effects, i.e., collective charge oscillations, in electrolytes in the scope of a nonlocal, two-fluid model using the hydrodynamic theory of charges. Notably, nonlocal quenching is observed for particle sizes spanning orders of magnitude, tunable via ion concentration and their mass and charge through choice of material. A plasmonic theory for ions in solution can bridge hard and soft matter theory and allow studying interaction effects from a photonic perspective in full analogy to solid metal particles. The semi-classical approach presented here can be fully integrated into standard nano-optic simulation frameworks and is considered to be of great interest for plasmonic photo-catalysis introducing nonlocal aspects into electrolyte-electrode interactions.

Nanoparticles&mdash, regularly patterned or randomly dispersed&mdash, are a key ingredient for emerging technologies in photonics. Of particular interest are scattering and field enhancement effects of metal nanoparticles for energy harvesting and converting systems. An often neglected aspect in the modeling of nanoparticles are light interaction effects at the ultimate nanoscale beyond classical electrodynamics. Those arise from microscopic electron dynamics in confined systems, the accelerated motion in the plasmon oscillation and the quantum nature of the free electron gas in metals, such as Coulomb repulsion and electron diffusion. We give a detailed account on free electron phenomena in metal nanoparticles and discuss analytic expressions stemming from microscopic (Random Phase Approximation&mdash, RPA) and semi-classical (hydrodynamic) theories. These can be incorporated into standard computational schemes to produce more reliable results on the optical properties of metal nanoparticles. We combine these solutions into a single framework and study systematically their joint impact on isolated Au, Ag, and Al nanoparticles as well as dimer structures. The spectral position of the plasmon resonance and its broadening as well as local field enhancement show an intriguing dependence on the particle size due to the relevance of additional damping channels.

Renewable energy sources are among the most important ingredients for the development of a human society with sustainable environmental footprint. Among these, photovoltaics (PV) plays a key role and is therefore a field of intense research. The key parameters of a solar cell technology includes not only the energy conversion efficiency but also the operating lifetime and the overall cost of the energy produced. The latter must also be compared with other energy sources. The optimization of all these different aspects involves research across the whole photovoltaics value chain, starting from material science up to system optimization. Development of new solar cell device concepts is as important as search for new materials with more suitable optoelectronic properties or improved approaches for PV module design and integration in power distribution systems. This requires a comprehensive view on PV technology across all scales, from the atomic to the macroscopic and industrial scale. An important aspect of PV research and of development of new devices and systems, is theoretical modeling as an indispensable tool for both basic understanding and device optimization. This involves modeling also on all scales, from the microscopic properties of materials and nanostructures up to the behavior of PV modules. During the last decade, multiscale approaches have seen increasing interest for application in numerical simulation of electronic devices. In particular, modeling and understanding of advanced photovoltaic devices are expected to benefit from multiscale modeling, which allows describing consistently both macroscopic device behavior and local microscopic processes governing light absorption, loss mechanisms, carrier transport, and extraction. In fact, many advanced PV concepts rely on effects or contain structural features that are insufficiently described by standard numerical simulation approaches or semianalytic models, both regarding electronic and optical properties. The different length scales of the electronic and optical degrees of freedoms specifically lead to an intrinsic need for multiscale simulation, which is accentuated in many advanced photovoltaics concepts including nanostructured regions. Moreover, the active layers in solar cells generally require to have a certain thickness and a large overall device area, in order to absorb a sufficient amount of light. This special issue is an attempt to collect articles on modeling of PV devices and systems on all scales. It includes two experimental articles, one shedding some light on photoreflectance measurements when probing above the pump beam energy and the other discussing morphology in hybrid lead halide perovskite solar cells. One article describes numerical modeling of Cu2O on Si tandem cells based on a semiempirical approach. A further contribution shows a physics-based model of a quantum dot solar cell, including a comparison with experimental data. The remaining two papers deal with system relevant aspects, namely, power point tracking and electrical inverters for connecting PV modules or power plants with appliances.

We investigate nonlocal electrodynamics based on the generalized hydrodynamic approach including electron diffusion in holey gold films, showing extraordinary optical transmission (EOT). Dramatic changes with respect to the local approximation for rather large film thicknesses t less than or similar to 100 nm impact both reflectance and absorbance at normal incidence. Beyond the familiar resonance blueshift with the decreasing film thickness, the interference of longitudinal pressure waves in the holey structure generates an unexpected oscillatory response with geometrical parameters. An increase in the transmittance relative to the local result of up to 33% (typically up to +/- 6% at resonance) was observed, but it can also be suppressed when absorption dominates. We expect that our findings will stimulate additional studies of EOT when taking into consideration nonlocal effects in holey films of experimentally accessible parameters in two-dimensional hole arrays. Published by AIP Publishing.

We analyze the microscopic mechanism of the improvement of solar cell efficiency by plasmons in metallic components embedded in active optical medium of a cell. We focus on the explanation of the observed new channel of plasmon photovoltaic effect related to the influence of plasmons onto the internal cell electricity beyond the previously known plasmon mediated absorption of photons. The model situation we analyze is the hybrid chemical perovskite solar cell CH 3 NH 3 PbI 3 &minus, &alpha, Cl &alpha, with inclusion of core&ndash, shell Au/Si0 2 nanoparticles filling pores in the Al 2 O 3 or TiO 2 porous bases at the bottom of perovskite layer, application of which improved the cell efficiency from 10.7 to 11.4% and from 8.4 to 9.5%, respectively, as demonstrated experimentally, mostly due to the reduction by plasmons of the exciton binding energy.

This work discusses regular particle arrays as nanostructured front layers for possible application in photovoltaic devices yielding strongly increased forward scattering. I used a rigorous plane-wave method to investigate multi-type particle layers combining different radii and configurations. The absorbance was enhanced compared to the bare Si wafer and I demonstrated on mixing particles a broadband boost in the absorbance within the homogeneous wafer region, excluding parasitic absorption in the particle layer. I studied the efficiency enhancement for varying geometries. Multi-type layers made of Si disks with two different radii achieved up to 33% (24%) and with four different radii up to 40% (30%) improvement in the short circuit current and integrated absorbance, respectively, without yet standard anti-reflection coatings. Broadband efficiency enhancement for metal multi-type layers was not observed because they show strong parasitic absorption and boost the absorbance only in narrow wavelength regions. (C) 2016 Optical Society of America

We develop a methodology to incorporate nonlocal optical response of the free electron gas due to quantum-interaction effects in metal components of periodic two-dimensional plasmonic crystals and study the impact of spatial dispersion on promising building blocks for photonic circuits. Within the framework of the hydrodynamic model, we observe significant changes with respect to the commonly employed local-response approximation, but also in comparison with homogeneous metal films where nonlocal effects have previously been considered. Notable are the emergence of a contribution from nonlocality at normal incidence and the surprisingly large structural parameters at which finite blueshifts are observable, which we attribute to diffraction that offers nonvanishing in-plane wave vector components and increases the penetration depth of longitudinal (nonlocal) modes.

A nanostructured gold-silver-hybrid electrode for SER spectroelectrochemistry was developed which advantageously combines the electrochemical properties and chemical stability of Au and the strong surface enhancement of (resonance) Raman scattering by Ag. The layered device consists of a massive nanoscopically rough Ag electrode, a thin (2 nm) organic layer, and a ca. 20 nm thick Au film that may be coated by self-assembled monolayers for protein adsorption. The SERR-spectroscopic and electrochemical performance of this device is demonstrated using the heme protein cytochrome c as a benchmark model system, thereby extending, for the first time, SE(R)R studies of molecules on Au surfaces to excitation in the violet spectral range. The enhancement factor is only slightly lower than for Ag electrodes which can be rationalized in terms of an efficient transfer of plasmon resonance excitation from the Ag to the Au coating. This mechanism, which requires a thin dielectric layer between the two metals, is supported by theoretical calculations. Fil: Feng, Jiu-Ju. Technishe Universitat Berlin; Alemania Fil: Gernert, U.. Technishe Universitat Berlin; Alemania Fil: Sezer, M.. Technishe Universitat Berlin; Alemania Fil: Kuhlmann, U.. Technishe Universitat Berlin; Alemania Fil: Murgida, Daniel Horacio. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; Argentina. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Departamento de Química Inorgánica, Analítica y Química Física; Argentina Fil: David, C.. Technishe Universitat Berlin; Alemania Fil: Richter, M.. Technishe Universitat Berlin; Alemania Fil: Knorr, A.. Technishe Universitat Berlin; Alemania Fil: Hildebrandt, P.. Technishe Universitat Berlin; Alemania Fil: Weidinger, I. M.. Technishe Universitat Berlin; Alemania

Surface plasmons in metallic nanostructures including metallically nanomodified solar cells are conventionally studied and modeled by application of the Mie approach to plasmons or by the finite element solution of differential Maxwell equations with imposed boundary and material constraints (e.g., upon commercial COMSOL software system). Both approaches are essentially classical ones and neglect quantum particularities related to plasmon excitations in metallic components. We demonstrate that these quantum plasmon effects are of crucial importance especially in theoretical simulations of plasmon-aided photovoltaic phenomena. Quantum corrections considerably improve both the Mie and COMSOL approaches in this case. We present the semiclassical random phase approximation description of plasmons in metallic nanoparticles and apply the quantumFermi golden rule scheme to assess the sunlight energy transfer to the semiconductor solar cell mediated by surface plasmons in metallic nanoparticles deposited on the top of the battery. In addition, short-ranged electron-electron interaction in metals is discussed in the framework of the semiclassical hydrodynamic model. The significance of the related quantum corrections is illustrated by the quantumly improved COMSOL simulations. (C) 2017 Optical Society of America

8 pags.; 5 figs.; OCIS codes: (350.4600) Optical engineering; (160.2900) Optical storage materials; (050.5298) Photonic crystals; (000.2190) Experimental physics; (000.6800) Theoretical physics., We experimentally and theoretically explore near-field nanopatterning obtained by irradiation of hexagonal monolayers of micron-sized polystyrene spheres on photosensitive Ge2Sb5Te5 (GST) films. The imprinted patterns are strongly sensitive to the illumination conditions, as well as the size of the spheres and the orientation of the monolayer, which we change to demonstrate control over the resulting structures. We show that the presence of multiple scattering effects cannot be neglected to describe the resulting pattern. The experimental patterns imprinted are shown to be robust to small displacements and structural defects of the monolayer. Our method enables the design and experimental verification of patterns with multiple focii per particle and complex shapes, which can be directly implemented for large scale fabrication on different substrates. © 2014 Optical Society of America., We would like to acknowledge national support from Spanish National Research Projects (Consolider NanoLight.es, MAT2010-14885, and TEC2011-22422). C.D. acknowledges a FPU fellowship from the Spanish Ministerio de Educacion.

© 2014 American Chemical Society. We use an extension of the hydrodynamic model to study nonlocal effects in the collective plasmon excitations at metal surfaces and narrow gaps between metals, including the surface spill-out of conduction band electrons. In particular, we simulate metal surfaces consisting of a smooth conduction-electron density profile and an abrupt jellium edge. We focus on aluminum and gold as prototypical examples of simple and noble metals, respectively. Our calculations agree with the dispersion relations measured from planar surfaces for these materials. Systems involving small gaps display a regime of tunnelling electrons, which is partially captured by the overlap of electron densities. This extension of the hydrodynamic model to cope with inhomogeneous density profiles provides a relatively fast and accurate way of describing the optical response of metal surfaces at subnanometer distances.

6 pags, 4 figs, 1 tab, Random Al and Ag nanoparticle distributions are studied on varying substrates, where we exploit the nanosphere self-aggregation (NSA) method for fabrication. Relying on the measured particle size distributions of these samples, we develop a theoretical model that can be applied to arbitrary random nanostructure layers as is demonstrated for several distinct NSA samples. As a proof of concept, the optical properties of the exact same particles distributions, made from the quasi-random modelling input with electron beam lithography (EBL), are investigated from both theory and experiment. Our numerical procedure is based on rigorous solutions of Maxwell's equations and yields optical spectra of fully interacting randomly positioned nanoparticle arrays. These results constitute a new methodology for improving the optical performance of layers of nanoparticles with direct application to enhanced photovoltaics. © 2012 Published by Elsevier B.V. All rights reserved., We would liketo thankfully mention financial support by the EU (FP7-248909-LIMA). C.D. further acknowledges a FPU fellowship by the Spanish Ministerio de Educación

7 pags, 4 figs, Plasmons in metals can oscillate on a sub-wavelength length scale and this large-k response constitutes an inherent prerequisite for fascinating effects such as perfect imaging and intriguing wave phenomena associated with the epsilon-near-zero (ENZ) regime. While there is no upper cut-off within the local-response approximation (LRA) of the plasma polarization, nonlocal dynamics suppress response beyond ω/v F, where v F is the Fermi velocity of the electron gas. Nonlocal response has previously been found to pose limitations to field-enhancement phenomena. Accounting for nonlocal hydrodynamic response, we show that perfect imaging is surprisingly only marginally affected by nonlocal properties of a metal slab, even for a deep subwavelength case and an extremely thin film. Similarly, for the ENZ response we find no indications of nonlocal response jeopardizing the basic behaviors anticipated from the LRA. Finally, our study of waveguiding of gap plasmons even shows a positive nonlocal influence on the propagation length. © 2013 Macmillan Publishers Limited. All rights reserved., C. D. acknowledges a FPU fellowship by the Spanish Ministerio de Educación. J. C. gratefully acknowledges financial support from the Danish Council for Independent Research and a Sapere Aude grant (12-134776). The Center for Nanostructured Graphene is sponsored by the Danish National Research Foundation, Project DNRF58.

Spatial nonlocality is known to play an important role in nano-optics when small nanometer-sized structures are involved, but few efforts have been made to assess nonlocal effects in a rigorous way. We present two different approaches to account for nonlocality in metal nanoparticles: (i) the nonretarded specular reflection model and (ii) the retarded hydrodynamical model. Excellent agreement with available experiments is obtained from our parameter-free simulations, which lead to dramatic differences with respect to local theory. Both models predict sizable plasmon blue shifts and broadenings in individual metal nanoparticles, nanoshells, particle dimers, and Yagi-Uda antennas. An analysis of plasmon resonances for varying particle size and spacing allows us to separate nonlocal and retardation effects within the hydrodynamical model. We find a wide range of geometrical parameters for which nonlocal effects coexist with significant retardation. This study is particularly relevant for broad, active areas involving applications of local field enhancement to biosensing and nonlinear optics in plasmonics. © 2011 American Chemical Society., This work has been supported by the Spanish MICINN (MAT2010-14885 and Consolider NanoLight.es) and the European Commission (FP7-ICT-2009-4-248909-LIMA and FP7-ICT-2009-4-248855-N4E).

Spatial nonlocality is known to play an important role at distances of a few nanometers, but few efforts have been made to theoretically investigate nonlocal effects in a rigorous way. We explore the effect of nonlocal response, which can be critical in the optical performance of metals at distances of 1–2 nanometers. This is particularly significant in situations for which small regions dominate the response of a larger structure. We present two different approaches to account for nonlocality in metal nanoparticles: (i) the non‐retarded specular reflection model (SRM) and (ii) the fully retarded hydrodynamical model. Comparison with available experiments results in excellent agreement with our parameter‐free modelling of nonlocal effects, which produce dramatic changes with respect to the customary local theory. We show that nonlocal effects in both models produce sizable plasmon blue shift and broadening in single metal nanoparticles as well as in dimers and shell structures. The hydrodynamical model in particular offers a way to include smooth electron distributions at surfaces and is therefore a competitor to ab initio methods.