Polarized coherent emission outside high-symmetry points of dye-coupled plasmonic lattices.

Developing intense, coherent and ultra-fast light sources with nanoscale dimensions is a crucial issue for many applications in nanophotonics. To date, plasmonic nanolasers represent one of the most promising nanophotonic devices capable of this remarkable feature. In the present work we report on the emission properties of two-dimensional Au hexagonal nanodome arrays, fabricated by nanosphere lithography, coupled with a dye liquid solution used as the gain medium. Low-threshold stimulated emission at room temperature is demonstrated by spectral and angle-resolved photoluminescence measurements performed as a function of the pump fluence. The emission arises with narrow angular divergence in off-normal direction, out of high-symmetry points of the plasmonic lattice. The polarization properties of the stimulated emission are investigated, revealing a strong linear polarization character controlled by the polarization orientation of the pumping beam, while the first-order temporal coherence properties are measured by using a tilted-mirrors Michelson interferometer. Finally, by comparing the results obtained for the plasmonic Au nanodomes arrays with those of purely dielectric nanoarrays, the role of the plasmonic modes and the photonic lattice modes in the emission process is highlighted.

Au-Ag nanoalloy molecule-like clusters for enhanced quantum efficiency emission of Er³âº ions in silica.

The occurrence of a very efficient non-resonant energy transfer process forming ultrasmall Au-Ag nanoalloy clusters and Er(3+) ions is investigated in silica. The enhancement of the room temperature Er(3+) emission efficiency by an order of magnitude is achieved by coupling rare-earth ions to molecule-like (Au(x)Ag(1-x))N alloy nanoclusters with N = 10-15 atoms and x = 0.6 obtained by optimized sequential ion implantation on Er-implanted silica. For comparison, AuN nanoclusters obtained by the same approach and with the same size and numerical density showed an enhancement by only a factor of 2 with respect to pure Er emission, demonstrating the beneficial effect of using nanoalloyed clusters. The temperature evolution of the energy transfer process is investigated by photoluminescence and exhibits a maximum efficiency at about 600 °C, where the clusters reach the optimal size and the silica matrix completely recovers the implantation damage. The nanoalloy cluster composition and size have been studied by EXAFS analysis, which indicated a stronger Ag-O interaction with respect to the Au-O one and a preferential location of the Ag atoms at the nanoalloy cluster surface.

Energy-transfer from ultra-small Au nanoclusters to Er³âº ions: a short-range mechanism.

Sub-nanometric Au nanoclusters are known to act as very efficient sensitizers for the luminescent emission of Er(3+) ions in silica through a non-resonant broad-band energy-transfer mechanism. In the present work the energy-transfer process is investigated in detail by room temperature photoluminescence characterization of Er and Au co-implanted silica systems in which a different degree of coupling between Er(3+) ions and Au nanoclusters is obtained. The results allow us to definitely demonstrate the short-range nature of the interaction in agreement with non-radiative energy-transfer mechanisms. Moreover, an upper limit to the interaction length is also set by the Au-Au intercluster semi-distance which is smaller than 2.4 nm in the present case.

Quasi-BIC Modes in All-Dielectric Slotted Nanoantennas for Enhanced Er3+ Emission.

In the quest for new and increasingly efficient photon sources, the engineering of the photonic environment at the subwavelength scale is fundamental for controlling the properties of quantum emitters. A high refractive index particle can be exploited to enhance the optical properties of nearby emitters without decreasing their quantum efficiency, but the relatively modest Q-factors (Q ∼ 5-10) limit the local density of optical states (LDOS) amplification achievable. On the other hand, ultrahigh Q-factors (up to Q ∼ 109) have been reported for quasi-BIC modes in all-dielectric nanostructures. In the present work, we demonstrate that the combination of quasi-BIC modes with high spectral confinement and nanogaps with spacial confinement in silicon slotted nanoantennas lead to a significant boosting of the electromagnetic LDOS in the optically active region of the nanoantenna array. We observe an enhancement of up to 3 orders of magnitude in the photoluminescence intensity and 2 orders of magnitude in the decay rate of the Er3+ emission at room temperature and telecom wavelengths. Moreover, the nanoantenna directivity is increased, proving that strong beaming effects can be obtained when the emitted radiation couples to the high Q-factor modes. Finally, via tuning the nanoanntenna aspect ratio, a selective control of the Er3+ electric and magnetic radiative transitions can be obtained, keeping the quantum efficiency almost unitary.

Selective Control of Eu3+ Radiative Emission by Hyperbolic Metamaterials.

In recent years the quest for novel materials possessing peculiar abilities of manipulating light at the nanoscale has been significantly boosted due to the strict demands of advanced nanophotonics and quantum technologies. In this framework radiative decay engineering of quantum emitters is of paramount importance for developing efficient single-photon sources or nanolasers. Hyperbolic metamaterials stand out among the best cutting-edge candidates for photoluminescence control owing to their potentially unlimited photonic density of states and their ability to sustain high-k modes that allow us to strongly enhance the radiative decay rate of quantum light emitters. The aim of the present paper is to show how Au/Al2O3 hyperbolic multilayers can be used to selectively control the photoluminescence of coupled Eu3+ emitters. We point out an enhancement of the Eu3+ transitions when they are in the hyperbolic regime of the metamaterials and a significant alteration of the ED and MD branching ratios by changing the emitter-metamaterial distance.

Optimal geometry for plasmonic sensing with non-interacting Au nanodisk arrays.

Combining finite elements method electrodynamic simulations and cost-effective and scalable nanofabrication techniques, we carried out a systematic investigation and optimization of the sensing properties of non-interacting gold nanodisk arrays. Such plasmonic nanoarchitectures offer a very effective platform for fast and simple, label-free, optical bio- and chemical-sensing. We varied their main geometrical parameters (diameter and height) to monitor the plasmonic resonance position and to find the configurations that maximize the sensitivity to small layers of an analyte (local sensitivity) or to the variation of the refractive index of an embedding medium (bulk sensitivity). The spectral position of the plasmonic resonance can be tuned over a wide range from the visible to the near-IR region (500-1300 nm) and state-of-the-art performances can be obtained using the optimized nanodisks; we obtained local and bulk sensitivities of S 0 = 11.9 RIU-1 and S bulk = 662 nm RIU-1, respectively. Moreover, the results of the simulations are compared with the performances of experimentally synthesized non-interacting Au nanodisk arrays fabricated by combining sparse colloidal lithography and hollow mask lithography, with the parameters obtained by the sensitivity numerical optimization. An excellent agreement between the experimental and the simulated results is demonstrated, confirming that the optimization performed with the simulations is directly applicable to nanosensors realized with cost-effective methods, due to the quite large stability basin around the maximum sensitivities.

Rare-earth fluorescence thermometry of laser-induced plasmon heating in silver nanoparticles arrays.

The laser-induced plasmon heating of an ordered array of silver nanoparticles, under continuous illumination with an Ar laser, was probed by rare-earth fluorescence thermometry. The rise in temperature in the samples was monitored by measuring the temperature-sensitive photoluminescent emission of a europium complex (EuTTA) embedded in PMMA thin-films, deposited onto the nanoparticles array. A maximum temperature increase of 19 °C was determined upon resonant illumination with the surface plasmon resonance of the nanoarray at the highest pump Ar laser power (173 mW). The experimental results were supported by finite elements method electrodynamic simulations, which provided also information on the temporal dynamics of the heating process. This method proved to be a facile and accurate approach to probe the actual temperature increase due to photo-induced plasmon heating in plasmonic nanosystems.

Ultra-fast dynamics in the nonlinear optical response of silver nanoprism ordered arrays.

In this work we present the study of the ultra-fast dynamics of the nonlinear optical response of a honeycomb array of silver triangular nanoprisms, performed using a femtosecond pulsed laser tuned with the dipolar surface plasmon resonance of the nanoarray. Nonlinear absorption and refraction, and their time-dependence, were explored using the z-scan and time-resolved excite-probe techniques. Nonlinear absorption is shown to change sign with the input irradiance and the behavior was explained on the basis of a three-level model. The response time was determined to be in the picosecond regime. A technique based on a variable frequency chopper was also used in order to discriminate the thermal and electronic contributions to the nonlinearity, which were found to have opposite signs. All these findings propel the investigated nanoprism arrays as good candidates for applications in advanced ultra-fast nonlinear nanophotonic devices.

GaN-Based Laser Wireless Power Transfer System.

The aim of this work is to present a potential application of gallium nitride-based optoelectronic devices. By using a laser diode and a photodetector, we designed and demonstrated a free-space compact and lightweight wireless power transfer system, whose efficiency is limited by the efficiency of the receiver. We analyzed the effect of the electrical load, temperature, partial absorption and optical excitation distribution on the efficiency, by identifying heating and band-filling as the most impactful processes. By comparing the final demonstrator with a commercial RF-based Qi system, we conclude that the efficiency is still low at close range, but is promising in medium to long range applications. Efficiency may not be a limiting factor, since this concept can enable entirely new possibilities and designs, especially relevant for space applications.

Spectral dependence of nonlinear absorption in ordered silver metallic nanoprism arrays.

Ordered metallic nanoprism arrays have been proposed as novel and versatile systems for the observation of nonlinear effects such as nonlinear absorption. The study of the effect of the local field reinforcement on the fast optical third order nonlinear response around the Surface Plasmon Resonance is of great interest for many plasmonic applications. In this work, silver nanoprism arrays have been synthesized by the nanosphere lithography method. A low repetition rate tunable picosecond laser source was used to study the irradiance and wavelength dependence of the nonlinear absorption properties around the dipolar and quadrupolar resonances of the nanoarray with the use of the z-scan technique. The irradiance dependence of the on-resonance nonlinearity was studied, and a spectral region where nonlinear absorption is negligible was identified. This is important for the possible application of these materials in optical information processing devices.

Optimal geometric parameters of ordered arrays of nanoprisms for enhanced sensitivity in localized plasmon based sensors.

Plasmonic sensors based on ordered arrays of nanoprisms are optimized in terms of their geometric parameters like size, height, aspect ratio for Au, Ag or Au0.5-Ag0.5 alloy to be used in the visible or near IR spectral range. The two figures of merit used for the optimization are the bulk and the surface sensitivity: the first is important for optimizing the sensing to large volume analytes whereas the latter is more important when dealing with small bio-molecules immobilized in close proximity to the nanoparticle surface. A comparison is made between experimentally obtained nanoprisms arrays and simulated ones by using Finite Elements Methods (FEM) techniques.

Nonlinear absorption tuning by composition control in bimetallic plasmonic nanoprism arrays.

The nonlinear absorption properties of bidimensional arrays of Au-Ag bilayered nanoprisms have been investigated by z-scan measurements as a function of the bimetallic nanoprism composition. A tunable ps laser system was used to excite the ultrafast, electronic nonlinear response matching the laser wavelength with the quadrupolar surface plasmon resonances, in the visible range, of each nanoprism array. Due to the strong electromagnetic field confinement effects at the nanoprism tips, demonstrated by finite element method simulations, these nanosystems proved to have enhanced nonlinear optical properties. Moreover, a tunable changeover from reverse saturable absorption (RSA) to saturable absorption (SA) can be obtained by properly controlling the bimetallic composition of the nanoprisms, without modifying the overall morphology of the nanosystems. This capability makes these nanosystems extremely interesting for the realization of solid-state nanophotonic devices with enhanced ultrafast nonlinear optical properties.

Core-shell-like Au sub-nanometer clusters in Er-implanted silica.

The very early steps of Au metal cluster formation in Er-doped silica have been investigated by high-energy resolution fluorescence-detected X-ray absorption spectroscopy (HERFD-XAS). A combined analysis of the near-edge and extended part of the experimental spectra shows that Au cluster nucleation starts from a few Au and O atoms covalently interconnected, likely in the presence of embryonic Au-Au correlation. The first Au clusters, characterized by a well defined Au-Au coordination distance, form upon 400 °C inert annealing. The estimated upper limit of the Gibbs free energy for the associated heterogeneous nucleation is 0.06 eV per atom, suggesting that the Au nucleation is assisted by matrix defects, most likely non-bridging oxygen atoms. The experimental results indicate that the formed subnanometer Au clusters can be applied as effective core-shell systems in which the Au atoms of the 'core' develop a metallic character, whereas the Au atoms in the 'shell' can retain a partially covalent bond with O atoms of the silica matrix. High structural disorder at the Au site is found upon neutral annealing at a moderate temperature (600 °C), likely driven by the configurational disorder of the defective silica matrix. A suitable choice of the Au concentration and annealing temperature allows tailoring of the Au cluster size in the sub-nanometer range. The interaction of the Au cluster surface with the surrounding silica matrix is likely responsible for the infrared luminescence previously reported on the same systems.

Near-infrared room temperature luminescence of few-atom Au aggregates in silica: a path for the energy-transfer to Er³âº ions.

Ultra-small molecule-like AuN nanoclusters made by a number of atoms N less than 30 were produced by ion implantation in silica substrates. Their room temperature photoluminescence properties in the visible and near-infrared range have been investigated and correlated with the Er sensitization effects observed in Er-Au co-implanted samples. The intense photoluminescence emission under 488 nm laser excitation occurs in three different spectral regions around 750 nm (band A), 980 nm (band B) and 1150 nm (band C) as a consequence of the formation of discrete energy levels in the electronic structure of the molecule-like AuN nanoclusters. Indeed, energy maxima of bands A and C scale with N(-1/3) as expected for quantum confined systems. Conversely, the energy maximum of band B appears to be almost independent of size, suggesting a contribution of electronic surface states. A clear correlation between the formation of band B in the samples and Er-related photoemission is demonstrated: the band at 980 nm related to AuN nanoclusters resonant with the corresponding Er(3+) absorption level, is suggested as an effective de-excitation channel through which the Au-related photon energy may be transferred from Au nanoclusters to Er ions (either directly or mediated by photon absorption), eventually producing the Er-related infrared emission at 1540 nm.