Normal Incidence Excitation of Out-of-Plane Lattice Resonances in Bipartite Arrays of Metallic Nanostructures.

As a result of their coherent interaction, two-dimensional periodic arrays of metallic nanostructures support collective modes commonly known as lattice resonances. Among them, out-of-plane lattice resonances, for which the nanostructures are polarized in the direction perpendicular to the array, are particularly interesting since their unique configuration minimizes radiative losses. Consequently, these modes present extremely high quality factors and field enhancements that make them ideal for a wide range of applications. However, for the same reasons, their excitation is very challenging and has only been achieved at oblique incidence, which adds a layer of complexity to experiments and poses some limitations on their usage. Here, we present an approach to excite out-of-plane lattice resonances in bipartite arrays under normal incidence. Our method is based on exploiting the electric-magnetic coupling between the nanostructures, which has been traditionally neglected in the characterization of arrays made of metallic nanostructures. Using a rigorous coupled dipole model, we demonstrate that this coupling provides a general mechanism to excite out-of-plane lattice resonances under normal incidence conditions. We complete our study with a comprehensive analysis of a potential implementation of our results using an array of nanodisks with the inclusion of a substrate and a coating. This work provides an efficient approach for the excitation of out-of-plane lattice resonances at normal incidence, thus paving the way for the leverage of the extraordinary properties of these optical modes in a wide range of applications.

A Quasi-Bound States in the Continuum Dielectric Metasurface-Based Antenna-Reactor Photocatalyst.

Metasurfaces are a class of two-dimensional artificial resonators, creating new opportunities for strong light-matter interactions. One type of nonradiative optical metasurface that enables substantial light concentration is based on quasi-Bound States in the Continuum (quasi-BIC). Here we report the design and fabrication of a quasi-BIC dielectric metasurface that serves as an optical frequency antenna for photocatalysis. By depositing Ni nanoparticle reactors onto the metasurface, we create an antenna-reactor photocatalyst, where the virtually lossless metasurface funnels light to drive a chemical reaction. This quasi-BIC-Ni antenna-reactor drives H2 dissociation under resonant illumination, showing strong polarization, wavelength, and optical power dependencies. Both E-field-induced electronic and photothermal heating effects drive the reaction, supported by load-dependent reactivity studies and our theoretical model. This study unlocks new opportunities for photocatalysis that employ dielectric metasurfaces for light harvesting in an antenna-reactor format.

Single-Photon Emitting Arrays by Capillary Assembly of Colloidal Semiconductor CdSe/CdS/SiO2 Nanocrystals.

The controlled placement of colloidal semiconductor nanocrystals (NCs) onto planar surfaces is crucial for scalable fabrication of single-photon emitters on-chip, which are critical elements of optical quantum computing, communication, and encryption. The positioning of colloidal semiconductor NCs such as metal chalcogenides or perovskites is still challenging, as it requires a nonaggressive fabrication process to preserve the optical properties of the NCs. In this work, periodic arrays of 2500 nanoholes are patterned by electron beam lithography in a poly(methyl methacrylate) (PMMA) thin film on indium tin oxide/glass substrates. Colloidal core/shell CdSe/CdS NCs, functionalized with a SiO2 capping layer to increase their size and facilitate deposition into 100 nm holes, are trapped with a close to optimal Poisson distribution into the PMMA nanoholes via a capillary assembly method. The resulting arrays of NCs contain hundreds of single-photon emitters each. We believe this work paves the way to an affordable, fast, and practical method for the fabrication of nanodevices, such as single-photon-emitting light-emitting diodes based on colloidal semiconductor NCs.

Radially and Azimuthally Pure Vortex Beams from Phase-Amplitude Metasurfaces.

To exploit the full potential of the transverse spatial structure of light using the Laguerre-Gaussian basis, it is necessary to control the azimuthal and radial components of the photons. Vortex phase elements are commonly used to generate these modes of light, offering precise control over the azimuthal index but neglecting the radially dependent amplitude term, which defines their associated corresponding transverse profile. Here, we experimentally demonstrate the generation of high-purity Laguerre-Gaussian beams with a single-step on-axis transformation implemented with a dielectric phase-amplitude metasurface. By vectorially structuring the input beam and projecting it onto an orthogonal polarization basis, we can sculpt any vortex beam in phase and amplitude. We characterize the azimuthal and radial purities of the generated vortex beams, reaching a purity of 98% for a vortex beam with l =50 and p = 0. Furthermore, we comparatively show that the purity of the generated vortex beams outperforms those generated with other well-established phase-only metasurface approaches. In addition, we highlight the formation of "ghost" orbital angular momentum orders from azimuthal gratings (analogous to ghost orders in ruled gratings), which have not been widely studied to date. Our work brings higher-order vortex beams and their unlimited potential within reach of wide adoption.

Layer-by-layer assembly of CsPbX3 nanocrystals into large-scale homostructures.

Advances in surface chemistry of CsPbX3 (where X = Cl, Br or I) nanocrystals (NCs) enabled the replacement of native chain ligands in solution. However, there are few reports on ligand exchange carried out on CsPbX3 NC thin films. Solid-state ligand exchange can improve the photoluminescence quantum yield (PLQY) of the film and promote a change in solubility of the solid surface, thus enabling multiple depositions of subsequent nanocrystal layers. Fine control of nanocrystal film thickness is of importance for light-emitting diodes (LEDs), solar cells and lasers alike. The thickness of the emissive material film is crucial to assure the copious recombination of charges injected into a LED, resulting in bright electroluminescence. Similarly, solar cell performance is determined by the amount of absorbed light, and hence the light absorber content in the device. In this study, we demonstrate a layer-by-layer (LbL) assembly method that results in high quality films, whose thicknesses can be finely controlled. In the solid state, we replaced oleic acid and oleylamine ligands with didodecyldimethylammonium bromide or ammonium thiocyanate that enhance the PLQY of the film. The exchange is carried out through a spin-coating technique, using solvents with strategic polarity to avoid NC dissolution or damage. Exploiting this technique, the deposition of various layers results in considerable thickening of films as proven by atomic force microscope measurements. The ease of handling of our combined process (i.e. ligand exchange and layer-by-layer deposition) enables thickness control over CsPbX3 NC films with applicability to other perovskite nanomaterials paving the way for a large variety of layer permutations.