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Harmonic generation mechanisms are of great interest in nanoscience and nanotechnology, since they allow generating visible light by using near-infrared radiation, which is particularly suitable for its countless applications in bionanophotonics and optoelectronics. In this context, multilayer metal−dielectric nanocavities are widely used for light confinement and waveguiding at the nanoscale. They exhibit intense and localized resonances that can be conveniently tuned in the near-infrared and are therefore ideal for enhancing nonlinear effects in this spectral range. In this work, we experimentally investigate the nonlinear emission properties of multilayer metal−dielectric nanocavities. By engineering their absorption efficiency and exploiting their intrinsic interface-induced symmetry breaking, we achieve an almost 2 orders of magnitude higher second-harmonic generation efficiency compared to gold nanostructures featuring the same geometry and optical resonant behavior. In particular, while both the third-order nonlinear susceptibility and conversion efficiency are comparable with those of the Au nanoresonators, we estimate a second-order nonlinear susceptibility of the order of 1 pm/V, which is comparable with that of typical nonlinear crystals. We envision that our system, which combines the advantages of both plasmonic and dielectric materials, might enable the realization of composite and multifunctional nanosystems for the efficient manipulation of nonlinear optical processes at the nanoscale.

We propose to exploit the natural mechanical instability of thin solid films to form regular patterns of mono- crystalline atomically smooth silicon and germanium nanostructures that cannot be realized with conventional methods. The solid-state dewetting dynamics is guided by pre-patterning the sample by a combination of electron-beam lithography and reactive-ion etching, obtaining precise control over number, size, shape, and relative position of the final Si1-xGex structures. Here we describe our progress in the spectroscopic investigation of individual dewetted Si1-xGex nanoislands: in the linear regime, bright Mie-type localized resonances are detected in the visible spectral range, with a spectral position that can be tuned by modifying the size of the nanoparticles. In the non-linear regime, instead, sizable third-harmonic generation is observed at the level of single islands. We believe that these results will be pivotal to a novel approach in spectral filtering, sensing and structural color with all-dielectric photonic devices.

We demonstrate optically tunable control of second-harmonic generation in all dielectric nano-antennas: by using a control beam which is absorbed by the nano-resonator, we thermo-optically change the refractive index of the radiating element to modulate amplitude and phase of the second-harmonic signal. For a moderate temperature increase, sizeable modulation is demonstrated; the large tunability of the single meta-atom response paves the way to exciting avenues for reconfigurable homogeneous and heterogeneous metasurfaces.

The scattering and absorption of light by nano-objects is a key physical property exploited in many applications, including biosensing and photovoltaics. Yet, its quantification at the single object level is challenging, and often requires expensive and complicated techniques. We report a method based on a commercial transmission microscope to measure the optical scattering and absorption cross-sections of individual nano-objects. The method applies to micro-spectroscopy and wide-field image analysis, offering fine spectral information and high throughput sample characterization. Accurate cross-section determination requires a detailed modeling of the measurement, which we develop, accounting for the geometry of the illumination and detection, as well as for the presence of a sample substrate. We demonstrate the method on three model systems (gold spheres, gold rods, and polystyrene spheres), which include metallic and dielectric particles, spherical and elongated, placed in a homogeneous medium or on a dielectric substrate. Furthermore, by comparing the measured cross-sections with numerical simulations, we are able to determine structural parameters of the studied system, such as the particle diameter and aspect ratio. Our method therefore holds the potential to complement electron microscopy as a simpler and cost-effective tool for structural characterization of single nano-objects.

Nonlinear metasurfaces are a key-asset in nanophotonics, given their ability to scale down nonlinear optics to sub-µm thicknesses. To date, they are mainly realized using small-gap semiconductors, which hampers applications in the visible (VIS) range. High refractive-index transparent materials, such as lithium niobate (LiNbO 3 ), could be used to circumvent this limitation [1] , [2] , [3] , but efficient operation in this strategic spectral window is hindered by nanofabrication challenges. Here we show the first monolithic nonlinear metasurface based on LiNbO 3 for second-harmonic generation (SHG) in the VIS range with efficiency comparable to recent work in the near-infrared [3] . By tuning the pump polarization, we demonstrate efficient steering and polarization encoding of SHG, opening novel opportunities for nonlinear meta-optics.

High refractive index dielectric nanostructures can be exploited to enhance nonlinear optical processes via the strong light confinement by their resonant modes. The sensitive dependence of these m...

Nonlinear metasurfaces have become prominent tools for controlling and engineering light at the nanoscale. Usually, the polarization of the total generated third harmonic is studied. However, diffraction orders may present different polarizations. Here, we design an high quality factor silicon metasurface for third harmonic generation and perform back focal plane imaging of the diffraction orders, which present a rich variety of polarization states. Our results demonstrate the possibility of tailoring the polarization of the generated nonlinear diffraction orders paving the way to a higher degree of wavefront control.

We report efficient second-harmonic emission by single multilayer metal–dielectric nanocavities. Engineering the intrinsic interface-induced symmetry breaking by resonant optical absorption design, allows to achieve almost two orders of magnitude higher second-harmonic generation efficiency compared to gold nanostructures with the same geometry. We estimate a second-order nonlinear susceptibility of the order of 1 pm/V, which is comparable to widely used nonlinear crystals. We envision that our system, which combines the advantages of both plasmonic and dielectric materials, might enable the realization of composite nano-systems for an efficient multi-purpose manipulation of nonlinear optical processes at the nanoscale.

Nanoscale optical integration is nowadays a strategic technological challenge and the ability of generating and manipulating nonlinear optical processes in sub-wavelength volumes is pivotal to realize efficient sensing probes and photonic sources for the next-generation communication technologies. Yet, confining nonlinear processes below the diffraction limit remains a challenging task because phase-matching is not a viable approach at the nanoscale. The localized fields associated to the resonant modes of plasmonic and dielectric nanoantennas offer a route to enhance and control nonlinear processes in highly confined volumes. In my talk I will discuss two nonlinear platforms based on plasmonic and dielectric nanostructures. The first relies on a broken symmetry antenna design, which brings about an efficient second harmonic generation (SHG). We recently applied this concept to an extended array of non-centrosymmetric nanoantennas for sensing applications. I will also show the evidence of a cascaded second-order process in Third Harmonic Generation (THG) in these nanoantennas. Recently, dielectric nanoantennas emerged as an alternative to plasmonic nanostructures for nanophotonics applications, thanks to their sharp magnetic and electric Mie resonances along with the low ohmic losses in the visible/near-infrared region of the spectrum. I will present our most recent studies on the nonlinear properties of AlGaAs dielectric nanopillars. The strong localized modes along with the broken symmetry in the crystal structure of AlGaAs allow obtaining more than two orders of magnitude higher SHG efficiency with respect to plasmonic nanoantennas with similar spatial footprint and using the same pump power. I will also discuss a few key strategies we recently adopted to optically switch the SHG in these antennas even on the ultrafast time scale. Finally, I will show how to effectively engineer the sum frequency generation via the Mie resonances in these nanoantennas. These results draw a viable blueprint towards room-temperature all optical logic operation at the nanoscale.

In this work we propose a high-quality factor semiconductor nanoparticles array made of rectangular silicon nanobricks. Our optimized metasurface can dramatically boost third harmonic generation, with a complex polarization dependence in the different diffraction orders.

We present a wide-field imaging technique recently developed by us to measure quantitatively the optical extinction cross section σext of individual nanoparticles. The technique is simple, high speed, and enables the simultaneous acquisition of hundreds of nanoparticles in the wide-field image for statistical analysis, with a sensitivity corresponding to the detection of a single gold nanoparticle down to 2nm diameter. Notably, the method is applicable to any nanoparticle (dielectric, semiconducting, metallic), and can be easily and cost-effectively implemented on a conventional wide-field microscope. Of specific significance for accurate quantification, we show that σext depends on the numerical aperture of the microscope illumination due to the oblique incidence, even for spherical particles in an isotropic environment. This "long shadow" effect needs to be taken into account when comparing σext to theoretical values calculated under plane wave illumination at normal incidence. Owing to the accurate experimental quantification of σext, one can then use it to determine the nanoparticle size, as demonstrated here on gold nanoparticles of 30nm nominal diameter. This technique thus has the potential to become a simple and cost-effective new tool for accurate size characterization of single small nanoparticles, complementing time consuming and expensive methods such as electron microscopy.

The optimization of nonlinear optical processes at the nanoscale is a crucial step for the development of nanoscale photon sources for quantum-optical networks. The development of innovative plasmonic nanoantenna designs and hybrid nanostructures to enhance optical nonlinearities in very small volumes represents one of the most promising routes. In such systems, the upconversion of photons can be achieved with high efficiencies via third-order processes, such as third harmonic generation (THG), thanks to the resonantly-enhanced volume currents. Conversely, second-order processes, such as second harmonic generation (SHG), are often inhibited by the symmetry of metal lattices and of common nanoantenna geometries. SHG and THG processes in plasmonic nanostructures are generally treated independently, since they both represent a small perturbation in the light-matter interaction mechanisms. In this work, we demonstrate that this paradigm does not hold in general, by providing evidence of a cascaded process in THG, which is fueled by SHG and sizably contributes to the overall yield. We address this mechanism by unveiling an anomalous fingerprint in the polarization state of the nonlinear emission from non-centrosymmetric gold nanoantennas and point out that such cascaded processes may also appear for structures that exhibit only moderate SHG yields - signifying its general relevance in plasmon-enhanced nonlinear optics. The presence of this peculiar mechanism in THG from plasmonic nanoantennas at telecommunication wavelengths allows gaining further insight on the physics of plasmon-enhanced nonlinear optical processes. This could be crucial in the realization of nanoscale elements for photon conversion and manipulation operating at room-temperature., 25 pages, 4 figures

Semiconductor nanowires (NWs) formed by non-nitride III-V compounds grow preferentially with wurtzite (WZ) lattice. This is contrary to bulk and two-dimensional layers of the same compounds, where only zincblende (ZB) is observed. The absorption spectrum of WZ materials differs largely from their ZB counterparts and shows three transitions, referred to as A, B, and C in order of increasing energy, involving the minimum of the conduction band and different critical points of the valence band. In this work, we determine the temperature dependence (T = 10-310 K) of the energy of transitions A, B, and C in ensembles of WZ InP NWs by photoluminescence (PL) and PL excitation (PLE) spectroscopy. For the whole temperature and energy ranges investigated, the PL and PLE spectra are quantitatively reproduced by a theoretical model taking into account contribution from both exciton and continuum states. WZ InP is found to behave very similarly to wide band gap III-nitrides and II-VI compounds, where the energy of A, B, and C displays the same temperature dependence. This finding unveils a general feature of the thermal properties of WZ materials that holds regardless of the bond polarity and energy gap of the crystal. Furthermore, no differences are observed in the temperature dependence of the fundamental band gap energy in WZ InP NWs and ZB InP (both NWs and bulk). This result points to a negligible role played by the WZ/ZB differences in determining the deformation potentials and the extent of the electron-phonon interaction that is a direct consequence of the similar nearest neighbor arrangement in the two lattices.

Nonlinear metasurfaces constitute a key asset in meta-optics, given their ability to scale down nonlinear optics to sub-micrometer thicknesses. To date, nonlinear metasurfaces have been mainly realized using narrow band gap semiconductors, with operation limited to the near-infrared range. Nonlinear meta-optics in the visible range can be realized using transparent materials with high refractive index, such as lithium niobate (LiNbO3). Yet, efficient operation in this strategic spectral window has been so far prevented by the nanofabrication challenges associated with LiNbO3, which considerably limit the aspect ratio and minimum size of the nanostructures (i.e., meta-atoms). Here we demonstrate the first monolithic nonlinear periodic metasurface based on LiNbO3 and operating in the visible range. Realized through ion beam milling, our metasurface features a second-harmonic (SH) conversion efficiency of 2.40 × 10–8 at a pump intensity as low as 0.5 GW/cm2. By tuning the pump polarization, we demonstrate efficient steering and polarization encoding into narrow SH diffraction orders, opening novel opportunities for polarization-encoded nonlinear meta-optics.

We demonstrate monolithic lithium niobate metasurfaces for enhanced second- harmonic generation in the visible spectrum. Our approach offers a conversion efficiency above 5*10-5 with applications in novel nonlinear and quantum light sources.

We demonstrate optically tunable control of second-harmonic generation in all-dielectric nanoantennas: by using a control beam that is absorbed by the nanoresonator, we thermo-optically change the refractive index of the radiating element to modulate the amplitude of the second-harmonic signal. For a moderate temperature increase of roughly 40 K, modulation of the efficiency up to 60% is demonstrated; this large tunability of the single meta-atom response paves the way to exciting avenues for reconfigurable homogeneous and heterogeneous metasurfaces.