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.
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.