Nonlinear asymmetric imaging with AlGaAs metasurface.

Nowadays, dielectric metasurfaces are a promising platform in many different research fields such as sensing, lasing, all-optical modulation and nonlinear optics. Among all the different kinds of such thin structures, asymmetric geometries are recently attracting increasing interest. In particular, nonlinear light-matter interaction in metasurfaces constitutes a valid approach for achieving miniaturized control over light. Here, we demonstrate nonlinear asymmetric generation of light in a dielectric metasurface via second harmonic generation. By inverting the illumination direction of the pump, the nonlinear emitted power is modulated by more than one order of magnitude. Moreover, we demonstrate how a properly designed metasurface can generate two completely different images at the second harmonic when the direction of illumination is reversed. Our results may pave the way to important opportunities for the realization of compact nanophotonic devices for imaging applications by densely integrating numerous nonlinear resonators.

Near to short wave infrared light generation through AlGaAs-on-insulator nanoantennas.

AlGaAs-on-insulator (AlGaAs-OI) has recently emerged as a promising platform for nonlinear optics at the nanoscale. Among the most remarkable outcomes, second-harmonic generation (SHG) in the visible/near infrared spectral region has been demonstrated in AlGaAs-OI nanoantennas (NAs). In order to extend the nonlinear frequency generation towards the short wave infrared window, in this work we propose and demonstrate via numerical simulations difference frequency generation (DFG) in AlGaAs-OI NAs. The NA geometry is finely adjusted in order to obtain simultaneous optical resonances at the pump, signal and idler wavelengths, which results in an efficient DFG with conversion efficiencies up to 0.01%. Our investigation includes the study of the robustness against random variations of the NA geometry that may occur at fabrication stage. Overall, these outcomes identify what we believe to be a new potential and yet unexplored application of AlGaAs-OI NAs as compact devices for the generation and control of the radiation pattern in the near to short infrared spectral region.

Nonlinear THz Generation through Optical Rectification Enhanced by Phonon-Polaritons in Lithium Niobate Thin Films.

We investigate nonlinear THz generation from lithium niobate films and crystals of different thicknesses by optical rectification of near-infrared femtosecond pulses. A comparison between numerical studies and polarization-resolved measurements of the generated THz signal reveals a 2 orders of magnitude enhancement in the nonlinear response compared to optical frequencies. We show that this enhancement is due to optical phonon modes at 4.5 and 7.45 THz and is most pronounced for films thinner than 2 µm where optical-to-THz conversion is not limited by self-absorption. These results shed new light on the employment of thin film lithium niobate platforms for the development of new integrated broadband THz emitters and detectors. This may also open the door for further control (e.g., polarization, directivity, and spectral selectivity) of the process in nanophotonic structures, such as nanowires and metasurfaces, realized in the thin film platform. We illustrate this potential by numerically investigating optical-to-THz conversion driven by localized surface phonon-polariton resonances in sub-wavelength lithium niobate rods.

High-harmonic generation from a subwavelength dielectric resonator.

Higher-order optical harmonics entered the realm of nanostructured solids being observed recently in optical gratings and metasurfaces with a subwavelength thickness. Structuring materials at the subwavelength scale allows us toresonantly enhance the efficiency of nonlinear processes and reduce the size of high-harmonic sources. We report the observation of up to a seventh harmonic generated from a single subwavelength resonator made of AlGaAs material. This process is enabled by careful engineering of the resonator geometry for supporting an optical mode associated with a quasi-bound state in the continuum in the mid-infrared spectral range at around λ = 3.7 µm pump wavelength. The resonator volume measures ~0.1 λ3. The resonant modes are excited with an azimuthally polarized tightly focused beam. We evaluate the contributions of perturbative and nonperturbative nonlinearities to the harmonic generation process. Our work proves the possibility to miniaturize solid-state sources of high harmonics to the subwavelength volumes.

Control of second-harmonic generation in all-dielectric intersubband metasurfaces by controlling the polarity of χ(2).

All-dielectric metasurfaces have recently led to a paradigm shift in nonlinear optics as they allow for circumventing the phase matching constraints of bulk crystals and offer high nonlinear conversion efficiencies when normalized by the light-matter interaction volume. Unlike bulk crystals, in all-dielectric metasurfaces nonlinear conversion efficiencies primarily rely on the material nonlinearity, field enhancements, and the modal overlaps, therefore most efforts to date have only focused on utilizing these degrees of freedom. In this work, we demonstrate that for second-harmonic generation in all-dielectric metasurfaces, an additional degree of freedom is the control of the polarity of the nonlinear susceptibility. We demonstrate that semiconductor heterostructures that support resonant nonlinearities based on quantum-engineered intersubband transitions provide this new degree of freedom. We can flip and control the polarity of the nonlinear susceptibility of the dielectric medium along the growth direction and couple it to the Mie-type photonic modes. Here we demonstrate that engineering the χ(2) polarity in the meta-atom enables the control of the second-harmonic radiation pattern and conversion efficiency. Our results therefore open a new direction for engineering and optimizing second-harmonic generation using all-dielectric intersubband nonlinear metasurfaces.

Enhanced Five-Photon Photoluminescence in Subwavelength AlGaAs Resonators.

Multiphoton processes of absorption photoluminescence have enabled a wide range of applications including three-dimensional microfabrication, data storage, and biological imaging. While the applications of two-photon and three-photon absorption and luminescence have matured considerably, higher-order photoluminescence processes remain more challenging to study due to their lower efficiency, particularly in subwavelength systems. Here, we report the observation of five-photon luminescence from a single subwavelength nanoantenna at room temperature enabled by the Mie resonances. We excite an AlGaAs resonator at around 3.6 µm and observe photoluminescence at around 740 nm. We show that the interplay of the Mie multipolar modes at the subwavelength scale can enhance the efficiency of the five-photon luminescence by at least 4 orders of magnitude, being limited only by sensitivity of our detector. Our work paves the way toward applications of higher-order multiphoton processes at the subwavelength scales enabled by the physics of Mie resonances.

THz-photonics transceivers by all-dielectric phonon-polariton nonlinear nanoantennas.

The THz spectrum (spanning from 0.3 to 30 THz) offers the potential of a plethora of applications, ranging from the imaging through non transparent media to wireless-over-fiber communications and THz-photonics. The latter framework would greatly benefit from the development of optical-to-THz wavelength converters. Exploiting Difference Frequency Generation in a nonlinear all dielectric nanoantenna, we propose a compact solution to this problem. By means of a near-infrared pump beam (at [Formula: see text]), the information signal in the optical domain (at [Formula: see text]) is converted to the THz band (at [Formula: see text]). The approach is completely transparent with respect to the modulation format, and can be easily integrated in a metasurface platform for simultaneous frequency and spatial moulding of THz beams.

Efficient Frequency Conversion with Geometric Phase Control in Optical Metasurfaces.

Metasurfaces have appeared as a versatile platform for miniaturized functional nonlinear optics due to their design freedom in tailoring wavefronts. The key factor that limits its application in functional devices is the low conversion efficiency. Recently, dielectric metasurfaces governed by either high-quality factor modes (quasi-bound states in the continuum) or Mie modes, enabling strong light-matter interaction, have become a prolific route to achieve high nonlinear efficiency. Here, an effective way of spatial nonlinear phase control by using the Pancharatnam-Berry phase principle with a high third harmonic conversion efficiency of 10-4 W-2 is demonstrated both numerically and experimentally. It is found that the magnetic Mie resonance appears to be the main contributor to the third harmonic response, while the contribution from the quasi-bound states in the continuum is negligible. This is confirmed by a phenomenological model based on coupled anharmonic oscillators. Besides, the metasurface provides experimentally a high diffraction efficiency (80%-90%) in both polarization channels. A functional application of this approach is shown by experimentally reconstructing an encoded polarization-multiplexed vortex beam array with different topological charges at the third harmonic frequency with high fidelity. The approach has the potential viability for future on-chip nonlinear signal processing and wavefront control.

An All-Dielectric Polaritonic Metasurface with a Giant Nonlinear Optical Response.

Enhancing the efficiency of second-harmonic generation using all-dielectric metasurfaces to date has mostly focused on electromagnetic engineering of optical modes in the meta-atom. Further advances in nonlinear conversion efficiencies can be gained by engineering the material nonlinearities at the nanoscale, however this cannot be achieved using conventional materials. Semiconductor heterostructures that support resonant nonlinearities using quantum engineered intersubband transitions can provide this new degree of freedom. By simultaneously optimizing the heterostructures and meta-atoms, we experimentally realize an all-dielectric polaritonic metasurface with a maximum second-harmonic generation power conversion factor of 0.5 mW/W2 and power conversion efficiencies of 0.015% at nominal pump intensities of 11 kW/cm2. These conversion efficiencies are higher than the record values reported to date in all-dielectric nonlinear metasurfaces but with 3 orders of magnitude lower pump power. Our results therefore open a new direction for designing efficient nonlinear all-dielectric metasurfaces for new classical and quantum light sources.

Ultrafast, All Optically Reconfigurable, Nonlinear Nanoantenna.

The enhancement of nonlinear optical effects via nanoscale engineering is a hot topic of research. Optical nanoantennas increase light-matter interaction and provide, simultaneously, a high throughput of the generated harmonics in the scattered light. However, nanoscale nonlinear optics has dealt so far with static or quasi-static configurations, whereas advanced applications would strongly benefit from high-speed reconfigurable nonlinear nanophotonic devices. Here we propose and experimentally demonstrate ultrafast all-optical modulation of the second harmonic (SH) from a single nanoantenna. Our design is based on a subwavelength AlGaAs nanopillar driven by a control femtosecond light pulse in the visible range. The control pulse photoinjects free carriers in the nanostructure, which in turn induce dramatic permittivity changes at the band edge of the semiconductor. This results in an efficient modulation of the SH signal generated at 775 nm by a second femtosecond pulse at the 1.55 µm telecommunications (telecom) wavelength. Our results can lead to the development of ultrafast, all optically reconfigurable, nonlinear nanophotonic devices for a broad class of telecom and sensing applications.

Optical tuning of dielectric nanoantennas for thermo-optically reconfigurable nonlinear metasurfaces.

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.

Steering and Encoding the Polarization of the Second Harmonic in the Visible with a Monolithic LiNbO3 Metasurface.

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.

Strong Coupling in All-Dielectric Intersubband Polaritonic Metasurfaces.

Mie-resonant dielectric metasurfaces are excellent candidates for both fundamental studies related to light-matter interactions and for numerous applications ranging from holography to sensing to nonlinear optics. To date, however, most applications using Mie metasurfaces utilize only weak light-matter interaction. Here, we go beyond the weak coupling regime and demonstrate for the first time strong polaritonic coupling between Mie photonic modes and intersubband (ISB) transitions in semiconductor heterostructures. Furthermore, along with demonstrating ISB polaritons with Rabi splitting as large as 10%, we also demonstrate the ability to tailor the strength of strong coupling by engineering either the semiconductor heterostructure or the photonic mode of the resonators. Unlike previous plasmonic-based works, our new all-dielectric metasurface approach to generate ISB polaritons is free from ohmic losses and has high optical damage thresholds, thereby making it ideal for creating novel and compact mid-infrared light sources based on nonlinear optics.

Tuning the Ultrafast Response of Fano Resonances in Halide Perovskite Nanoparticles.

The full control of the fundamental photophysics of nanosystems at frequencies as high as few THz is key for tunable and ultrafast nanophotonic devices and metamaterials. Here we combine geometrical and ultrafast control of the optical properties of halide perovskite nanoparticles, which constitute a prominent platform for nanophotonics. The pulsed photoinjection of free carriers across the semiconducting gap leads to a subpicosecond modification of the far-field electromagnetic properties that is fully controlled by the geometry of the system. When the nanoparticle size is tuned so as to achieve the overlap between the narrowband excitons and the geometry-controlled Mie resonances, the ultrafast modulation of the transmittivity is completely reversed with respect to what is usually observed in nanoparticles with different sizes, in bulk systems, and in thin films. The interplay between chemical, geometrical, and ultrafast tuning offers an additional control parameter with impact on nanoantennas and ultrafast optical switches.

Switching the second harmonic generation by a dielectric metasurface via tunable liquid crystal.

Optical modulators are key ingredients in optoelectronics applications ranging from energy harvesting, sensor and imaging devices. In this framework, nonlinear photon conversion mechanisms constitute an attractive opportunity to add logic capabilities to these apparatuses. Here, we investigate the directionality of the emitted second harmonic signal generated in a dielectric metasurface consisting of AlGaAs nanocylinders embedded into a liquid crystal matrix. We numerically demonstrate that, by switching the liquid crystal orientation with a realistic voltage bias, it is possible to modulate the total power and the emission pattern of the SH signal coming from the proposed metasurface. Our results open important opportunities for tunable metadevices such as nonlinear holograms and dynamic displays.

Gain-loss engineering of bound states in the continuum for enhanced nonlinear response in dielectric nanocavities.

We reveal the potential of bound states in the continuum (BIC) to enhance the nonlinear response in specialty optical resonators in the presence of gain and loss. We demonstrate this phenomenon in a square core-shell AlGaAs nanowire having a proper engineered spatial variation of gain and loss to sustain quasi-BICs. The presence of these high-quality modes at both fundamental and second-harmonic wavelengths leads to an extremely high enhancement in second harmonic generation, thus preluding a framework to fabricate composite media with high effective nonlinearity.

Second harmonic generation in monolithic lithium niobate metasurfaces.

Second-order nonlinear metasurfaces have proven their ability to efficiently convert the frequency of incident signals over subwavelength thickness. However, the availability of second-order nonlinear materials for such metasurfaces has so far been limited to III-V semiconductors, which have low transparency in the visible and impose constraints on the excitation geometries due to the lack of diagonal second-order susceptibility components. Here we propose a new design concept for second-order nonlinear metasurfaces on a monolithic substrate, which is not limited by the availability of thin crystalline films and can be applied to any non-centrosymmetric material. We exemplify this concept in a monolithic Lithium Niobate metasurface with cylinder-shaped corrugations for enhanced field confinement. By optimizing the geometrical parameters, we show enhanced second harmonic generation from a near-infrared pump beam with conversion efficiency above 10-5 using 1 GW/cm2 pump intensity. Our approach enables new opportunities for practical designs of generic metasurfaces for nonlinear and quantum light sources.

Evidence of Cascaded Third-Harmonic Generation in Noncentrosymmetric Gold Nanoantennas.

The optimization of nonlinear optical processes on the nanoscale is a crucial step for the integration of complex functionalities into compact photonic devices and metasurfaces. In such systems, photon upconversion can be achieved with higher 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 because they typically represent small perturbations in the light-matter interaction mechanisms. In this work, we demonstrate that this paradigm does not hold for plasmon-enhanced nonlinear optics by providing evidence of a sum-frequency generation (SFG) process seeded by SHG, which sizably contributes to the overall THG yield. We address this mechanism by unveiling a characteristic fingerprint in the polarization state of the THG emission from gold noncentrosymmetric nanoantennas, which directly reflects the asymmetric distribution of second-harmonic fields within the structure and does not depend on the model one employs to describe photon upconversion. We suggest that such cascaded processes may also appear for structures that exhibit only moderate SHG yields. The presence of this peculiar mechanism in THG from plasmonic nanoantennas at telecommunication wavelengths allows us to gain further insight into 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.

Silicon Metasurfaces for Third Harmonic Geometric Phase Manipulation and Multiplexed Holography.

Nonlinear wavefront control is a crucial requirement in realizing nonlinear optical applications with metasurfaces. Numerous aspects of nonlinear frequency conversion and wavefront control have been demonstrated for plasmonic metasurfaces. However, several disadvantages limit their applicability in nonlinear nanophotonics, including high dissipative loss and low optical damage threshold. In contrast, it has been shown that metasurfaces made of high-index dielectrics can provide strong nonlinear responses. Regardless of the recent progress in nonlinear optical processes using all-dielectric nanostructures and metasurfaces, much less advancement has been made in realizing a full wavefront control directly with the generation process. Here, we demonstrate the nonlinear wavefront control for the third-harmonic generation with a silicon metasurface. We use a Pancharatnam-Berry phase approach to encode phase gradients and holographic images on nanostructured silicon metasurfaces. We experimentally demonstrate the polarization-dependent wavefront control and the reconstruction of an encoded hologram at the third-harmonic wavelength with high fidelity. Further, we show that holographic multiplexing is possible by utilizing the polarization states of the third harmonic generation. Our approach eases design and fabrication processes and paves the way to an easy to use toolbox for nonlinear optical wavefront control with all-dielectric metasurfaces.

Shaping the Nonlinear Emission Pattern of a Dielectric Nanoantenna by Integrated Holographic Gratings.

We demonstrate the shaping of the second-harmonic (SH) radiation pattern from a single AlGaAs nanodisk antenna using coplanar holographic gratings. The SH radiation emitted from the antenna toward the-otherwise forbidden-normal direction can be effectively redirected by suitably shifting the phase of the grating pattern in the azimuthal direction. The use of such gratings allows increasing the SH power collection efficiency by 2 orders of magnitude with respect to an isolated antenna and demonstrates the possibility of intensity-tailoring for an arbitrary collection angle. Such reconstruction of the nonlinear emission from nanoscale antennas represents the first step toward the application of all-dielectric nanostructures for nonlinear holography.