All-optical free-space routing of upconverted light by metasurfaces via nonlinear interferometry.

All-optical modulation yields the promise of high-speed information processing. In this field, metasurfaces are rapidly gaining traction as ultrathin multifunctional platforms for light management. Among the featured functionalities, they enable light-wavefront manipulation and more recently demonstrated the ability to perform light-by-light manipulation through nonlinear optical processes. Here, by employing a nonlinear periodic metasurface, we demonstrate the all-optical routing of telecom photons upconverted to the visible range. This is achieved via the interference between two frequency-degenerate upconversion processes, namely, third-harmonic and sum-frequency generation, stemming from the interaction of a pump pulse with its frequency-doubled replica. By tuning the relative phase and polarization between these two pump beams, we route the upconverted signal among the diffraction orders of the metasurface with a modulation efficiency of up to 90%. This can be achieved by concurrently engineering the nonlinear emission of the individual elements (meta-atoms) of the metasurface along with its pitch. Owing to the phase control and ultrafast dynamics of the underlying nonlinear processes, free-space all-optical routing could be potentially performed at rates close to the employed optical frequencies divided by the quality factor of the optical resonances at play. Our approach adds a further twist to optical interferometry, which is a key enabling technique employed in a wide range of applications, such as homodyne detection, radar interferometry, light detection and ranging technology, gravitational-wave detection and molecular photometry. In particular, the nonlinear character of light upconversion combined with phase sensitivity is extremely appealing for enhanced imaging and biosensing.

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.

Fully Integrated Silicon Photonic Erbium-Doped Nanodiode for Few Photon Emission at Telecom Wavelengths.

Recent advancements in quantum key distribution (QKD) protocols opened the chance to exploit nonlaser sources for their implementation. A possible solution might consist in erbium-doped light emitting diodes (LEDs), which are able to produce photons in the third communication window, with a wavelength around 1550 nm. Here, we present silicon LEDs based on the electroluminescence of Er:O complexes in Si. Such sources are fabricated with a fully-compatible CMOS process on a 220 nm-thick silicon-on-insulator (SOI) wafer, the common standard in silicon photonics. The implantation depth is tuned to match the center of the silicon layer. The erbium and oxygen co-doping ratio is tuned to optimize the electroluminescence signal. We fabricate a batch of Er:O diodes with surface areas ranging from 1 µm × 1 µm to 50 µm × 50 µm emitting 1550 nm photons at room temperature. We demonstrate emission rates around 5 × 106 photons/s for a 1 µm × 1 µm device at room temperature using superconducting nanowire detectors cooled at 0.8 K. The demonstration of Er:O diodes integrated in the 220 nm SOI platform paves the way towards the creation of integrated silicon photon sources suitable for arbitrary-statistic-tolerant QKD protocols.

Liquid-Phase Exfoliation of Bismuth Telluride Iodide (BiTeI): Structural and Optical Properties of Single-/Few-Layer Flakes.

Bismuth telluride halides (BiTeX) are Rashba-type crystals with several potential applications ranging from spintronics and nonlinear optics to energy. Their layered structures and low cleavage energies allow their production in a two-dimensional form, opening the path to miniaturized device concepts. The possibility to exfoliate bulk BiTeX crystals in the liquid represents a useful tool to formulate a large variety of functional inks for large-scale and cost-effective device manufacturing. Nevertheless, the exfoliation of BiTeI by means of mechanical and electrochemical exfoliation proved to be challenging. In this work, we report the first ultrasonication-assisted liquid-phase exfoliation (LPE) of BiTeI crystals. By screening solvents with different surface tension and Hildebrandt parameters, we maximize the exfoliation efficiency by minimizing the Gibbs free energy of the mixture solvent/BiTeI crystal. The most effective solvents for the BiTeI exfoliation have a surface tension close to 28 mN m-1 and a Hildebrandt parameter between 19 and 25 MPa0.5. The morphological, structural, and chemical properties of the LPE-produced single-/few-layer BiTeI flakes (average thickness of ∼3 nm) are evaluated through microscopic and optical characterizations, confirming their crystallinity. Second-harmonic generation measurements confirm the non-centrosymmetric structure of both bulk and exfoliated materials, revealing a large nonlinear optical response of BiTeI flakes due to the presence of strong quantum confinement effects and the absence of typical phase-matching requirements encountered in bulk nonlinear crystals. We estimated a second-order nonlinearity at 0.8 eV of |χ(2)| ∼ 1 nm V-1, which is 10 times larger than in bulk BiTeI crystals and is of the same order of magnitude as in other semiconducting monolayers (e.g., MoS2).

Tailoring Third-Harmonic Diffraction Efficiency by Hybrid Modes in High-Q Metasurfaces.

Metasurfaces are versatile tools for manipulating light; however, they have received little attention as devices for the efficient control of nonlinearly diffracted light. Here, we demonstrate nonlinear wavefront control through third-harmonic generation (THG) beaming into diffraction orders with efficiency tuned by excitation of hybrid Mie-quasi-bound states in the continuum (BIC) modes in a silicon metasurface. Simultaneous excitation of the high-Q collective Mie-type modes and quasi-BIC modes leads to their hybridization and results in a local electric field redistribution. We probe the hybrid mode by measuring far-field patterns of THG and observe the strong switching between (0,-1) and (-1,0) THG diffraction orders from 1:6 for off-resonant excitation to 129:1 for the hybrid mode excitation, showing tremendous contrast in controlling the nonlinear diffraction patterns. Our results pave the way to the realization of metasurfaces for novel light sources, telecommunications, and quantum photonics.

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.

Third-harmonic light polarization control in magnetically resonant silicon metasurfaces.

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.

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.

Phonon-Mediated Interlayer Charge Separation and Recombination in a MoSe2/WSe2 Heterostructure.

Monolayer transition metal dichalcogenides bear great potential for photodetection and light harvesting due to high absorption coefficients. However, these applications require dissociation of strongly bound photogenerated excitons. The dissociation can be achieved by vertically stacking different monolayers to realize band alignment that favors interlayer charge transfer. In such heterostructures, the reported recombination times vary strongly, and the charge separation and recombination mechanisms remain elusive. We use two color pump-probe microscopy to demonstrate that the charge separation in a MoSe2/WSe2 heterostructure is ultrafast (∼200 fs) and virtually temperature independent, whereas the recombination accelerates strongly with temperature. Ab initio quantum dynamics simulations rationalize the experiments, indicating that the charge separation is temperature-independent because it is barrierless, involves dense acceptor states, and is promoted by higher-frequency out-of-plane vibrations. The strong temperature dependence of the recombination, on the other hand, arises from a transient indirect-to-direct bandgap modulation by low-frequency shear and layer breathing motions.

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.

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.

Room Temperature Resonant Photocurrent in an Erbium Low-Doped Silicon Transistor at Telecom Wavelength.

An erbium-doped silicon transistor prepared by ion implantation and co-doped with oxygen is investigated by photocurrent generation in the telecommunication range. The photocurrent is explored at room temperature as a function of the wavelength by using a supercontinuum laser source working in the µW range. The 1-µm² transistor is tuned to involve in the transport only those electrons lying in the Er-O states. The spectrally resolved photocurrent is characterized by the typical absorption line of erbium and the linear dependence of the signal over the impinging power demonstrates that the Er-doped transistor is operating far from saturation. The relatively small number of estimated photoexcited atoms (≈ 4 × 10 4 ) makes Er-dpoed silicon potentially suitable for designing resonance-based frequency selective single photon detectors at 1550 nm.

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.

Metal-dielectric hybrid nanoantennas for efficient frequency conversion at the anapole mode.

Background: Dielectric nanoantennas have recently emerged as an alternative solution to plasmonics for nonlinear light manipulation at the nanoscale, thanks to the magnetic and electric resonances, the strong nonlinearities, and the low ohmic losses characterizing high refractive-index materials in the visible/near-infrared (NIR) region of the spectrum. In this frame, AlGaAs nanoantennas demonstrated to be extremely efficient sources of second harmonic radiation. In particular, the nonlinear polarization of an optical system pumped at the anapole mode can be potentially boosted, due to both the strong dip in the scattering spectrum and the near-field enhancement, which are characteristic of this mode. Plasmonic nanostructures, on the other hand, remain the most promising solution to achieve strong local field confinement, especially in the NIR, where metals such as gold display relatively low losses. Results: We present a nonlinear hybrid antenna based on an AlGaAs nanopillar surrounded by a gold ring, which merges in a single platform the strong field confinement typically produced by plasmonic antennas with the high nonlinearity and low loss characteristics of dielectric nanoantennas. This platform allows enhancing the coupling of light to the nanopillar at coincidence with the anapole mode, hence boosting both second- and third-harmonic generation conversion efficiencies. More than one order of magnitude enhancement factors are measured for both processes with respect to the isolated structure. Conclusion: The present results reveal the possibility to achieve tuneable metamixers and higher resolution in nonlinear sensing and spectroscopy, by means of improved both pump coupling and emission efficiency due to the excitation of the anapole mode enhanced by the plasmonic nanoantenna.

Surface-enhanced chiroptical spectroscopy with superchiral surface waves.

We study the chiroptical properties of one-dimensional photonic crystals supporting superchiral surface waves by introducing a simple formalism based on the Fresnel reflection matrix. We show that the proposed framework provides useful insights on the behavior of all the relevant chiroptical quantities, allowing for a deeper understanding of surface-enhanced chiral sensing platforms based on one-dimensional photonic crystals. Finally, we analyze and discuss the limitations of such platforms as the surface concentration of the target chiral analytes is gradually increased.

Broadband, electrically tunable third-harmonic generation in graphene.

Optical harmonic generation occurs when high intensity light (>1010 W m-2) interacts with a nonlinear material. Electrical control of the nonlinear optical response enables applications such as gate-tunable switches and frequency converters. Graphene displays exceptionally strong light-matter interaction and electrically and broadband tunable third-order nonlinear susceptibility. Here, we show that the third-harmonic generation efficiency in graphene can be increased by almost two orders of magnitude by controlling the Fermi energy and the incident photon energy. This enhancement is due to logarithmic resonances in the imaginary part of the nonlinear conductivity arising from resonant multiphoton transitions. Thanks to the linear dispersion of the massless Dirac fermions, gate controllable third-harmonic enhancement can be achieved over an ultrabroad bandwidth, paving the way for electrically tunable broadband frequency converters for applications in optical communications and signal processing.

1.54 µm photoluminescence from Er:Ox centers at extremely low concentration in silicon at 300 K.

The demand for single photon emitters at λ=1.54 µm, which follows from the consistent development of quantum networks based on optical fiber technologies, makes Er:Ox centers in Si a viable resource, thanks to the I13/24→I415/2 optical transition of Er3+. While its implementation in high-power applications is hindered by the extremely low emission rate, the study of such systems in the low concentration regime remains relevant for quantum technologies. In this Letter, we explore the room-temperature photoluminescence at the telecomm wavelength from very low implantation doses of Er:Ox in Si. The lower-bound number of optically active Er atoms detected is of the order of 102, corresponding to a higher-bound value for the emission rate per individual ion of about 104 s-1.

Information storage and retrieval in a single levitating colloidal particle.

The binary switch is a basic component of digital information. From phase-change alloys to nanomechanical beams, molecules and atoms, new strategies for controlled bistability hold great interest for emerging technologies. We present a generic methodology for precise and parallel spatiotemporal control of nanometre-scale matter in a fluid, and demonstrate the ability to attain digital functionalities such as switching, gating and data storage in a single colloid, with further implications for signal amplification and logic operations. This fluid-phase bit can be arrayed at high densities, manipulated by either electrical or optical fields, supports low-energy, high-speed operation and marks a first step toward 'colloidal information'. The principle generalizes to any system where spatial perturbation of a particle elicits a differential response amenable to readout.

Mode matching in multiresonant plasmonic nanoantennas for enhanced second harmonic generation.

Boosting nonlinear frequency conversion in extremely confined volumes remains a challenge in nano-optics research, but can enable applications in nanomedicine, photocatalysis and background-free biosensing. To obtain brighter nonlinear nanoscale sources, approaches that enhance the electromagnetic field intensity and counter the lack of phase matching in nanoplasmonic systems are often employed. However, the high degree of symmetry in the crystalline structure of plasmonic materials (metals in particular) and in nanoantenna designs strongly quenches second harmonic generation. Here, we describe doubly-resonant single-crystalline gold nanostructures with no axial symmetry displaying spatial mode overlap at both the excitation and second harmonic wavelengths. The combination of these features allows the attainment of a nonlinear coefficient for second harmonic generation of ∼5 × 10(-10) W(-1), enabling a second harmonic photon yield higher than 3 × 10(6) photons per second. Theoretical estimations point toward the use of our nonlinear plasmonic nanoantennas as efficient platforms for label-free molecular sensing.