Backward Phase-Matched Second-Harmonic Generation from Stacked Metasurfaces.

We demonstrate phase-matched second-harmonic generation (SHG) from three-dimensional metamaterials consisting of stacked metasurfaces. To achieve phase matching, we utilize a novel mechanism based on phase engineering of the metasurfaces at the interacting wavelengths, facilitating phase-matched SHG in the unconventional backward direction. Stacking up to five metasurfaces,we obtain a phase-matched SHG signal, which scales superlinearly with the number of layers. Our results motivate further investigations to achieve higher conversion efficiencies also with more complex wave fronts.

Tailoring Second-Harmonic Emission from (111)-GaAs Nanoantennas.

Second-harmonic generation (SHG) in resonant dielectric Mie-scattering nanoparticles has been hailed as a powerful platform for nonlinear light sources. While bulk-SHG is suppressed in elemental semiconductors, for example, silicon and germanium due to their centrosymmetry, the group of zincblende III-V compound semiconductors, especially (100)-grown AlGaAs and GaAs, have recently been presented as promising alternatives. However, major obstacles to push the technology toward practical applications are the limited control over directionality of the SH emission and especially zero forward/backward radiation, resulting from the peculiar nature of the second-order nonlinear susceptibility of this otherwise highly promising group of semiconductors. Furthermore, the generated SH signal for (100)-GaAs nanoparticles depends strongly on the polarization of the pump. In this work, we provide both theoretically and experimentally a solution to these problems by presenting the first SHG nanoantennas made from (111)-GaAs embedded in a low index material. These nanoantennas show superior forward directionality compared to their (100)-counterparts. Most importantly, based on the special symmetry of the crystalline structure, it is possible to manipulate the SHG radiation pattern of the nanoantennas by changing the pump polarization without affecting the linear properties and the total nonlinear conversion efficiency, hence paving the way for efficient and flexible nonlinear beam-shaping devices.

Spatiospectral features of a soliton-assisted random laser in liquid crystals.

We report on novel features of random lasers assisted by near-infrared spatial solitons in nematic liquid crystals. Specifically, we study the role of light-induced reorientational waveguides (nematicons) on the spatial and spectral distributions of the laser modes. We show that the spatially spiky character of the laser emission propagating backwards with respect to the pump tends to disappear in the forward direction, due to the soliton confinement of the generated light. Moreover, the spectral features associated with various random laser resonances appear to merge upon guided-wave propagation along the nematicon, making the nematicon-aided random laser a bidirectional device with distinct emission properties at the two opposite outputs.

Collective Effects in Second-Harmonic Generation from Plasmonic Oligomers.

We investigate collective effects in plasmonic oligomers of different symmetries using second-harmonic generation (SHG) microscopy with cylindrical vector beams (CVBs). The oligomers consist of gold nanorods that have a longitudinal plasmon resonance close to the fundamental wavelength that is used for SHG excitation and whose long axes are arranged locally such that they follow the distribution of the transverse component of the electric field of radially or azimuthally polarized CVBs in the focal plane. We observe that SHG from such rotationally symmetric oligomers is strongly modified by the interplay between the polarization properties of the CVB and interparticle coupling. We find that the oligomers with radially oriented nanorods exhibit small coupling effects. In contrast, we find that the oligomers with azimuthally oriented nanorods exhibit large coupling effects that lead to silencing of SHG from the whole structure. Our experimental results are in very good agreement with numerical calculations based on the boundary element method. The work describes a new route for studying coupling effects in complex arrangements of nano-objects and thereby for tailoring the efficiency of nonlinear optical effects in such structures.

Less Is More: Enhancement of Second-Harmonic Generation from Metasurfaces by Reduced Nanoparticle Density.

We investigate optical second-harmonic generation (SHG) from metasurfaces where noncentrosymmetric V-shaped gold nanoparticles are ordered into regular array configurations. In contrast to expectations, a substantial enhancement of the SHG signal is observed when the number density of the particles in the array is reduced. More specifically, by halving the number density, we obtain over 5-fold enhancement in SHG intensity. This striking result is attributed to favorable interparticle interactions mediated by the lattice, where surface-lattice resonances lead to spectral narrowing of the plasmon resonances. Importantly, however, the results cannot be explained by the improved quality of the plasmon resonance alone. Instead, the lattice interactions also lead to further enhancement of the local fields at the particles. The experimental observations agree very well with results obtained from numerical simulations including lattice interactions.

Demonstration of longitudinally polarized optical needles.

Longitudinally polarized optical needles are beams that exhibit ultra-long depth of field, subwavelength transverse confinement, and polarization oriented along the longitudinal direction. Although several techniques have been proposed to generate such needles, their scarce experimental observations have been indirect and incomplete. Here, we demonstrate the creation and full three-dimensional verification of a longitudinally polarized optical needle. This needle is produced by generating a radially polarized Bessel-Gauss beam at the focus of a high numerical aperture microscope objective. Using three-dimensional spatial mapping of second-harmonic generation from a single vertically aligned GaAs nanowire, we directly verify such a longitudinally polarized optical needle's properties, which are formed at the focus. The needle exhibits a dominant polarization, which is oriented along the longitudinal direction, an ultra-long depth of field (30 λ), and high spatial homogeneity. These are in agreement with corresponding focal field calculations that use vector diffraction theory. Our findings open new opportunities for manipulation and utilization of longitudinally polarized optical needles.

Nonresonant Local Fields Enhance Second-Harmonic Generation from Metal Nanoislands with Dielectric Cover.

We study second-harmonic generation from gold nanoislands covered with amorphous titanium oxide (TiO_{2}) films. As the TiO_{2} thickness increases, the plasmon resonance of the nanoislands shifts away from the second-harmonic wavelength of 532 nm, diminishing the resonant enhancement of the process at this wavelength. Nevertheless, the second-harmonic signal is enhanced by up to a factor of 45 with increasing TiO_{2} thickness. This unexpected effect arises from the scaling of local fields at the fundamental wavelength of 1064 nm-which is at the far tail of the resonance-due to a change in the dielectric environment of the nanoislands.

On the molecular optical nonlinearity of halogen-bond-forming azobenzenes.

We study hyper-Rayleigh scattering and computed molecular hyperpolarizability in a series of azobenzene chromophores in chloroform and dimethylformamide as solvents. The chromophores form halogen or hydrogen bonds of varying strength with dimethylformamide molecules, differently from what is expected for chloroform. We show that hyperpolarizability is unaffected or sligthly lower with the azobenzene forming the strongest halogen bond. Solid supramolecular polymers with the same chromophores have previously demonstrated clearly higher second-order nonlinear responses when a halogen-bond-accepting polymer is used, the larger increase being associated with the stronger halogen bond. The present study proves that the higher optical nonlinearity in polymers lies in the better ordering of the chromophores instead of changes in molecular hyperpolarizability, highlighting the unique properties of halogen bonding in supramolecular chemistry.

All-optical guided-wave random laser in nematic liquid crystals.

Spatial solitons can affect and enhance random lasing in optically-pumped dyedoped nematic liquid crystals. Upon launching two collinear beams in the sample, the first to pump the fluorescent guest molecules and the second to induce a reorientational soliton, strikingly the second beam not only guides the emitted photons in the soliton waveguide, but also enhances the lasing efficiency and modulates its spectral width. By altering the scattering paths of the emitted photons, the soliton also contributes to the selection of the lasing modes, as further confirmed by the observed kinks in the input/output characteristics. These experimental results demonstrate that random lasing can be efficiently controlled by a light beam which does not interact with the gain molecules, opening a route towards light-controlled random lasers.

Nonlinear microscopy using cylindrical vector beams: Applications to three-dimensional imaging of nanostructures.

The three-dimensional (3D) optical fields that arise from the focusing of cylindrical vector beams (CVB) with radial and azimuthal polarizations provide new sources of contrast for optical microscopy of nano-objects. So far, these demonstrations have been restricted to two-dimensional transversal scanning, i.e., along the focal plane of interest, or use of point-like objects, i.e., single molecules and nanoparticles. Here, we demonstrate the first application of CVBs for 3D imaging of 3D nano-objects. This technique is done by acquiring 3D image scans of the second-harmonic generation signal from vertically-aligned semiconductor nanowires, whose second-order response is primarily driven by the longitudinal electric field, i.e., the field component along the nanowire axis. Our technique provides a new way to study individual nano-objects in three dimensions through the unique combination of nonlinear microscopy and CVBs.

Nonlinear imaging of nanostructures using beams with binary phase modulation.

We demonstrate nonlinear microscopy of oriented nanowires using excitation beams with binary phase modulation. A simple and intuitive optical scheme comprising a spatial light modulator gives us the possibility to control the phase across an incident Hermite-Gaussian beam of order (1,0) (HG10 mode). This technique allows us to gradually vary the spatial distribution of the longitudinal electric fields in the focal volume, as demonstrated by second-harmonic generation from vertically-aligned GaAs nanowires. These results open new opportunities for the full control of polarization in the focal volume to enhance light interaction with nanostructured materials.

Bulk second-harmonic generation from thermally evaporated indium selenide thin films.

We investigate bulk second-order nonlinear optical properties of amorphous indium selenide thin films fabricated by thermal evaporation. Such films are shown to exhibit strong and photostable second-harmonic generation (SHG). We report strong thickness dependence of the second-harmonic signals as characterized by the Maker-fringe method. The absolute value of the nonlinear susceptibility tensor of the film is addressed by analyzing the interference of SHG signals from the film and the glass substrate. The value of the joint non-diagonal component of the susceptibility is found to be 4 pm/V, which is comparable to that of widely used second-order nonlinear materials.

Third-harmonic generation imaging of three-dimensional microstructures fabricated by photopolymerization.

We demonstrate the capability of polarized third-harmonic generation (THG) for high contrast imaging of three-dimensional microstructures fabricated by photopolymerization. Using circular polarization of fundamental light, background-free optically-sectioned THG images were obtained from laser-written photopolymerized microstructures. The technique has great potential for simple and noninvasive characterization of photopolymerized devices, which typically show poor contrast in conventional light microscopy.

Photoinduced nonlinear optical response in azobenzene-functionalized molecular glass.

We show that mexylaminotriazine molecular glass functionalized with the azobenzene derivative Disperse Red 1 shows equally strong second-order nonlinear optical response as well-known polymers with the same photoactive component. Furthermore, even high chromophore loading does not adversely affect the nonlinear response. This suggests that chromophore-chromophore intermolecular interactions do not greatly limit the response of such molecular glasses, which therefore provide an excellent materials platform for nonlinear optical applications.

Recognition of multipolar second-order nonlinearities in thin-film samples.

We use two-beam second-harmonic generation to address thin films of silicon nitride (SiN). This technique is able to distinguish between the dipolar and higher-multipolar (magnetic and quadrupolar) contributions to the nonlinearity, as earlier shown for bulk samples. Our results for the SiN films exhibit strong multipolar signatures. Nevertheless, the results can be fully explained by the strong dipolar response of SiN once multiple reflections of the fundamental and second-harmonic fields within the film are properly taken into account. The results show that the recognition of multipolar nonlinearities requires extreme care for samples typically used for the characterization of new materials.

Surface lattice resonances in second-harmonic generation from metasurfaces.

We investigate the role of surface-lattice resonances (SLRs) in second-harmonic generation (SHG) from arrays of metal nanoparticles. The SLRs affect the generated signal when the sample is rotated away from normal incidence. The adjustment of the incident angle tunes the SLRs to the fundamental wavelength for SHG and improves the quality of the resonance for better resonance enhancement of SHG. Compared to normal incidence, an enhancement by a factor of 10 is observed. However, at certain incident angles, the enhancement is interrupted by diffraction anomalies, which redirect light into the substrate, increasing radiation damping and compromising the quality of the resonance.

Second-harmonic generation from metal nanoparticles: resonance enhancement versus particle geometry.

We demonstrate that optical second-harmonic generation (SHG) from arrays of noncentrosymmetric gold nanoparticles depends essentially on particle geometry. We prepare nanoparticles with different geometrical shapes (L and T) but similar wavelengths for the polarization-dependent plasmon resonances. In contrast to recent interpretations emphasizing resonances at the fundamental frequency, the T shape leads to stronger SHG when only one, instead of both, polarization component of the fundamental field is resonant. This is explained by the character of plasmon oscillations supported by the two shapes. Our numerical simulations for both linear and second-order responses display unprecedented agreement with measurements.

Second-harmonic generation imaging of semiconductor nanowires with focused vector beams.

We use second-harmonic generation (SHG) with focused vector beams to investigate individual vertically aligned GaAs nanowires. Our results provide direct evidence that SHG from oriented nanowires is mainly driven by the longitudinal field along the nanowire growth axis. Consequently, focused radial polarization provides a superior tool to characterize such nanowires compared to linear polarization, also allowing this possibility in the native growth environment. We model our experiments by describing the SHG process for zinc-blende structure and dipolar bulk nonlinearity.

Enhancement of second-harmonic generation from silicon nitride with gold gratings.

We report strong enhancement of second-harmonic generation in a hybrid nanostructure with gold gratings embedded in a silicon nitride film. Compared to a flat silicon nitride film, the enhancement factor can be as large as 102 to 103 for transverse magnetic and electric polarizations, respectively in good agreement with numerical results calculated using finite element method. For both polarizations, the enhancement arises from a resonance between the waveguide modes and grating.

Atomic layer deposited second-order nonlinear optical metamaterial for back-end integration with CMOS-compatible nanophotonic circuitry.

We report the fabrication of artificial unidimensional crystals exhibiting an effective bulk second-order nonlinearity. The crystals are created by cycling atomic layer deposition of three dielectric materials such that the resulting metamaterial is noncentrosymmetric in the direction of the deposition. Characterization of the structures by second-harmonic generation Maker-fringe measurements shows that the main component of their nonlinear susceptibility tensor is about 5 pm/V, which is comparable to well-established materials and more than an order of magnitude greater than reported for a similar crystal [Appl. Phys. Lett.107, 121903 (2015)APPLAB0003-695110.1063/1.4931492]. Our demonstration opens new possibilities for second-order nonlinear effects on CMOS-compatible nanophotonic platforms.