The resonance effects on the optical second harmonic generation from 140 nm silver nanoparticles is studied experimentally by hyper-Rayleigh scattering and numerically by finite element method calculations. We find that the interferences between the broad dipolar and narrow octupolar surface plasmon resonances leads to nonlinear Fano profiles that can be externally controlled by the incident polarization angle. These profiles are responsible for the nonlinear plasmon-induced transparency in the second harmonic generation.
We present a method, based on noncollinear second harmonic generation, to evaluate the non-zero elements of the nonlinear optical susceptibility. At a fixed incidence angle, the generated signal is investigated by varying the polarization state of both fundamental beams. The resulting polarization charts allows to verify if Kleinman symmetry rules can be applied to a given material or to retrieve the absolute value of the nonlinear optical tensor terms, from a reference measurement. Experimental measurements obtained from Gallium Nitride layers are reported. The proposed method does not require an angular scan thus is useful when the generated signal is strongly affected by sample rotation
In this article, we develop a classical electrodynamic theory to study the optical nonlinearities of metallic nanoparticles. The quasi-free electrons inside the metal are approximated as a classical Coulomb-interacting electron gas, and their motion under the excitation of an external electromagnetic field is described by the plasma equations. This theory is further tailored to study second-harmonic generation. Through detailed experiment-theory comparisons, we validate this classical theory as well as the associated numerical algorithm. It is demonstrated that our theory not only provides qualitative agreement with experiments, it also reproduces the overall strength of the experimentally observed second-harmonic signals.
Angle-resolved second harmonic generation (SHG) spectra of ZnO microwires show characteristic Fano resonances in the spectral vicinity of exciton-polariton modes. The output SHG spectra after SHG interacting with exciton polariton shows a resonant enhancement peak accompanied by a suppression dip originating from the constructive and destructive interference respectively. It is demonstrated that the Fano line shape, and thus the Fano asymmetry parameter q, can be tuned by the phase-shift of the two channels. The phase-dependent q was calculated and the model describes our experimental results well. In particular, the phase-to-q relation unveil the crucial information about the dynamics of the system, e.g., defining the line shape of output SHG spectra in a superposition of quantum states.
We demonstrate supermode-based second harmonic generation in an integrated nonlinear interferometer made of linear and nonlinear directional couplers. We use a fully-fibered pump shaper to demonstrate second harmonic generation pumped by the symmetric or anti- symmetric fundamental spatial modes. The selection of the pumping mode and thus of a specific SHG spectral profile is achieved through the selection of the fundamental wavelength and via a robust phase setting scheme. We use two methods: either post-selecting or actively setting the pumping mode. Such a modal phase matching paves the way for classical and quantum applications of coupled nonlinear photonic circuits, where multimode excitation, encoding and detection are a route for multiplexing and scaling up light-processing.
We report the observation of optical second harmonic generation (SHG) in single-layer indium selenide (InSe). We measure a second harmonic signal of $>10^3$ $textrm{cts/s}$ under nonresonant excitation using a home-built confocal microscope and a standard pulsed pico-second laser. We demonstrate that polarization-resolved SHG serves as a fast, non-invasive tool to determine the crystal axes in single-layer InSe and to relate the sharp edges of the flake to the armchair and zigzag edges of the crystal structure. Our experiment determines these angles to an accuracy better than $pm$ $0.2^{circ}$. Treating the two-dimensional material as a nonlinear polarizable sheet, we determine a second-order nonlinear sheet polarizability $| chi_{textrm{sheet}}^{(2)}|=(17.9 pm 11.0)times 10^{-20}$ $textrm{m}^2 textrm{V}^{-1}$ for single-layer InSe, corresponding to an effective nonlinear susceptibility value of $| chi_textrm{eff}^{(2)}| approx (223 pm 138) times 10^{-12}$ $textrm{m} textrm{V}^{-1}$ accounting for the sheet thickness ($textrm{d} approx 0.8$ $textrm{nm}$). We demonstrate that the SHG technique can also be applied to encapsulated samples to probe their crystal orientations. The method is therefore suitable for creating high quality van der Waals heterostructures with control over the crystal directions.