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Register a new userSecond harmonic generation by strongly coupled exciton-plasmons: the role of polaritonic states in nonlinear dynamics
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We investigate second harmonic generation (SHG) from hexagonal periodic arrays of triangular nano-holes of aluminum using a self-consistent methodology based on the hydrodynamics-Maxwell-Bloch approach. It is shown that angular polarization patterns of the far-field second harmonic response abide to three-fold symmetry constraints on tensors. When a molecular layer is added to the system and its parameters are adjusted to achieve the strong coupling regime between a localized plasmon mode and molecular excitons, Rabi splitting is observed from occurrence of both single- and two-photon transition peaks within the SHG power spectrum. It is argued that the splitting observed for both transitions results from direct transitions between lower and upper polaritonic states of the strongly coupled system. This interpretation can be accounted by a tailored three-level quantum model, with results in agreement with the unbiased numerical approach. Our results suggest the hybrid states formed in strongly coupled systems directly contribute to the nonlinear dynamics. This opens new directions in designing THz sources and nonlinear frequency converters.
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Light with light control of surface plasmon polaritons is theoretically demonstrated. A barely simple and compact source of these waves consists in a finite number of slits (evenly spaced) perforating a metal film. The system scatters electromagnetic fields in one side of the metal film when it is illuminated from the opposite side by a polarized light source. High intensity light sources moreover efficiently generate light at second harmonic and higher frequencies in the metal led by optical nonlinearities. It is shown how the mixing of fields scattered by the slits from a weak beam at $lambda$ wavelength, with the second harmonic fields generated by a high intensity $2 lambda$ beam, creates a destructive interference of surface plasmons in one of the two possible directions of emission from the slits, while these are enhanced along the opposite direction. The unidirectional launching of surface plasmons is due to the different properties of symmetry at $lambda$ whether they are linearly or nonlinearly generated. It is envisaged a nanodevice which might allow sending digital information codified in the surface plasmon field or be used to build ultra-narrow bandwidth surface plasmon frequency combs.
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 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
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.
Noble metals with well-defined crystallographic orientation constitute an appealing class of materials for controlling light-matter interactions on the nanoscale. Nonlinear optical processes, being particularly sensitive to anisotropy, are a natural and versatile probe of crystallinity in nano-optical devices. Here we study the nonlinear optical response of monocrystalline gold flakes, revealing a polarization dependence in second-harmonic generation from the {111} surface that is markedly absent in polycrystalline films. Apart from suggesting an approach for directional enhancement of nonlinear response in plasmonic systems, we anticipate that our findings can be used as a rapid and non-destructive method for characterization of crystal quality and orientation that may be of significant importance in future applications.
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