Optical second-harmonic generation of Janus MoSSe monolayer

The transition metal dichalcogenides (TMD) monolayers have shown strong second-harmonic generation (SHG) owing to their lack of inversion symmetry. These ultrathin layers then serve as the frequency converters that can be intergraded on a chip. Here, taking MoSSe as an example, we report the first detailed experimental study of the SHG of Janus TMD monolayer, in which the transition metal layer is sandwiched by the two distinct chalcogen layers. It is shown that the SHG effectively arises from an in-plane second-harmonic polarization under paraxial focusing and detection. Based on this, the orientation-resolved SHG spectroscopy is realized to readily determine the zigzag and armchair axes of the Janus crystal with an accuracy better than ±0.6°. Moreover, the SHG intensity is wavelength-dependent and can be greatly enhanced (～ 60 times) when the two-photon transition is resonant with the C-exciton state. Our findings uncover the SHG properties of Janus MoSSe monolayer, therefore lay the basis for its integrated frequency-doubling applications.     

Orientation of a photo-sensitive polymeric monolayer studied by second-harmonic generation

∞v to C_1v by the photo-isomerization process, with the azobenzene conformation retained as trans-isomer. Received: 5 April 1997     

Femtosecond time-resolved reflection second-harmonic generation on polycrystalline copper

Optical Second-Harmonic Generation (SHG) in reflection from a polycrystalline copper surface in air was studied using femtosecond time-resolved pump and probe measurements at =625 nm. The observed time dependence of second-harmonic yield from the probe beam demonstrates, that SHG is a very sensitive technique for measuring transient electron temperatures of metals even when these are covered by an oxide layer. For polycrystalline copper, an electron-phonon energy transfer time of 2 ps was observed, corresponding to a coupling constant of 3.75×10¹⁷ W/m³ K at average lattice temperatures of about 500 K. The analysis of experimental data indicates that the time dependence of SHG is governed by the linear dielectric function which, in turn, is affected by the electron temperature. There is no evidence for a temperature dependence of the nonlinear susceptibility ⁽²⁾.Paper presented at the 129th WE-Heraeus-Seminar on Surface Studies by Nonlinear Laser Spectroscopies, Kassel, Germany, May 30 to June 1, 1994     

Pulsed-laser annealing of GaAs surface studied by time-resolved second-harmonic generation in reflection

Experimental results are presented on the time dependence of the second-harmonic generation (SHG) of a mode-locked Q-switched Nd: YAG laser in reflection from both amorphous and crystalline GaAs surfaces during the pulsed-laser annealing under ruby laser irradiation. A dramatic increase of SHG by more than two orders of magnitude due to recrystallization of the noncentrosymmetric GaAs lattice in the process of pulsed-laser annealing is observed and the duration of surface recrystallization is measured to be not greater than 30–40 ns. The results can be fully understood in terms of the melting model of laser annealing.     

Total internal reflection second-harmonic generation: Probing the alkane water interface

Total internal reflection Second-Harmonic Generation (SHG) has been used to study a series of neat n-alkane/water interfaces. Polarization and incident angular-dependent measurements of the SH response show good agreement with theoretical predictions. Analysis of the incident and polarization angular-dependent SH response allows for determination of the nonlinear optical properties of molecules comprising the interfacial region. Based on Kleinman symmetry, the measured surface nonlinear susceptibilities suggest a high degree of interfacial order for octane and decane with less order indicated by the odd carbon n-alkanes examined, heptane and nonane. The SH response in reflection and transmission has been measured under a Total Internal Reflection (TIR) of the fundamental. The measured nonlinear susceptibilities in each case are found to be identical.     

Broadband second-harmonic generation in a double-tapered gallium arsenide slab using total internal reflection quasiphase matching

This article analytically describes broadband second-harmonic generation in a double-tapered gallium arsenide (GaAs) slab using total internal reflection quasi-phase matching technique. This double-tapered configuration ensures a combination of increasing and then decreasing bounce lengths which provides an extremely wide 3 dB bandwidth of 573.6 nm with a conversion efficiency of 1.929%, after considering reflection and absorption losses. Effect of varying the slab dimensions, viz., length and tapering angles, as well as the operating temperature on the performance parameters has also been incorporated in the analysis.     

Giant enhancement of second-harmonic generation from a nanocavity metasurface

Nonlinear plasmonic metasurfaces are compatible with complementary metal oxide semiconductor technology and highly promising for on-chip optical switching and modulations and nanoscale frequency conversions. However, the low nonlinearoptical response of metasurface devices limits their practical applications. To circumvent this constraint, we propose the design of a nanocavity plasmonic metasurface, in which the strong light localization in the nanocavity can be used to boost the efficiency of second-harmonic generation. Compared with the single-layer counterpart, experimental results show that the intensity of the second-harmonic waves in the nanocavity metasurface is enhanced by ~790 times. The proposed nanocavity plasmonic metasurfaces in this work may open new routes for developing highly efficient nonlinear metacrystals for on-chip nonlinear sources,nonlinear image encryption, information processing, and so on.     

Optically active second-harmonic generation from a uniaxial fluid medium

We have shown that optically active second-harmonic generation is allowed in a uniaxial fluid medium. A homeotropically aligned chiral smectic-A liquid crystal was used as an example. Phase matching was achievable by angle tuning. Chiral nonlinear susceptibility for the liquid crystal was deduced. The signal dropped precipitously as the sample underwent the transition from smectic-A to isotropic.     

Relativistic second-harmonic generation in a laser-produced plasma

Summary In this paper the relativistic second-harmonic generation of a high-power laser radiation in a laser-produced plasma has been studied theoretically in the presence of a self-generated magnetic field. The relativistic Vlasov equation has been employed for the nonlinear response of the electrons in the hot magnetized plasma. It is observed that the power conversion efficiency of the generated second harmonic wave is much higher for relativistic calculations than that for nonrelativistic calculations. To speed up publication, the authors of this paper have agreed to not receive the proofs for correction.     

Polarization-vortex-driven second-harmonic generation

Polarization vortices exist in the focus of a class of vector beams, the lowest order of which possess full vector symmetry about the axis of propagation of the beam. At high numerical apertures these beams are known to exhibit large, local, longitudinal fields in the focal region. At an interface these fields can be many times stronger than the largest available transverse component and are therefore candidates for a variety of different experiments in surface physics. The observation of vortex-driven surface second-harmonic generation at smooth metal and semiconductor surfaces and thin films is reported. By comparing the response to that of a purely transverse field, we show that the smooth surface responds primarily to the longitudinal field component.     

Broadening of the phase-matching bandwidth in quasi-phase-matched second-harmonic generation using GaN-based Bragg reflection waveguide

We present an analysis of a high index core symmetric Bragg reflection waveguide (BRW) design based on a GaN/AlxGa1-xN system for efficient quasi-phase-matched second-harmonic generation for broadband applications. By choosing the fundamental frequency to be a BRW mode and suitably tailoring the overall dispersion characteristics, the strong dispersion of the second-harmonic mode is partially canceled, leading to phase matching between the fundamental and second-harmonic over a broad range of wavelengths. The crucial interplay between the dispersive behavior of the fundamental and second-harmonic wave manifests as a broad acceptance bandwidth of approximately 33 nm accompanied with appreciable conversion efficiency (22.8%/W) for a 10 mm long waveguide. The impact of tailoring the dispersion characteristics on the conversion efficiency is also discussed.     

Transverse second-harmonic generation from disordered nonlinear crystals

We investigate the transverse second-harmonic generation in as grown strontium barium niobate (SBN) crystals with a random structure of anti-parallel ferroelectric domains. We consider both, single and counter-propagating pulse geometries. We investigate polarization properties of the second harmonic signal and discuss applications of this process for short pulses characterization. Presented at 9-th International Workshop on Nonlinear Optics Applications, NOA 2007, May 17–20, 2007, Świnoujście, Poland     

Enhanced second-harmonic generation from planar photonic crystals

Strongly enhanced second-harmonic generation is observed from a two-dimensional square lattice GaAs/AlGaAs photonic crystal waveguide when the fundamental beam, the second-harmonic beam, or both beams resonantly couple to a leaky eigenmode. P-polarized second-harmonic spectra are obtained for s-polarized, 150-fs pump pulses that are tuned from 5000 to 5600 cm(-1) and directed along the gamma-chi direction of the crystal for various angles of incidence. Compared with off-resonant conditions, enhancements of >1200x in the second-harmonic conversion are observed for resonant coupling of both the fundamental and the second-harmonic fields to leaky eigenmnodes. The angular and spectral positions of the peaks are in good agreement with simulations.     

Enhanced second-harmonic generation from resonant GaAs gratings

We theoretically study second harmonic generation in nonlinear, GaAs gratings. We find large enhancement of conversion efficiency when the pump field excites the guided mode resonances of the grating. Under these circumstances the spectrum near the pump wavelength displays sharp resonances characterized by dramatic enhancements of local fields and favorable conditions for second-harmonic generation, even in regimes of strong linear absorption at the harmonic wavelength. In particular, in a GaAs grating pumped at 1064?nm, we predict second-harmonic conversion efficiencies approximately 5 orders of magnitude larger than conversion rates achievable in either bulk or etalon structures of the same material.     

Enhanced second-harmonic generation from individual metallic nanoapertures

We demonstrate the ability of single-subwavelength-size nanoapertures fabricated in a gold metal thin film to enhance second-harmonic generation (SHG) as compared to a bare metal film. Nonlinear microscopy imaging with polarization resolution is used to quantify the SHG enhancement in circular and triangular nanoaperture shapes. The dependence of the measured SHG enhancement on circular aperture diameters is seen to originate from both phase retardation effects and field enhancements at the nanoaperture edge. Triangular nanoapertures exhibit superior SHG enhancement compared with circular ones, as expected from their noncentrosymmetric shape.     

Quadripartite entangled state from cascaded second-harmonic generation

A generation system of continuous-variable （CV） quadripartite entangled state based on two cascaded second- harmonic generation （SHG） cavities below the threshold is investigated. Two reflected fundamental bearias of the first cavity, the reflected second-harmonic beam and the output fourth-harmonic beam of the second cavity are proved to be entangled, and the dependence of the entanglement degree on the normalized frequency, pump parameter, fourth-harmonic loss parameter, and second-harmonic loss parameter is also analyzed. Due to the fact that the cavity parameters and the nonlinear crystals of the two SHG cavities can be freely chosen, the practicality of the proposed protocol is relatively perfect and the system can also be extended to the preparation of multicolor entangled states for a quantum network.     

Spectroscopic optical second-harmonic generation from semiconductor interfaces

Optical Second-Harmonic Generation (SHG) from semiconductor interfaces has been widely studied, but it is only recently, with the advent of commercial, tuneable, pulsed laser sources that the spectroscopic aspect of SHG has begun to be more widely exploited. Here, results from porous Si and Si(100)-Sb are reported, which illustrate the potential of spectroscopic SHG as a probe of semiconductor interfaces.Paper presented at the 129th Heraeus Seminar on Surface Studies by Nonlinear Laser Spectroscopies, Kassel, Germany, May 30 to June 1, 1994     

Nonadiabatic Kohn anomaly in a doped graphene monolayer

We compute, from first principles, the frequency of the E(2g), Gamma phonon (Raman G band) of graphene, as a function of the charge doping. Calculations are done using (i) the adiabatic Born-Oppenheimer approximation and (ii) time-dependent perturbation theory to explore dynamic effects beyond this approximation. The two approaches provide very different results. While the adiabatic phonon frequency weakly depends on the doping, the dynamic one rapidly varies because of a Kohn anomaly. The adiabatic approximation is considered valid in most materials. Here, we show that doped graphene is a spectacular example where this approximation miserably fails.