Extremely efficient terahertz second-harmonic generation from organic crystals

Achieving efficient and intense second-harmonic generation(SHG)in the terahertz(THz)spectrum holds great potential for a wide range of technical applications,including THz nonlinear functional devices,wireless communications,and data processing and storage.However,the current research on THz harmonic emission primarily focuses on inorganic materials,which often offers challenges in achieving both efficient and broadband SHG.Herein,the remarkable efficiency of organic materials in producing THz harmonics is studied and demonstrated,thereby opening up a new avenue for searching candidates for frequency-doubling devices in the THz band.By utilizing DAST,DSTMS,and OH1 crystals,we showcase their superior frequency conversion capabilities when pumped by the narrowband THz pulses centered at 2.4,1.6,and 0.8 THz.The SHG spans a high-frequency THz domain of 4.8 THz,achieving an unprecedented conversion efficiency of∼1.21%while maintaining a perturbative nonlinear response.The highly efficient SHG of these materials is theoretically analyzed by considering the combined effects of dispersion,phonon absorption,polarization,and the nonlinear susceptibility of organic crystals.This work presents a promising platform for efficient THz frequency conversion and generation across a wide range of frequencies,offering new opportunities for novel nonlinear THz applications in next-generation electronics and optics.

Broadband and continuous wave pumped second-harmonic generation from microfiber coated with layered GaSe crystal

The conversion-efficiency for second-harmonic(SH)in optical fibers is significantly limited by extremely weak second-order nonlinearity of fused silica,and pulse pump lasers with high peak power are widely employed.Here,we propose a simple strategy to efficiently realize the broadband and continuous wave(CW)pumped SH,by transferring a crystalline GaSe coating onto a microfiber with phase-matching diameter.In the experiment,high efficiency up to 0.08%W-1mm-1 is reached for a C-band pump laser.The high enough efficiency not only guarantees SH at a single frequency pumped by a CW laser,but also multi-frequencies mixing supported by three CW light sources.Moreover,broadband SH spectrum is also achieved under the pump of a superluminescent light-emitting diode source with a 79.3 nm bandwidth.The proposed scheme provides a beneficial method to the enhancement of various nonlinear parameter processes,development of quasi-monochromatic or broadband CW light sources at new wavelength regions.

Time-domain analysis of second-harmonic generation of primary Lamb wave propagation in an elastic plate

Within the second-order perturbation approximation, this paper investigates the physical process of generation of the time-domain second harmonic by a primary Lamb wave waveform in an elastic plate. The present work is performed based on the preconditions that the phase velocity matching is satisfied and that the transfer of energy from the primary Lamb wave to the double frequency Lamb wave is not zero. It investigates the influences of the difference between the group velocities of the primary Lamb wave and the double frequency Lamb wave, the propagation distance and the duration of the primary Lamb wave waveform on the envelope shape of the time-domain second harmonic. It finds that the maximum magnitude of the envelope of the second-harmonic waveform can grow within some propagation distance even if the condition of group velocity matching is not satisfied. Our analyses also indicate that the maximum magnitude of the envelope of the second-harmonic waveform is kept constant beyond a specific propagation distance. Furthermore, it concludes that the integration amplitude of the time-domain second-harmonic waveform always grows with propagation distance within the second-order perturbation. The present research yields new physical insight not previously available into the effect of generation of the time-domain second harmonic by propagation of a primary Lamb wave waveform.

Numerical Perspective of Second-Harmonic Generation of Circumferential Guided Wave Propagation in a Circular Tube

The effect of second-harmonic generation （SHG） by primary （fundamental） circumferential guided wave （CGW） propagation is investigated from a numerical standpoint. To enable that the second harmonic of the primary CGW mode can accumulate along the circumferential direction, an appropriate mode pair of primary and double frequency CGWs is chosen. Finite element simulations and evaluations of nonlinear CGW propagation are analyzed for the selected CGW mode pair. The numerical simulations performed directly demonstrate that the response of SHG is completely generated by the desired primary CGW mode that satisfies the condition of phase velocity matching at a specific driving frequency, and that the second harmonic of the primary CGW mode does have a cumulative effect with circumferential angles. The numerical perspective obtained yields an insight into the complicated physical process of SHG of primary CGW propagation unavailable previously.

INFINITELY MANY SOLITARY WAVES DUE TO THE SECOND-HARMONIC GENERATION IN QUADRATIC MEDIA

In this paper, we consider the following coupled Schrodinger system with χ^(2) nonlinearities {-Δu1+V1(x)u1=αu1u2,x∈R^N,-Δu2+V2(x)u2=α/2u^21+βu^22,x∈R^N.which arises from second-harmonic generation in quadratic media. Here V1(x) and V2(x) are radially positive functions, 2 ≤ N < 6, α > 0 and α > β. Assume that the potential functions V1(x) and V2(x) satisfy some algebraic decay at infinity. Applying the finite dimensional reduction method, we construct an unbounded sequence of non-radial vector solutions of synchronized type.

Enhancement effect of cumulative second-harmonic generation by closed propagation feature of circumferential guided waves

On the basis of second-order perturbation approximate and modal expansion approach,we investigate the enhancement effect of cumulative second-harmonic generation(SHG)of circumferential guided waves(CGWs)in a circular tube,which is inherently induced by the closed propagation feature of CGWs.An appropriate mode pair of primary-and double-frequency CGWs satisfying the phase velocity matching and nonzero energy flux is selected to ensure that the second harmonic generated by primary CGW propagation can accumulate along the circumference.Using a coherent superposition of multi-waves,a model of unidirectional CGW propagation is established for analyzing the enhancement effect of cumulative SHG of primary CGW mode selected.The theoretical analyses and numerical simulations performed directly demonstrate that the second harmonic generated does have a cumulative effect along the circumferential direction and the closed propagation feature of CGWs does enhance the magnitude of cumulative second harmonic generated.Potential applications of the enhancement effect of cumulative SHG of CGWs are considered and discussed.The theoretical analysis and numerical simulation perspective presented here yield an insight previously unavailable into the physical mechanism of the enhancement effect of cumulative SHG by closed propagation feature of CGWs in a circular tube.

Optical second-harmonic generation of Janus MoSSe monolayer

The transition metal dichalcogenides(TMD)monolayers have shown strong second-harmonic generation(SHG)ow-ing 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.

Analysis of Second-Harmonic Generation of Low-Frequency Dilatational Lamb Waves in a Two-Layered Composite Plate

We analyze the effect of second-harmonic generation（SHG） of primary Lamb wave propagation in a two-layered composite plate, and then investigate the influence of interfacial properties on the said effect at low frequency. It is found that changes in the interfacial properties essentially affect the dispersion relation and then the maximum cumulative distance of the double-frequency Lamb wave generated. This will remarkably influence the efficiency of SHG. To overcome the complications arising from the inherent dispersion and multimode natures in analyzing the SHG effect of Lamb waves, the present work focuses on the analysis of the SHG effect of low-frequency dilatational Lamb wave propagation. Both the numerical analysis and finite element simulation indicate that the SHG effect of low-frequency dilatational Lamb wave propagation is found to be much more sensitive to changes in the interfacial properties than primary Lamb waves. The potential of using the SHG effect of low-frequency dilatational Lamb waves to characterize a minor change in the interfacial properties is analyzed.

Experimental Observation of Cumulative Second-Harmonic Generation of Circumferential Guided Wave Propagation in a Circular Tube

The experimental observation of cumulative second-harmonic generation of the primary circumferential guided wave propagation is reported. A pair of wedge transducers is used to generate the primary circumferential guided wave desired and to detect its fundamental-frequency and second-harmonic amplitudes on the outside surface of the circular tube. The amplitudes of the fundamental waves and the second harmonics of the circumferential guided wave propagation are measured for different separations between the two wedge transducers. At the driving frequency where the primary and the double-frequency circumferential guided waves have the same linear phase velocities, the clear second-harmonic signals can be observed. The quantitative relationships between the second-harmonic amplitudes and circumferential angle are analyzed. It is experimentally verified that the second harmonics of primary circumferential guided waves do have a cumulative growth effect with the circumferential angle.

Imaging the crystal orientation of 2D transition metal dichalcogenides using polarization-resolved second-harmonic generation

We use laser-scanning nonlinear imaging microscopy in atomically thin transition metal dichalcogenides(TMDs)to reveal information on the crystalline orientation distribution,within the 2D lattice.In particular,we perform polarization-resolved second-harmonic generation(PSHG)imaging in a stationary,raster-scanned chemical vapor deposition(CVD)-grown WS2 flake,in order to obtain with high precision a spatially resolved map of the orientation of its main crystallographic axis(armchair orientation).By fitting the experimental PSHG images of sub-micron resolution into a generalized nonlinear model,we are able to determine the armchair orientation for every pixel of the image of the 2D material,with further improved resolution.This pixel-wise mapping of the armchair orientation of 2D WS2 allows us to distinguish between different domains,reveal fine structure,and estimate the crystal orientation variability,which can be used as a unique crystal quality marker over large areas.The necessity and superiority of a polarization-resolved analysis over intensity-only measurements is experimentally demonstrated,while the advantages of PSHG over other techniques are analysed and discussed.

Review on second-harmonic generation of ultrasonic guided waves in solid media(Ⅰ): Theoretical analyses

Considering the high sensitivity of the nonlinear ultrasonic measurement technique and great advantages of the guided wave testing method, the use of nonlinear ultrasonic guided waves provides a promising means for evaluating and characterizing the hidden and/or inaccessible damage/degradation in solid media. Increasing attention on the development of the testing method based on nonlinear ultrasonic guided waves is largely attributed to the theoretical advances of nonlinear guided waves propagation in solid media. One of the typical acoustic nonlinear responses is the generation of second harmonics that can be used to effectively evaluate damage/degradation in materials/structures. In this paper, the theoretical progress of second-harmonic generation（SHG） of ultrasonic guided wave propagation in solid media is reviewed. The advances and developments of theoretical investigations on the effect of SHG of ultrasonic guided wave propagation in different structures are addressed. Some obscure understandings and the ideas in dispute are also discussed.

Analysis of second-harmonic generation microscopy under refractive index mismatch

On the basis of the vector diffraction theory and Green＇s function method, this paper investigates the effects of refractive index mismatch on second-harmonic generation （SHG） microscopy. The polarization distribution and SHG intensity are calculated as functions of the sample radius and probe depth. The numerical results show that refractive index mismatch can result in peak intensity degradation, increase secondary lobes and extension of second- harmonic polarization distribution. Because of the attenuation of polarization intensity, the detected SHG intensity significantly decreases with increasing probe depth, which can limit the imaging depth of SHG microscopy inside thick samples. Forward SHG intensity decays slowly than backward SHG, due to the combination of extension second-harmonic polarization distribution and strong dependency of forward SHG on sample radius.

Optical second-harmonic generation imaging for identifying gastrointestinal stromal tumors

Gastrointestinal stromal tumors(GISTs)are the most common mesenchymal tumors arising in the digest tract.It brings a challenge to diagnosis because it is asymptomatic clinically.It is well known that tumor development is often accompanied by the changes in the morphology of collagen fibers.Nowadays,an emerging optical imaging technique,second-harmonic generation(SHG),can directly identify collagen fibers without staining due to its noncentrosymmetric properties.Therefore,in this study,we attempt to assess the feasibility of SHG imaging for detecting GISTs by monitoring the morphological changes of collagen fibers in tumor microenvironment.We found that collagen alterations occurred obviously in the GISTs by comparing with normal tissues,and furthermore,two morphological features from SHG images were extracted to quantitatively assess the morphological difference of collagen fibers between normal muscular layer and GISTs by means of automated image analysis.Quantitative analyses show a significant difference in the two collagen features.This study demonstrates the potential of SHG imaging as an adjunctive diagnostic tool for label-free identification of GISTs.

Phase Effects at Second-Harmonic Generation in ZnO/PMMA Nanocomposite Films

In this paper analysis of constant-intensity approximation of nonlinear interaction of the second-harmonic generation in ZnO/PMMA nanocomposite films for different concentrations of ZnO was carried out with regard to the losses and phase changes of all the interacting waves. The investigated samples were manufactured on the basis of ZnO nanoparticles embedded into polyvinylchloride polymeric matrix （PMMA） by the method of electrochemical deposition. The main goal of work is the exploration of the ZnO morphology and parameters of the second order susceptibilities. It is verified that the surface effects in ZnO/PMMA structures will give a larger contribution than the volume effects. The factors restricting the efficiency of the process of frequency conversion have been analyzed.

Deep learning for determining pure isotropic proton spectra from solidstate spectra

Recently,an article on ^(1)H solid-state NMR spectra was published,in which the authors proposed a deep learning approach to infer the pure isotropic proton NMR spectra obtained at an infinite magic angle spinning(MAS)rate.This approach even allowed to obtain,by far,the best resolved ^(1)H spectra of molecular solids[1](https://doi.org/10.1002/anie.202216607).Deep learning based artificial intelligence is developing rapidly,and its application is deepening.Currently,there are many applications of deep learning in the field of magnetic resonance,such as the reconstruction of the under-sampled multidimensional spectra[2-4],the deconvolution of two-dimensional NMR spectra[5]and noise suppression and weak peak retrial[6],etc.

Tunable spectral continuous shift of high-order harmonic generation in atoms by a plasmon-assisted shaping pulse

We delve into the phenomenon of high-order harmonic generation within a helium atom under the influence of a plasmon-assisted shaping pulse.Our findings reveal an intriguing manipulation of the frequency peak position in the harmonic emission by adjusting the absolute phase parameter within the frequency domain of the shaping pulse.This phenomenon holds potential significance for experimental setups necessitating precisely tuned single harmonics.Notably,we observe a modulated shift in the created harmonic photon energy,spanning an impressive range of 1.2 eV.This frequency peak shift is rooted in the asymmetry exhibited by the rising and falling edges of the laser pulse,directly influencing the position of the peak frequency emission.Our study quantifies the dependence of this tuning range and the asymmetry of the laser pulse,offering valuable insights into the underlying mechanisms driving this phenomenon.Furthermore,our investigation uncovers the emergence of semi-integer order harmonics as the phase parameter is altered.We attribute this discovery to the intricate interference between harmonics generated by the primary and secondary return cores.This observation introduces an innovative approach for generating semi-integer order harmonics,thus expanding our understanding of high-order harmonic generation.Ultimately,our work contributes to the broader comprehension of complex phenomena in laser-matter interactions and provides a foundation for harnessing these effects in various applications,particularly those involving precise spectral control and the generation of unique harmonic patterns.

Wavelength calibration and spectral analysis of vacuum ultraviolet spectroscopy in EAST

A vacuum ultraviolet(VUV)spectroscopy with a focal length of 1 m has been engineered specifically for observing edge impurity emissions in Experimental Advanced Superconducting Tokamak(EAST).In this study,wavelength calibration for the VUV spectroscopy is achieved utilizing a zinc lamp.The grating angle and charge-coupled device(CCD)position are carefully calibrated for different wavelength positions.The wavelength calibration of the VUV spectroscopy is crucial for improving the accuracy of impurity spectral data,and is required to identify more impurity spectral lines for impurity transport research.Impurity spectra of EAST plasmas have also been obtained in the wavelength range of 50–300 nm with relatively high spectral resolution.It is found that the impurity emissions in the edge region are still dominated by low-Z impurities,such as carbon,oxygen,and nitrogen,albeit with the application of fulltungsten divertors on the EAST tokamak.

Core level excitation spectra of La and Mn ions in LaMnO3

Manganese-based perovskite is popular for research on ferromagnetic materials,and its spectroscopic studies are essential for understanding its electronic structure,dielectric,electrical,and magnetic properties.In this paper,the M-edge spectra of La ions and the M-edge,L-edge,and K-edge spectra of Mn ions in LaMnO3 are calculated by considering both the free-ion multiplet calculation and the crystal field effects.We analyze spectral shapes,identify peak origins,and estimate the oxidation states of La and Mn ions in LaMnO3 theoretically.It is concluded that La ions in LaMnO3 predominantly exist in the trivalent state,while Mn ions exist primarily in the trivalent state with a minor presence of tetravalent ions.Furthermore,the calculated spectra are in better conformity with the experimental spectra when the proportion of Mn3+is 90%and Mn4+is 10%.This article enhances our comprehension of the oxidation states of La and Mn within the crystal and also provides a valuable guidance for spectroscopic investigations of other manganates.

Discrimination of pressed sesame oil:A comparison study of non-targeted UV spectral fingerprints combined with different chemometric methods

This study explores the utilization of various chemometric analytical methods for determining the quality of pressed sesame oil with different adulteration levels of refined sesame oil using UV spectral fingerprints.The goal of this study was to provide a reliable tool for assessing the quality of sesame oil.The UV spectra of 51 samples of pressed sesame oil and 420 adulterated samples with refined sesame oil were measured in the range of 200-330 nm.Various classification and prediction methods,including linear discrimination analysis(LDA),support vector machines(SVM),soft independent modeling of class analogy(SIMCA),partial least squares regression(PLSR),support vector machine regression(SVR),and back-propagation neural network(BPNN),were employed to analyze the UV spectral data of pressed sesame oil and adulterated sesame oil.The results indicated that SVM outperformed the other classification methods in qualitatively identifying adulterated sesame oil,achieving an accuracy of 96.15%,a sensitivity of 97.87%,and a specificity of 80%.For quantitative analysis,BPNN yielded the best prediction results,with an R^(2) value of 0.99,RMSEP of 2.34%,and RPD value of 10.60(LOD of 8.60%and LOQ of 28.67%).Overall,the developed models exhibited significant potential for rapidly identifying and predicting the quality of sesame oil.

Cobe Spectra与Fenwal CS 3000 Plus血细胞分离器外周血造血干/祖细胞的采集效能比较

为了评价Cobe Spectra(Version 6.1)和Fenwal CS 3000 Plus两种血细胞分离机在造血干／祖细胞采集中的 采集效能,对36人64次外周血造血干／祖细胞的采集进行了回顾性分析。20人42次使用Cobe Spectra采集,16人 22次使用Fenwal CS 3000 Plus采集。对CD34+细胞采集量、采集效率以及红细胞与血小板的采集量进行比较。结 果表明:Cobe Spectra和Fenwal CS 3000 Plus在CD34+细胞采集量和采集效率上无显著差异。CD34+细胞采集量 与供者白细胞、单核细胞、造血祖细胞、CD34+细胞的动员情况呈正相关,在多因素stepwise线性回归模型中,采集 前外周血干／祖细胞浓度是唯一有意义的影响因素。Fenwal CS 3000 Plus的采集效率与外周血单核细胞量呈负相 关。Fenwal CS 3000 Plus对红细胞的收集量显著高于Cobe Spectra,并且采集后供者外周血血小板降低程度较Cobe Spectra更严重。结论:Cobe Spectra(Version 6.1)和Fenwal CS 3000 Plus在CD34+细胞的采集能力上无显著差别。 当外周血单核细胞数量高,或是血型不合移植的及血小板减少的供者,推荐使用Cobe Spectra血细胞分离机。