Non-Invasive Second Harmonic Generation (SHG) in Macroscopy (MacroSHG) as Bio-Diagnosis to Image Collagen Network Organization in Extracellular Matrix

In this work, we have considered a new multimodality imaging for macroscopy based on Second Harmonic Generation (SHG) method to monitor invasivelessly the matrix collagen. As the triple helicoidally structure of collagen molecules appearing as not centrosymetric, very organized and spatially oriented, collagen fibrils give rise to a very strong SHG signal and can be imaged without any exogenous dye. To integrate a multidimensional scale with a large field of view (non-sliced samples), we have adapted and validated an instrumental coupling between a two photon excitation laser and a macroscope to collect cartography of SHG signal. We introduced an index (F-SHG) based on decay time response measured by TCSPC for respectively Fluorescence (F) and Second Harmonic Generation (SHG) values. For various sample where protein collagen is the major component of extracellular matrix (vessel, skin, carotide vessel, rat femoral head cartilage, mouse tumor, human wharton’s jelly and rat tendon) or not (nacre), we compared the index distribution obtained with MacroSHG. In this work, we showed for the first time that multiscale large field imaging (Macroscopy) combined to Multimodality approaches (SHG-TCSPC) could be an innovative and non-invasive technique to detect and identify some biological interest molecules (collagen) in biomedical topics.

Irradiation Effect on Second Harmonic Generation of Dyes Doped KDP Crystals

Most irradiation studies in the hydrogen bonded ferroelectrics have been concentrated on the transient defects induced by ionising radiation, such as ultraviolet （UV） light, where the defects are closely related to the optical properties. But heavy ion beam irradiation effects have rarely been studied. The structural, optical, and non-linear optical properties of the doped crystals were analyzed with the characterization studies, such as powder XRD, UV-Visible and second harmonic generation （SHG） measurements, respectively. The results for doped KDP crystal were compared with the results of the pure KDP crystals. The experiment results showed that Li^3＋ irradiation leads to the development of a well-defined surface H peak in dye doped KDP crystals. The stability of KDP single crystal was improved by doping organic dyes. The nano-islands of dye in KDP were likely to be dissolved and enhance the non-linear optical properties of these materials.

Second Harmonic Generation of Lamb Wave in Numerical Perspective

The influences of phase and group velocity matching on cumulative second harmonic generation of Lamb waves are investigated in numerical perspective. Finite element simulations of nonlinear Lamb wave propagation are performed for Lamb wave mode pairs with exact and approximate phase velocity matching, with and without group velocity matching, respectively. The evolution of time-domain second harmonic Lamb waves is analyzed with the propagation distance. The amplitudes of primary and second harmonic waves are calculated to characterize the acoustic nonlinearity. The results verify that phase velocity matching is necessary for generation of the cumulative second harmonic Lamb wave in numerical perspective, while group velocity matching is demonstrated to not be a necessary condition.

Photoinduced Second Harmonic Generation of Bi_2S_3 Microcrystallite Doped Silica Glass

Silica glasses doped with Bi2S3 microcystallite was prepared by the sol-gel process. Photoinduced second harmonic generation (SHG) was observed in the glass when it was irradiated with intense 1.06 mum and frequency doubled laser beams from a mode-locked Nd: YAG laser. It was found that the signal intensity increased with the irradiating time and approached a saturation gradually. The effect may be explained reasonably by the DC field model.

Dual bound states in the continuum enhanced second harmonic generation with transition metal dichalcogenides monolayer

The emergence of two dimensional(2D)materials has opened new possibilities for exhibiting second harmonic genera-tion(SHG)at the nanoscale,due to their remarkable optical response related to stable excitons at room temperature.However,the ultimate atomic-scale interaction length with light makes the SHG of Transition Metal Dichalcogenides(TM-Ds)monolayers naturally weak.Here,we propose coupling a monolayer of TMDs with a photonic grating slab that works with doubly resonant bound states in the continuum(BIC).The BIC slabs are designed to exhibit a pair of BICs,reson-ant with both the fundamental wave(FW)and the second harmonic wave(SHW).Firstly,the spatial mode matching can be fulfilled by tilting FW's incident angle.We theoretically demonstrate that this strategy leads to more than four orders of magnitude enhancement of SHG efficiency than a sole monolayer of TMDs,under a pump light intensity of 0.1 GW/cm^(2).Moreover,we demonstrate that patterning the TMDs monolayer can further enhance the spatial overlap coefficient,which leads to an extra three orders of magnitude enhancement of SHG efficiency.These results demonstrate remarkable pos-sibilities for enhancing SHG with nonlinear 2D materials,opening many opportunities for chip-based light sources,nano-lasers,imaging,and biochemical sensing.

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.

Second Harmonic Generation in Some Donor-Acceptor Substituted Chalcone Derivatives

A series of five chalcone derivatives with different substituents in para and meta posions have been synthesized, and single crystals were successfully grown in aceton solution by slow evaporation solution growth technique (SESGT). Single crystal X-ray studies revealed that all the crystals crystallized in noncentrosymmetric space group with their molecular dipoles perfectly aligned in a direction-favorable for large nonlinear optical effects. Kurtz powder tests revealed that all five materials have second-harmonic-generating properties with maximum efficiencies of approximately 14 times that of urea standard. UV-vis-NIR spectroscopy and thermogravimetric analyses are also presented for all of the reported materials. Among the five chalcones, high quality single crystals of 4-Methoxy-4'-chlorochalcone were grown by SESGT, and its crystalline perection were studied by using a high resolution X-ray diffractometry (HRXRD).

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.

Tunable Second Harmonic Generation with High Conversion Efficiency in Periodically Poled Lithium Niobate Channel Waveguide

The experiment on quasi-phase-matched second harmonic generation (SHG) in a channel waveguide was reported. The waveguide was made by annealed proton exchange in the periodically poled lithium niobate (PPLN) with the period of PPLN of 14.9 μm, which was designed for cascading wavelength conversion in dense wavelength division multiplexer optical communications. The measurement results of SHG conversion efficiency as a function of fundamental wavelength at room temperature fit well to sinc^2 shape. The peak of SHG conversion efficiency was 75%·W~ -1 ·cm~ -2 as well as reported. The relationship between the center fundamental wavelength and temperature shows that SHG can be effectively tuned by the temperature in PPLN waveguide.

Modulation of the second-harmonic generation in MoS_(2) by graphene covering

Nonlinear optical frequency mixing,which describes new frequencies generation by exciting nonlinear materials with intense light field,has drawn vast interests in the field of photonic devices,material characterization,and optical imaging.Investigating and manipulating the nonlinear optical response of target materials lead us to reveal hidden physics and develop applications in optical devices.Here,we report the realization of facile manipulation of nonlinear optical responses in the example system of MoS_(2) monolayer by van der Waals interfacial engineering.We found that,the interfacing of monolayer graphene will weaken the exciton oscillator strength in MoS_(2) monolayer and correspondingly suppress the second harmonic generation(SHG)intensity to 30%under band-gap resonance excitation.While with off-resonance excitation,the SHG intensity would enhance up to 130%,which is conjectured to be induced by the interlayer excitation between MoS_(2) and graphene.Our investigation provides an effective method for controlling nonlinear optical properties of two-dimensional materials and therefore facilitates their future applications in optoelectronic and photonic devices.

Order-Disorder Transition of Carboxyl Terminated Chains in Polydiacetylenes Vesicles Probed by Second Harmonic Generation and Two-Photon Fluorescence

To understand and control the interfacial properties of polydiacetylenes(PDAs)vesicles withπ-conjugated backbone is very important for their colorimetric sensing of chemical and biological targets.In this work,we adopted 10,12-pentacosadiynoic acid(PCDA)as the model molecule to prepare PDAs vesicles in aqueous solution with different forms(from monomer to blue-to-purple-to-red phase)by controlling the UV irradiation dose.The variations of the interfacial conformation of PDAs vesicles during chromatic transitions were inspected by the adsorption behaviors of probe molecules(4-(4-diethylaminostyry)-1-methylpyridinium iodide,D289)on vesicle surface with surface-specific second harmonic generation(SHG)and zeta potential measurements.Resonant SHG signal from D289 adsorbed on vesicle surface attenuated sharply,and the adsorption free energy as well as the corresponding two-photon fluorescence signal decreased slightly in chromatic transitions.While,the change in the surface density of the adsorbed D289 molecules for PDAs vesicles with different forms was relatively small as estimated from zeta potential measurements.The attenuation of the SHG intensity was thus attributed to the overall order-disorder transition and the changed orientation of D289 molecules caused by the gradual distortion of carboxyl head group driven by backbone perturbation.

Properties of periodic multicrystal configurations in walk-off-compensating second harmonic generation of ultrashort pulses

This work designs a four-platelet periodic multicrystal configuration in the second harmonic generation of ultra- short pulses as a new walk-off-compensating device. It theoretically investigates a proposed active and a typical passive compensating scheme with the undepleted-pump approximation. The result shows that the angular and spectral band- widths are proportional to the number of crystal pairs as expected, but the temperature tunability is basically unaltered owing to inter-plate pulse interference. At the same time, an analysis reveals that a misuse of the phase mismatch factor is responsible for a historic controversy about pulse interference. A real design of an ultraviolet second harmonic generation （262.5 nm） is considered in a passive periodic [3-Barium Borate-calcite configuration, where the inter-plate pulse interference is found to form an azimuthal tuning restriction and to lower plate length tolerance. A subsequent numerical simulation with pump depletion is in good accordance with theoretical prediction.

Study of narrow-band second harmonic generation from a broad-band fundamental pulse

This paper studies the type-I phase-matched second harmonic generation using 25-fs input laser pulses in a thick BBO crystal. The harmonic signal exhibits a narrow spectrum bandwidth, even though the input pulse has a broad bandwidth. The energy transfer efficiency and modulation of the fundamental spectrum are investigated.

Orientation Angle of Molecules at Hexadecane-Water Interface Studied with Total Internal Reflection Second Harmonic Generation

The orientation angle is an important parameter that reflects the structure of molecules at interfaces. In order to obtain this parameter, second order nonlinear spectroscopic techniques including second harmonic generation （SHG） and sum frequency generation-vibrational spec- troscopy （SFG-VS） have been successfully applied through analysis of the nonlinear signal from various polarizations. In some SHG and SFG-VS experiments, total internal reflection （TIR） configuration has been adopted to get enhanced signals. However, the reports on the detailed procedure of the polarization analysis and the calculation of the orientation angle of interracial molecules under TIR configuration are still very few. In this paper, we mea- sured the orientation angles of two molecules at the hexadecane-water interface under TIR and Non-TIR experimental configurations. The results measured from polarization analysis in TIR configuration consist with those obtained from Non-TIR configuration. This work demonstrates the feasibility and accuracy of polarization analysis in the determination of the orientation angle of molecules at the interfaces under TIR-SHG configuration.

Surface second harmonic generation of chiral molecules using three-coupled-oscillator model

Based on the three-coupled-oscillator molecular model we proposed, the relation between the second-order susceptibilities of a chiral film and the molecular hyperpolarizabilities is given. The effect of microscopic parameters on the second-order susceptibilities is simulated numerically and the difference between the efficiencies of s-polarized secondharmonic fields induced by the left- and the right-handed circularly-polarized fundamental beams is discussed. The theoretical basis for studying second-order nonlinear optical properties of the chiral molecular media with a tripod-like structure is provided in this paper.

Phase-matched second-harmonic generation in hybrid polymer-LN waveguides

Here we propose a hybrid polymer-LN waveguide for achieving phase-matched second-harmonic generation(SHG).From the aspect of super-mode theory,the geometric parameters of the hybrid semi-nonlinear waveguide were optimized to utilize both symmetric(even)and antisymmetric(odd)modes of the pump and SHG waves so as to facilitate phase matching with large modal overlap.Phase matching between a fundamental even(TE_(00)-like)mode at 1320 nm and a fundamental odd(TE_(01)-like)mode at 660 nm was found with a calculated modal overlap integral of 0.299,while utilizing the largest nonlinear coefficient d_(33),and achieving an efficient calculated normalized conversion efficiency of 148%W^(-1)·cm^(-2).Considering the fabrication feasibility of such hybrid waveguide with features including etchless,large dimension,and low structural sensitivity,we believe our findings would provide a useful reference for future on-chip efficient nonlinear conversion devices.

MULTIPHOTON MICROSCOPIC IMAGING OF MOUSE INTESTINAL MUCOSA BASED ON TWO-PHOTON EXCITED FLUORESCENCE AND SECOND HARMONIC GENERATION

Multiphoton microscopy(MPM),based on two-photon excited fuorescence and second harmonic generation,enables direct noninvasive visualization of tissue architecture and cell morphology in live tissues without the administration of exogenous contrast agents.In this paper,we used MPM to image the microstructures of the mucosa in fresh,unfixed,and unstained intestinal tissue of mouse.The morphology and distribution of the main components in mucosa layer such as columnar cells,goblet cells,intestinal glands,and a little collagen fibers were clearly observed in MPM images,and then compared with standard H&:E images from paired specimens.Our results indicate that MPM combined with endoscopy and miniaturization probes has the potential application in the clinical diagnosis and in vivo monitoring of early intestinal cancer.

Second harmonic generation in inhomogeneous MgO:LiNbO_3 waveguides

A fibre laser at 1111.6 nm is frequency doubled by two inhomogeneous MgO：LiNbO3 waveguides and the output powers of 85 mW and 49 mW at 555.8 nm have been generated with the conversion efficiencies of 47% and 27% respectively. By analysing the second harmonic generation temperature tuning curves, we investigate the influence of the optical inhomogeneities upon the conversion efficiency. The final result shows that the efficiency difference is mainly affected by the optical inhomogeneities in our case.

Second harmonic generation of metal nanoparticles under tightly focused illumination

The near-field and far-field second harmonic （SH） responses of a metal spherical nanoparticle placed in the focal region of a highly focused beam are investigated by using the calculation model based on three-dimensional finite-difference time-domain （FDTD） method. The results show that off-axis backward-propagating SH response can be reinforced by tightly focusing, due to the increase of the relative magnitude of the longitudinal field component and the phase shift along the propagation direction.

Broadband and efficient second harmonic generation in LiNbO_(3)-LiTaO_(3) composite ridge waveguides at telecom-band

Broadband nonlinear frequency conversions of optical waves are widely employed in multiple areas of optics and photonics. However, the broadening of conversion bandwidth is often at a cost of reduction in efficiency, which may induce a limitation on practical applications. Here we theoretically propose a novel design of LiNbO_(3) ridge waveguides on LiTaO_(3) substrates which can be used for efficient and broadband second harmonic generation. Through group velocity engineering of the ridge waveguides, acceptance bandwidth over 20 nm with a high conversion efficiency of > 25%W^(-1)·cm^(-2) is achieved at telecom-band.