The quantum metric manifested as the Riemannian metric in the parameter space of Bloch bands,characterizes the topology and geometry of quantum states.The second harmonic generation(SHG),as one of the fundamental nonl...The quantum metric manifested as the Riemannian metric in the parameter space of Bloch bands,characterizes the topology and geometry of quantum states.The second harmonic generation(SHG),as one of the fundamental nonlinear optical responses that links geometry of optical transitions to physical observables,despite being widely studied in various materials,its relation to quantum metric,especially in the dynamical regime,stays obscure.展开更多
In this theoretical study,we investigate the generation of second harmonics(SH)during the interaction of a laser beam with a metallic nanoparticle(MNP)trimer.Utilizing a classical electrodynamics framework,we explore ...In this theoretical study,we investigate the generation of second harmonics(SH)during the interaction of a laser beam with a metallic nanoparticle(MNP)trimer.Utilizing a classical electrodynamics framework,we explore the nonlinear interactions between the laser beam fields and nanoparticles(NPs),accounting for dipole-dipole interactions among the particles.Analytical expressions are derived to quantify the impact of these interactions on SH radiation power for two distinct polarizations of the laser beam.Our findings indicate that when the laser electric field is aligned parallel to the trimer's symmetry axis,there is a significant enhancement in SH radiation power compared to a single non-interacting NP,accompanied by a red-shift in the plasmon resonance peak.Conversely,when the laser electric field is perpendicular to the trimer axis,the SH radiation power from each NP decreases,and the plasmon resonance peak experiences a blue-shift.Additionally,we examine the influence of particle size and interparticle separation on SH generation.These results provide valuable insights into the role of interparticle interactions in enhancing nonlinear optical processes in NP assemblies,with potential implications for the design of nanophotonic devices.展开更多
Collagen characterization is crucial for disease diagnostics,prevention,and understanding,with growing focus on quantitative analysis at tissue and fibril levels.Numerous models have been developed to quantify structu...Collagen characterization is crucial for disease diagnostics,prevention,and understanding,with growing focus on quantitative analysis at tissue and fibril levels.Numerous models have been developed to quantify structural changes in collagen linked to various pathologies.However,many approaches remain limited to conceptual descriptions or rely on custom software,often requiring programming skills,which re-stricts their clinical application and potential impact.We introduce CollagenFitJ,a plugin for the open-source software platform ImageJ/FIJI,which represents a widely used microscopy image analysis tool.CollagenFitJ makes use of the cylindrical symmetry model for collagen to enable facile quantitative assessment of polarization-resolved second harmonic generation microscopy image stacks.The plugin’s main outputs are collagen structure-related maps(e.g.,orientation and anisotropy of collagen fibrils within the focal volume),which can be accompanied by distribution and randomness maps for a series of structure-related parameters.We describe and validate the use of CollagenFitJ on images acquired on rat-tail tendons,collagen capsules surrounding human thyroid nodules,and mouse colon tumors,using both scanning and widefield second harmonic generation microscopy datasets.The plugin was designed to be user-friendly,requiring little to no experience in image processing and coding to facilitate access for life scientists,medical staff,and microscopy practitioners with limited coding skills or time availability required for coding.展开更多
Silicon nitride photonics has emerged as a promising integrated optical platform due to its broad transparency window,low optical loss,and mature fabrication technology.However,the inherent centrosymmetric crystal str...Silicon nitride photonics has emerged as a promising integrated optical platform due to its broad transparency window,low optical loss,and mature fabrication technology.However,the inherent centrosymmetric crystal structure of silicon nitride fundamentally restricts its applications in second-order nonlinear optical processes.Monolayer transition metal dichalcogenides,particularly tungsten disulfide(WS_(2)),exhibit strong second-order nonlinear responses,making them ideal candidates for nonlinear photonic applications.Herein,we demonstrate a heterogeneously integrated platform combining silicon nitride waveguides with chemical vapor deposition(CVD)-grown monolayer WS_(2),enabling second harmonic generation.A specially designed silica cladding featuring gentle-slope profile on silicon nitride strip waveguides facilitates the integration of centimeter-scale WS_(2)film with photonic circuits.This approach provides a robust solution for incorporating second-order nonlinearity into silicon nitride photonic systems.The demonstrated platform holds significant potential for advancing quantum networks,visible-light lasers,and integrated optical modulation/detection systems.展开更多
Second harmonic generation(SHG),a fundamental and widely-studied phenomenon in nonlinear optics,has attracted significant attention for its ability to convert fundamental frequencies into their second harmonics.While ...Second harmonic generation(SHG),a fundamental and widely-studied phenomenon in nonlinear optics,has attracted significant attention for its ability to convert fundamental frequencies into their second harmonics.While the dominant SHG research has been focused on the optical and infrared regimes,its investigation in the microwave range presents challenges due to the requirements of materials with higher nonlinear coefficients and high-power microwave sources.Here,we provide an overview of methods together with underlying mechanisms for SHG in microwave frequencies,and discuss prospects and insights into the future developments of SHG-based technologies.The discussions on both numerical analyses and experimental studies will offer guidance for further SHG research and communication advancements in microwave regime.展开更多
Designing novel two-dimensional structures and precisely modulating their second harmonic generation(SHG)attributes are key to advancing nonlinear photonic technologies.In this work,through first-principles calculatio...Designing novel two-dimensional structures and precisely modulating their second harmonic generation(SHG)attributes are key to advancing nonlinear photonic technologies.In this work,through first-principles calculations,we propose a novel tetrahedral phase of transition metal dichalcogenides(TMDs)and validate its structural feasibility in a family of compounds,i.e.,ZX_(2)(Z=Ti,Zr,Hf;X=S,Se,Te).Cohesive energy and phonon dispersion calculations further demonstrate that eight of nine possible ZX_(2)monolayers are dynamically stable.All the ZX_(2)monolayers exhibit pronounced out-of-plane SHG with nonlinear susceptibility components reaching the order of 10^(2)pm/V.Strain engineering imposes a profound influence on the SHG response of ZX_(2)monolayers by reducing symmetry and modifying nonlinear susceptibility components.The redshift and significant enhancement of the prominent peak in SHG spectra are also revealed due to strain-induced charge redistribution and band gap reduction.Intriguingly,strain-driven nonlinear optical switching effects are realized in the ZX_(2)monolayers,with a reversible switching of SHG component ordering under tensile and compressive strain.In such a case,the anisotropic SHG pattern transforms from fourfold to twofold symmetry under the strain.Our work demonstrates the efficacy of strain engineering in precisely enhancing SHG,paving the way for the integration of novel TMD structures into tunable and flexible nonlinear optical devices.展开更多
The heterostructures incorporated with two or more distinctive two-dimensional(2D)materials have attracted great attention be-cause they could give rise to enhanced prop-erty in comparison with their individual counte...The heterostructures incorporated with two or more distinctive two-dimensional(2D)materials have attracted great attention be-cause they could give rise to enhanced prop-erty in comparison with their individual counterparts.Here,a water-assisted two-step rapid physical vapor deposition(rPVD)method was explored and used to synthesize Bi_(2)Te_(3)-Sb_(2)Te_(3)lateral het-erostructures(LHS)successfully.The Bi_(2)Te_(3)-Sb_(2)Te_(3)LHS is in nearly uniform size,and grows along three particular orientations with the intersection angles of 120°.Inter-estingly,we found that the water molecules play a significant role in determining the growth orientation,namely whether it will grow along the vertical or lateral direction in 2D structure.Hence,a growth mechanism of LHS based on the water-assisted two-step rPVD was present,which can be used as a general strategy and extended to the growth of other 2D heterostruc-tures or homostructures,such as SnS-SnSe LHS and SnS-SnS lateral homostructures.Fur-thermore,the second-harmonic generation intensity of the Bi_(2)Te_(3)-Sb_(2)Te_(3)LHS is much stronger than that of the Bi_(2)Te_(3)/Sb_(2)Te_(3)vertical heterostructures(VHS).This work opens a new approach for the synthesis of water-assisted lateral 2D heterostructures or homostruc-tures and offers a new method to enhance the second-harmonic generation properties of topo-logical insulating materials.展开更多
Directed self-assembly has been used to create micro-nano scale patterns,including chiral periodic structures of organic molecules,for potential applications in optics,photonics,metamaterials,and medical and sensing t...Directed self-assembly has been used to create micro-nano scale patterns,including chiral periodic structures of organic molecules,for potential applications in optics,photonics,metamaterials,and medical and sensing technologies.This study presents a straightforward approach for fabricating large-scale chiral grating porphyrin assemblies through template-assisted techniques.The solution of tetrakis(4-sulfonatophenyl)porphyrin(TPPS)was induced by chiral amino acids(L/D-arginine and L/D-serine)to selfassemble into highly ordered chiral grating structures with the assistance of sodium dodecyl sulfate(SDS).The structures show precise line widths(5.5μm)and gaps(18μm).Using in situ optical microscopy and second harmonic generation(SHG)microscopy,the chiral characteristics and dynamic evolution of the template-assisted self-assembly are investigated.It is found that the chirality of amino acids induced TPPS self-assembled into chiral structures and the liquid contraction interface significantly enhanced the chirality of the assemblies.This study is significant for understanding the mechanism of chiral evolution and designing novel micro-nano materials with predetermined chiral properties.展开更多
Polarization-dependent second harmonic generation is a widely utilized technique for characterizing symmetry.However,in collinear reflective geometry,the essential beam-splitting device significantly influences both t...Polarization-dependent second harmonic generation is a widely utilized technique for characterizing symmetry.However,in collinear reflective geometry,the essential beam-splitting device significantly influences both the polarization state of the fundamental and harmonic beams,thereby affecting the accuracy of the obtained second-order nonlinear susceptibility.Here,we propose a data correction method to solve this problem to obtain accurate secondorder nonlinear susceptibility.The feasibility and generality of the method are demonstrated through theoretical and experimental validation.展开更多
Two alkali-metal sulfamates nonlinear optical(NLO)crystals,Li(NH_(2)SO_(3))and Na(NH_(2)SO_(3)),have been obtained through the facile evaporation method.Li(NH_(2)SO_(3))crystallizes in the polar space group Pca2_(1)(N...Two alkali-metal sulfamates nonlinear optical(NLO)crystals,Li(NH_(2)SO_(3))and Na(NH_(2)SO_(3)),have been obtained through the facile evaporation method.Li(NH_(2)SO_(3))crystallizes in the polar space group Pca2_(1)(No.29).The structure of Li(NH_(2)SO_(3))can be described as a 3D network formed by[LiO_(4)]^(7-)polyhedral connecting with NH_(2)SO_(3)^(-)tetrahedra through corner-sharing.Na(NH_(2)SO_(3))crystallizes in the polar space group P2_(1)2_(1)2_(1)(No.19).The structure of Na(NH_(2)SO_(3))can be described as a 3D network formed by distorted[NaO_(6)]^(11-)octahedral connecting with NH_(2)SO_(3)^(-)tetrahedra through corner-sharing.The UV-Vis-near-infrared spectra demonstrate that Li(NH_(2)SO_(3))and Na(NH_(2)SO_(3))possessed large optical band gaps of 5.25 and 4.81 eV,respectively.Powder second-harmonic generation(SHG)measurements demonstrate that the SHG intensity of Li(NH_(2)SO_(3))and Na(NH_(2)SO_(3))were 0.32 times and 0.31 times that of KH_(2)PO_(4),respectively.First-principles calculations confirm the nonlinear optical performance mainly derived from the synergistic effect of amino sulfonate anions and alkali metal oxide anionic polyhedra.CCDC:2339109,Li(NH_(2)SO_(3));2339110,Na(NH_(2)SO_(3)).展开更多
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 p...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.展开更多
The chemical preparation, crystal structure and infrared spectroscopic characterization of the triaqua（4-amino-6-methoxypyrimidine） cuprate（II） sulfate, [Cu（C5H7N3）（H2O）3]SO4, is reported. The compound crystal...The chemical preparation, crystal structure and infrared spectroscopic characterization of the triaqua（4-amino-6-methoxypyrimidine） cuprate（II） sulfate, [Cu（C5H7N3）（H2O）3]SO4, is reported. The compound crystallizes in the noncentrosymmetric orthorhombic space group P212121 with lattice parameters a = 7.9025（3）, b = 11.1189（4）, c = 12.9720（4） , V = 1139.81（7） ~3 and Z = 4. The Cu（II） cation is fivecoordinated, in an early half-way between square pyramidal and trigonal bipyramidal fashion, by two nitrogen atoms of the 4-amino-6-methoxypyrimidine ligand and three water oxygen atoms. In the atomic arrangement, the organic ligands and the 5-connected Cu centers are linked with each other to give a 1-D corrugated hybrid chain running along the b-axis direction. The chains are interconnected by the SO4^（2-） anions via O–H...O, O–H...S, C–H...O and N–H...O hydrogen bonds to form layers spreading parallel to the（011） plane. The vibrational absorption bands were identified by infrared spectroscopy. Quantitative measurements of the second harmonic generation（SHG） of a powdered sample at 1064 nm were performed and a relative efficiency of 5.2 times the KDP standard was observed. Magnetic properties were also defined to characterize the complex. Magnetic measurements revealed that this material had a onedimensional antiferromagnetic character. The magnetic parameters were g = 2.11 and 2J/k B = -36 K.展开更多
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 d...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.展开更多
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 te...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.展开更多
Thin-film lithium niobate is a promising material platform for integrated nonlinear photonics,due to its high refractive index contrast with the excellent optical properties.However,the high refractive index contrast ...Thin-film lithium niobate is a promising material platform for integrated nonlinear photonics,due to its high refractive index contrast with the excellent optical properties.However,the high refractive index contrast and correspondingly small mode field diameter limit the attainable coupling between the waveguide and fiber.In second harmonic generation processes,lack of efficient fiber-chip coupling schemes covering both the fundamental and second harmonic wavelengths has greatly limited the overall efficiency.We design and fabricate an ultra-broadband tri-layer edge coupler with a high coupling efficiency.The coupler allows efficient coupling of 1 dB∕facet at 1550 nm and 3 dB∕facet at 775 nm.This enables us to achieve an ultrahigh overall second harmonic generation normalized efficiency(fiber-to-fiber)of 1027%W^(−1)cm^(−2)(on-chip second harmonic efficiency∼3256%W^(−1)cm^(−2))in a 5-mm-long periodically-poled lithium niobate waveguide,which is two to three orders of magnitude higher than that in state-of-the-art devices.展开更多
The purpose of this study is to explore the second harmonic generation(SHG)of a high power Cosh-Gaussian beam in cold collisionless plasma.The ponderomotive force causes carrier redistribution from high field to low f...The purpose of this study is to explore the second harmonic generation(SHG)of a high power Cosh-Gaussian beam in cold collisionless plasma.The ponderomotive force causes carrier redistribution from high field to low field region in presence of a Cosh-Gaussian beam thereby producing density gradients in the transverse direction.The density gradients so produced the results in electron plasma wave(EPW)generation at the frequency of the input beam.The EPW interacts with the input beam resulting in the production of 2nd harmonics.WKB and paraxial approximations are employed for obtaining the 2nd order differential equation describing the behavior of the beam’s spot size against normalized distance.The impact of well-established laser-plasma parameters on the behavior of the beam’s spot size and SHG yield are also analyzed.The focusing behavior of the beam and SHG yield is enhanced with an increase in the density of plasma,the radius of the beam and the decentred parameter,and with a decrease in the intensity of the beam.The results of the current problem are really helpful for complete information of laser-plasma interaction physics.展开更多
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 admini...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.展开更多
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 gene...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.展开更多
Stimulus re s ponsive materials can provide a variety of desirable properties in one equipment unit,such as optoelectronic devices,data communications,actuators,memories,sensors and capacitors.However,it remains a lar...Stimulus re s ponsive materials can provide a variety of desirable properties in one equipment unit,such as optoelectronic devices,data communications,actuators,memories,sensors and capacitors.However,it remains a large challenge to design such stimulus responsive materials,especially functional materials having both dielectric switch and second harmonic generation(SHG).Here,a new stimuli-responsive switchable material [(CH_(3))_(3)N(CH_(2))_(2)Cl]_(2)]Mn(SCN)_(4)(H_(2)O)_(2)] was discovered as a potential secondharmonic generation(SHG) dielectric switch.It is worth noting that it has SHG characteristics before and after undergoing reversible high-temperature phase transitions.In this work,we successfully refined the tetramethylammonium cation to obtain a quasi-spherical cation,which is tetramethylchloroethylamine(TMCEM) cation.By substituting H with a halogen,the increased steric hindrance of the molecular makes energy barrier increased,resulting in the reversible high-temperature phase transition.At the same time,the interactions of quasi-spherical cations and [Mn(SCN)_(4)(H_(2)O)_(2)]^(2-) anions affect a noncentrosymmetric structure to induce the SHG effect.These findings provide a new approach to design novel functional switch materials.展开更多
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 ...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.展开更多
基金supported by National Natural Science Foundation of China(Grant Nos.12025407,12474246,and 12450401)the National Key Research and Development Program of China(Grant No.2021YFA1400201)the Chinese Academy of Sciences(Grant Nos.YSBR-047 and XDB33030100)。
文摘The quantum metric manifested as the Riemannian metric in the parameter space of Bloch bands,characterizes the topology and geometry of quantum states.The second harmonic generation(SHG),as one of the fundamental nonlinear optical responses that links geometry of optical transitions to physical observables,despite being widely studied in various materials,its relation to quantum metric,especially in the dynamical regime,stays obscure.
文摘In this theoretical study,we investigate the generation of second harmonics(SH)during the interaction of a laser beam with a metallic nanoparticle(MNP)trimer.Utilizing a classical electrodynamics framework,we explore the nonlinear interactions between the laser beam fields and nanoparticles(NPs),accounting for dipole-dipole interactions among the particles.Analytical expressions are derived to quantify the impact of these interactions on SH radiation power for two distinct polarizations of the laser beam.Our findings indicate that when the laser electric field is aligned parallel to the trimer's symmetry axis,there is a significant enhancement in SH radiation power compared to a single non-interacting NP,accompanied by a red-shift in the plasmon resonance peak.Conversely,when the laser electric field is perpendicular to the trimer axis,the SH radiation power from each NP decreases,and the plasmon resonance peak experiences a blue-shift.Additionally,we examine the influence of particle size and interparticle separation on SH generation.These results provide valuable insights into the role of interparticle interactions in enhancing nonlinear optical processes in NP assemblies,with potential implications for the design of nanophotonic devices.
基金supported by the Ministry of Research,Innovation and Digitalization,CNCS-UEFISCDI[Grant Nos.RO-NO-2019-0601(MEDYCONAI),PN-III-P4-PCE-2021-0444(RESONANO)]PN-IV-P1-PCE-2023-1137+2 种基金supported in part by IN2SIGHT,European Union’s Horizon 2020(GA.no.964481)by the Research Council of Lithuania(LMTLTAgreement No.P-MIP-23-237).
文摘Collagen characterization is crucial for disease diagnostics,prevention,and understanding,with growing focus on quantitative analysis at tissue and fibril levels.Numerous models have been developed to quantify structural changes in collagen linked to various pathologies.However,many approaches remain limited to conceptual descriptions or rely on custom software,often requiring programming skills,which re-stricts their clinical application and potential impact.We introduce CollagenFitJ,a plugin for the open-source software platform ImageJ/FIJI,which represents a widely used microscopy image analysis tool.CollagenFitJ makes use of the cylindrical symmetry model for collagen to enable facile quantitative assessment of polarization-resolved second harmonic generation microscopy image stacks.The plugin’s main outputs are collagen structure-related maps(e.g.,orientation and anisotropy of collagen fibrils within the focal volume),which can be accompanied by distribution and randomness maps for a series of structure-related parameters.We describe and validate the use of CollagenFitJ on images acquired on rat-tail tendons,collagen capsules surrounding human thyroid nodules,and mouse colon tumors,using both scanning and widefield second harmonic generation microscopy datasets.The plugin was designed to be user-friendly,requiring little to no experience in image processing and coding to facilitate access for life scientists,medical staff,and microscopy practitioners with limited coding skills or time availability required for coding.
基金Project supported by the National Innovative Training Program for College Students of China(Grant No.2023069)the University Research and Innovation Project of the National University of Defense Technology。
文摘Silicon nitride photonics has emerged as a promising integrated optical platform due to its broad transparency window,low optical loss,and mature fabrication technology.However,the inherent centrosymmetric crystal structure of silicon nitride fundamentally restricts its applications in second-order nonlinear optical processes.Monolayer transition metal dichalcogenides,particularly tungsten disulfide(WS_(2)),exhibit strong second-order nonlinear responses,making them ideal candidates for nonlinear photonic applications.Herein,we demonstrate a heterogeneously integrated platform combining silicon nitride waveguides with chemical vapor deposition(CVD)-grown monolayer WS_(2),enabling second harmonic generation.A specially designed silica cladding featuring gentle-slope profile on silicon nitride strip waveguides facilitates the integration of centimeter-scale WS_(2)film with photonic circuits.This approach provides a robust solution for incorporating second-order nonlinearity into silicon nitride photonic systems.The demonstrated platform holds significant potential for advancing quantum networks,visible-light lasers,and integrated optical modulation/detection systems.
基金supported by the National Natural Science Foun-dation of China(No.12274339).
文摘Second harmonic generation(SHG),a fundamental and widely-studied phenomenon in nonlinear optics,has attracted significant attention for its ability to convert fundamental frequencies into their second harmonics.While the dominant SHG research has been focused on the optical and infrared regimes,its investigation in the microwave range presents challenges due to the requirements of materials with higher nonlinear coefficients and high-power microwave sources.Here,we provide an overview of methods together with underlying mechanisms for SHG in microwave frequencies,and discuss prospects and insights into the future developments of SHG-based technologies.The discussions on both numerical analyses and experimental studies will offer guidance for further SHG research and communication advancements in microwave regime.
基金supported by the National Natural Science Foundation of China(Grant Nos.12304220,12174157,12074150,and 12374174)the Natural Science Foundation of Jiangsu Province(Grant No.BK20230518)+2 种基金the China Postdoctoral Science Foundation(Grant No.2023M731383)the College Student Innovation Project(Grant No.202410299946X)the Scientific Research Project of Jiangsu University(Grant No.22A397).
文摘Designing novel two-dimensional structures and precisely modulating their second harmonic generation(SHG)attributes are key to advancing nonlinear photonic technologies.In this work,through first-principles calculations,we propose a novel tetrahedral phase of transition metal dichalcogenides(TMDs)and validate its structural feasibility in a family of compounds,i.e.,ZX_(2)(Z=Ti,Zr,Hf;X=S,Se,Te).Cohesive energy and phonon dispersion calculations further demonstrate that eight of nine possible ZX_(2)monolayers are dynamically stable.All the ZX_(2)monolayers exhibit pronounced out-of-plane SHG with nonlinear susceptibility components reaching the order of 10^(2)pm/V.Strain engineering imposes a profound influence on the SHG response of ZX_(2)monolayers by reducing symmetry and modifying nonlinear susceptibility components.The redshift and significant enhancement of the prominent peak in SHG spectra are also revealed due to strain-induced charge redistribution and band gap reduction.Intriguingly,strain-driven nonlinear optical switching effects are realized in the ZX_(2)monolayers,with a reversible switching of SHG component ordering under tensile and compressive strain.In such a case,the anisotropic SHG pattern transforms from fourfold to twofold symmetry under the strain.Our work demonstrates the efficacy of strain engineering in precisely enhancing SHG,paving the way for the integration of novel TMD structures into tunable and flexible nonlinear optical devices.
基金supported by the Natural Science Foundation of Fujian Province of China(2022J01646)。
文摘The heterostructures incorporated with two or more distinctive two-dimensional(2D)materials have attracted great attention be-cause they could give rise to enhanced prop-erty in comparison with their individual counterparts.Here,a water-assisted two-step rapid physical vapor deposition(rPVD)method was explored and used to synthesize Bi_(2)Te_(3)-Sb_(2)Te_(3)lateral het-erostructures(LHS)successfully.The Bi_(2)Te_(3)-Sb_(2)Te_(3)LHS is in nearly uniform size,and grows along three particular orientations with the intersection angles of 120°.Inter-estingly,we found that the water molecules play a significant role in determining the growth orientation,namely whether it will grow along the vertical or lateral direction in 2D structure.Hence,a growth mechanism of LHS based on the water-assisted two-step rPVD was present,which can be used as a general strategy and extended to the growth of other 2D heterostruc-tures or homostructures,such as SnS-SnSe LHS and SnS-SnS lateral homostructures.Fur-thermore,the second-harmonic generation intensity of the Bi_(2)Te_(3)-Sb_(2)Te_(3)LHS is much stronger than that of the Bi_(2)Te_(3)/Sb_(2)Te_(3)vertical heterostructures(VHS).This work opens a new approach for the synthesis of water-assisted lateral 2D heterostructures or homostruc-tures and offers a new method to enhance the second-harmonic generation properties of topo-logical insulating materials.
基金funding from the National Natural Science Foundation of China(NSFC,Nos.22173112 and 91856121)Chinese Academy of Sciences for support(No.YJKYYQ20180014)。
文摘Directed self-assembly has been used to create micro-nano scale patterns,including chiral periodic structures of organic molecules,for potential applications in optics,photonics,metamaterials,and medical and sensing technologies.This study presents a straightforward approach for fabricating large-scale chiral grating porphyrin assemblies through template-assisted techniques.The solution of tetrakis(4-sulfonatophenyl)porphyrin(TPPS)was induced by chiral amino acids(L/D-arginine and L/D-serine)to selfassemble into highly ordered chiral grating structures with the assistance of sodium dodecyl sulfate(SDS).The structures show precise line widths(5.5μm)and gaps(18μm).Using in situ optical microscopy and second harmonic generation(SHG)microscopy,the chiral characteristics and dynamic evolution of the template-assisted self-assembly are investigated.It is found that the chirality of amino acids induced TPPS self-assembled into chiral structures and the liquid contraction interface significantly enhanced the chirality of the assemblies.This study is significant for understanding the mechanism of chiral evolution and designing novel micro-nano materials with predetermined chiral properties.
基金This work was supported by the National Natural Science Foundation of China(No.U2230203)the Fundamental Research Funds for the Central Universities.
文摘Polarization-dependent second harmonic generation is a widely utilized technique for characterizing symmetry.However,in collinear reflective geometry,the essential beam-splitting device significantly influences both the polarization state of the fundamental and harmonic beams,thereby affecting the accuracy of the obtained second-order nonlinear susceptibility.Here,we propose a data correction method to solve this problem to obtain accurate secondorder nonlinear susceptibility.The feasibility and generality of the method are demonstrated through theoretical and experimental validation.
文摘Two alkali-metal sulfamates nonlinear optical(NLO)crystals,Li(NH_(2)SO_(3))and Na(NH_(2)SO_(3)),have been obtained through the facile evaporation method.Li(NH_(2)SO_(3))crystallizes in the polar space group Pca2_(1)(No.29).The structure of Li(NH_(2)SO_(3))can be described as a 3D network formed by[LiO_(4)]^(7-)polyhedral connecting with NH_(2)SO_(3)^(-)tetrahedra through corner-sharing.Na(NH_(2)SO_(3))crystallizes in the polar space group P2_(1)2_(1)2_(1)(No.19).The structure of Na(NH_(2)SO_(3))can be described as a 3D network formed by distorted[NaO_(6)]^(11-)octahedral connecting with NH_(2)SO_(3)^(-)tetrahedra through corner-sharing.The UV-Vis-near-infrared spectra demonstrate that Li(NH_(2)SO_(3))and Na(NH_(2)SO_(3))possessed large optical band gaps of 5.25 and 4.81 eV,respectively.Powder second-harmonic generation(SHG)measurements demonstrate that the SHG intensity of Li(NH_(2)SO_(3))and Na(NH_(2)SO_(3))were 0.32 times and 0.31 times that of KH_(2)PO_(4),respectively.First-principles calculations confirm the nonlinear optical performance mainly derived from the synergistic effect of amino sulfonate anions and alkali metal oxide anionic polyhedra.CCDC:2339109,Li(NH_(2)SO_(3));2339110,Na(NH_(2)SO_(3)).
基金Supported by the National Natural Science Foundation of China under Grant Nos 51325504,11474093,11622430 and 11474361the National Key Research and Development Program of China(2016YFC0801903-02)the Fundamental Research Funds for the Central Universities
文摘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.
基金support provided by the Secretary of State for Scientific Research and Technology of TunisiaThe X-ray diffractometer was funded by NSF Grant 0087210, Ohio Board of Regents Grant CAP-491 and by Youngstown State University, USA
文摘The chemical preparation, crystal structure and infrared spectroscopic characterization of the triaqua（4-amino-6-methoxypyrimidine） cuprate（II） sulfate, [Cu（C5H7N3）（H2O）3]SO4, is reported. The compound crystallizes in the noncentrosymmetric orthorhombic space group P212121 with lattice parameters a = 7.9025（3）, b = 11.1189（4）, c = 12.9720（4） , V = 1139.81（7） ~3 and Z = 4. The Cu（II） cation is fivecoordinated, in an early half-way between square pyramidal and trigonal bipyramidal fashion, by two nitrogen atoms of the 4-amino-6-methoxypyrimidine ligand and three water oxygen atoms. In the atomic arrangement, the organic ligands and the 5-connected Cu centers are linked with each other to give a 1-D corrugated hybrid chain running along the b-axis direction. The chains are interconnected by the SO4^（2-） anions via O–H...O, O–H...S, C–H...O and N–H...O hydrogen bonds to form layers spreading parallel to the（011） plane. The vibrational absorption bands were identified by infrared spectroscopy. Quantitative measurements of the second harmonic generation（SHG） of a powdered sample at 1064 nm were performed and a relative efficiency of 5.2 times the KDP standard was observed. Magnetic properties were also defined to characterize the complex. Magnetic measurements revealed that this material had a onedimensional antiferromagnetic character. The magnetic parameters were g = 2.11 and 2J/k B = -36 K.
文摘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.
基金financial supports from the National Natural Science Foundation of China(Grant No.11604150)Fundamental Research Funds for the Central Universities of China(Grant No.ZYGX2020J010)M.Rahmani.acknowledges support from the UK Research and Innovation Future Leaders Fellowship(MR/T040513/1)。
文摘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.
基金sponsored by the National Key R&D Program of China(Grant No.2019YFA0705000)the National Natural Science Foundation of China(Grant Nos.11690031 and 11761131001).
文摘Thin-film lithium niobate is a promising material platform for integrated nonlinear photonics,due to its high refractive index contrast with the excellent optical properties.However,the high refractive index contrast and correspondingly small mode field diameter limit the attainable coupling between the waveguide and fiber.In second harmonic generation processes,lack of efficient fiber-chip coupling schemes covering both the fundamental and second harmonic wavelengths has greatly limited the overall efficiency.We design and fabricate an ultra-broadband tri-layer edge coupler with a high coupling efficiency.The coupler allows efficient coupling of 1 dB∕facet at 1550 nm and 3 dB∕facet at 775 nm.This enables us to achieve an ultrahigh overall second harmonic generation normalized efficiency(fiber-to-fiber)of 1027%W^(−1)cm^(−2)(on-chip second harmonic efficiency∼3256%W^(−1)cm^(−2))in a 5-mm-long periodically-poled lithium niobate waveguide,which is two to three orders of magnitude higher than that in state-of-the-art devices.
文摘The purpose of this study is to explore the second harmonic generation(SHG)of a high power Cosh-Gaussian beam in cold collisionless plasma.The ponderomotive force causes carrier redistribution from high field to low field region in presence of a Cosh-Gaussian beam thereby producing density gradients in the transverse direction.The density gradients so produced the results in electron plasma wave(EPW)generation at the frequency of the input beam.The EPW interacts with the input beam resulting in the production of 2nd harmonics.WKB and paraxial approximations are employed for obtaining the 2nd order differential equation describing the behavior of the beam’s spot size against normalized distance.The impact of well-established laser-plasma parameters on the behavior of the beam’s spot size and SHG yield are also analyzed.The focusing behavior of the beam and SHG yield is enhanced with an increase in the density of plasma,the radius of the beam and the decentred parameter,and with a decrease in the intensity of the beam.The results of the current problem are really helpful for complete information of laser-plasma interaction physics.
基金supported by the Program for Changjiang Scholars and Innovative Research Team in University(Grant No.IRT1115)the National Natural Science Foundation of China(Grant Nos.81271620,61275006,81101209,30970783).
文摘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.
文摘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.
基金supported by the National Natural Science Foundation of China(Nos.21673038,21771037,21805033)Natural Science Foundation of Jiangsu Province(JSNSF,No.BK20170659)。
文摘Stimulus re s ponsive materials can provide a variety of desirable properties in one equipment unit,such as optoelectronic devices,data communications,actuators,memories,sensors and capacitors.However,it remains a large challenge to design such stimulus responsive materials,especially functional materials having both dielectric switch and second harmonic generation(SHG).Here,a new stimuli-responsive switchable material [(CH_(3))_(3)N(CH_(2))_(2)Cl]_(2)]Mn(SCN)_(4)(H_(2)O)_(2)] was discovered as a potential secondharmonic generation(SHG) dielectric switch.It is worth noting that it has SHG characteristics before and after undergoing reversible high-temperature phase transitions.In this work,we successfully refined the tetramethylammonium cation to obtain a quasi-spherical cation,which is tetramethylchloroethylamine(TMCEM) cation.By substituting H with a halogen,the increased steric hindrance of the molecular makes energy barrier increased,resulting in the reversible high-temperature phase transition.At the same time,the interactions of quasi-spherical cations and [Mn(SCN)_(4)(H_(2)O)_(2)]^(2-) anions affect a noncentrosymmetric structure to induce the SHG effect.These findings provide a new approach to design novel functional switch materials.
文摘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.
