High-precision optical frequency measurement serves as a cornerstone of modern science and technology,enabling advancements in fields ranging from fundamental physics to quantum information technologies.Obtaining prec...High-precision optical frequency measurement serves as a cornerstone of modern science and technology,enabling advancements in fields ranging from fundamental physics to quantum information technologies.Obtaining precise photon frequencies,especially in the ultraviolet or even extreme ultraviolet regimes,is a key goal in both light–matter interaction experiments and engineering applications.High-order harmonic generation(HHG)is an ideal light source for producing such photons.In this work,we propose an optical temporal interference model(OTIM)that establishes an analogy with multi-slit Fraunhofer diffraction(MSFD)to manipulate fine-frequency photon generation by exploiting the temporal coherence of HHG processes.Our model provides a unified physical framework for three distinct non-integer HHG generation schemes:single-pulse,shaped-pulse,and laser pulse train approaches,which correspond to single-MSFD-like,double-MSFD-like,and multi-MSFD-like processes,respectively.Arbitrary non-integer HHG photons can be obtained using our scheme.Our approach provides a new perspective for accurately measuring and controlling photon frequencies in fields such as frequency comb technology,interferometry,and atomic clocks.展开更多
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
Multi-electron and multi-orbital effects play a crucial role in the interaction of strong laser fields with complex molecules.Here,multi-electron effects encompass not only electron-electron Coulomb interactions and e...Multi-electron and multi-orbital effects play a crucial role in the interaction of strong laser fields with complex molecules.Here,multi-electron effects encompass not only electron-electron Coulomb interactions and exchangecorrelation effects but also the interference between the dynamics of different electron wave packets.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
Permanent dipole moments induced high-order harmonic generation(HHG)signals offer a potential approach to producing elliptically or even circularly polarized X-ray attosecond sources.Previous studies on this topic hav...Permanent dipole moments induced high-order harmonic generation(HHG)signals offer a potential approach to producing elliptically or even circularly polarized X-ray attosecond sources.Previous studies on this topic have mainly focused on diatomic molecules such as CO and HeH.Based on this scheme,significant HHG signals in the direction perpendicular to the molecular axis can be observed in both the high-energy and low-energy regions.However,we found that the high-order harmonics induced by the permanent dipole moments of polyatomic complex molecules involve more intricate physical processes.Using time-dependent density functional theory,we simulated the dynamics of HHG from NH2COOH and NH2COSH interacting with linearly polarized lasers.We found that the harmonic signals in the direction perpendicular to the N-C bond were significantly enhanced in the high-energy photon region.Our analysis indicates that this is due to the complex molecular configuration of NH_(2)COOH and NH_(2)COSH:while the NH_(2) group has C_(2v) symmetry,both COOH and COSH groups lack this symmetry.This structural characteristic results in permanent dipole moments being felt only when electrons return to either COSH or COOH groups,but not to NH_(2) group.Additionally,our results reveal a multi-plateau structure in HHG signal along laser polarization direction,a phenomenon arising from multi-electron and multiorbital effects during interaction between complex molecule and strong laser field.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
We theoretically investigate the high-order harmonic generation(HHG)of defect-free solids by solving the timedependent Schrodinger equation(TDSE).The results show that the harmonic intensity can be enhanced,harmonic o...We theoretically investigate the high-order harmonic generation(HHG)of defect-free solids by solving the timedependent Schrodinger equation(TDSE).The results show that the harmonic intensity can be enhanced,harmonic order can be extended,and modulation near the cutoff order becomes smaller for the second plateau by increasing the time delay.These effects are due to an increase of the electron population in higher energy bands,where the larger band gap allows electrons to release more energy,and the long electronic paths are suppressed.Additionally,we also investigate the HHG of defective solids by Bohmian trajectories(BT).It is found that the harmonic intensity of the second plateau can be further enhanced.Simultaneously,cutoff order is also extended due to Bohmian particles moving farther away from the defective zone.展开更多
We present a comprehensive study on the role of various excited states in high-order harmonic generation of hydrogen atoms driven by a long-wavelength(1500 nm)laser field.By numerically solving the time-dependent Schr...We present a comprehensive study on the role of various excited states in high-order harmonic generation of hydrogen atoms driven by a long-wavelength(1500 nm)laser field.By numerically solving the time-dependent Schrodinger equation(TDSE)and performing a time-frequency analysis,we investigate the influence of individual excited states on the harmonic spectrum.Our results reveal that the 2s excited state primarily contributes to the enhancement of high-energy harmonic yields by facilitating long electron trajectories,while the 2p excited state predominantly suppresses harmonic yields in the lower-energy region(20th-50th orders)by altering the contributions of electron trajectories.Our results highlight the critical role of the excited states in the HHG process,even at longer laser wavelengths.展开更多
We performed real-time and real-space numerical simulations of high-order harmonic generation in the threedimensional structured molecule methane(CH_(4)) using time-dependent density functional theory. By irradiating ...We performed real-time and real-space numerical simulations of high-order harmonic generation in the threedimensional structured molecule methane(CH_(4)) using time-dependent density functional theory. By irradiating the methane molecule with an elliptically polarized laser pulse polarized in the x–y plane, we observed significant even-order harmonic emission in the z-direction. By analyzing the electron dynamics in the electric field and the multi-orbital effects of the molecule, we revealed that electron recombination near specific atoms in methane is the primary source of highorder harmonic generation in the z-direction. Furthermore, we identified the dominant molecular orbitals responsible for the enhancement of harmonics in this direction and demonstrated the critical role played by multi-orbital effects in this process.展开更多
Two types of bound states in continuum(BICs),symmetry-protected and Brillouin zone folding driven,are identified in hollow Si nanorod arrays.By modulating the direction and distance of the air holes from the center of...Two types of bound states in continuum(BICs),symmetry-protected and Brillouin zone folding driven,are identified in hollow Si nanorod arrays.By modulating the direction and distance of the air holes from the center of the nanorods,it is possible to achieve either a single quasi-BIC or three quasi-BICs.The transmission spectra exhibit ultra-narrow lines,and the quasi-BICs demonstrate ultra-high Q factors.Additionally,efficient third-harmonic generation occurs at low pump intensities.The results indicate that the proposed nanostructures of two types of BICs with a flexible modulation hold great potential applications for nonlinear photonic devices.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
We experimentally demonstrated a diode-pumped Kerr-lens mode-locked femtosecond（fs） laser with a self-frequency doubling Yb：YCa_4O（BO_3）_3 crystal.Sub-40 fs laser pulses were directly generated from the oscillato...We experimentally demonstrated a diode-pumped Kerr-lens mode-locked femtosecond（fs） laser with a self-frequency doubling Yb：YCa_4O（BO_3）_3 crystal.Sub-40 fs laser pulses were directly generated from the oscillator without extracavity compression.The central wavelength was tunable from 1039 nm to 1049 nm with a typical bandwidth of 35 nm and an average output power of 53 mW.For the first time,a self-frequency doubled second harmonic green laser with tunable range from 519 nm to 525 nm was observed.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
The spatial distribution in high-order harmonic generation（HHG） is theoretically investigated by using a few-cycle laser pulse from a two-dimensional model of a hydrogen molecular ion. The spatial distribution in HH...The spatial distribution in high-order harmonic generation（HHG） is theoretically investigated by using a few-cycle laser pulse from a two-dimensional model of a hydrogen molecular ion. The spatial distribution in HHG demonstrates that the harmonic spectra are sensitive to the carrier envelope phase and the duration of the laser pulse. The HHG can be restrained by a pulse with the duration of 5 fs in the region from the 90 th to 320th order. This characteristic is illustrated by the probability density of electron wave packet distribution. The electron is mainly located near the nucleus along the positive-x direction from 3.0 o.c. to 3.2 o.c., which is an important time to generate the HHG in the plateau area. We also demonstrate the time-frequency distribution in the region of the positive-and negative-x direction to explain the physical mechanism.展开更多
基金supported by the National Natural Science Foundation of China(Grant No.12304379)the Natural Science Foundation of Liaoning Province(Grant No.2024BS-269)the Guangdong Basic and Applied Basic Research Foundation(Grant No.025A1515011117)。
文摘High-precision optical frequency measurement serves as a cornerstone of modern science and technology,enabling advancements in fields ranging from fundamental physics to quantum information technologies.Obtaining precise photon frequencies,especially in the ultraviolet or even extreme ultraviolet regimes,is a key goal in both light–matter interaction experiments and engineering applications.High-order harmonic generation(HHG)is an ideal light source for producing such photons.In this work,we propose an optical temporal interference model(OTIM)that establishes an analogy with multi-slit Fraunhofer diffraction(MSFD)to manipulate fine-frequency photon generation by exploiting the temporal coherence of HHG processes.Our model provides a unified physical framework for three distinct non-integer HHG generation schemes:single-pulse,shaped-pulse,and laser pulse train approaches,which correspond to single-MSFD-like,double-MSFD-like,and multi-MSFD-like processes,respectively.Arbitrary non-integer HHG photons can be obtained using our scheme.Our approach provides a new perspective for accurately measuring and controlling photon frequencies in fields such as frequency comb technology,interferometry,and atomic clocks.
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 National Key Research and Development Program of China(Grant No.2022YFE0134200)the National Natural Science Foundation of China(Grant No.12204214)+1 种基金the Fundamental Research Funds for the Central Universities(Grant No.GK202207012)QCYRCXM-2022-241。
文摘Multi-electron and multi-orbital effects play a crucial role in the interaction of strong laser fields with complex molecules.Here,multi-electron effects encompass not only electron-electron Coulomb interactions and exchangecorrelation effects but also the interference between the dynamics of different electron wave packets.
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supported by the Fundamental Research Funds for the Central Universities(Grant Nos.GK202207012 and QCYRCXM-2022-241).
文摘Permanent dipole moments induced high-order harmonic generation(HHG)signals offer a potential approach to producing elliptically or even circularly polarized X-ray attosecond sources.Previous studies on this topic have mainly focused on diatomic molecules such as CO and HeH.Based on this scheme,significant HHG signals in the direction perpendicular to the molecular axis can be observed in both the high-energy and low-energy regions.However,we found that the high-order harmonics induced by the permanent dipole moments of polyatomic complex molecules involve more intricate physical processes.Using time-dependent density functional theory,we simulated the dynamics of HHG from NH2COOH and NH2COSH interacting with linearly polarized lasers.We found that the harmonic signals in the direction perpendicular to the N-C bond were significantly enhanced in the high-energy photon region.Our analysis indicates that this is due to the complex molecular configuration of NH_(2)COOH and NH_(2)COSH:while the NH_(2) group has C_(2v) symmetry,both COOH and COSH groups lack this symmetry.This structural characteristic results in permanent dipole moments being felt only when electrons return to either COSH or COOH groups,but not to NH_(2) group.Additionally,our results reveal a multi-plateau structure in HHG signal along laser polarization direction,a phenomenon arising from multi-electron and multiorbital effects during interaction between complex molecule and strong laser field.
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supported by the Natural Science Foundation of Jilin Province of China(Grant No.20230101014JC)the Fundamental Research Funds for the Central Universities(Grant No.2572021BC05)the National Natural Science Foundation of China(Grant No.12374265)。
文摘We theoretically investigate the high-order harmonic generation(HHG)of defect-free solids by solving the timedependent Schrodinger equation(TDSE).The results show that the harmonic intensity can be enhanced,harmonic order can be extended,and modulation near the cutoff order becomes smaller for the second plateau by increasing the time delay.These effects are due to an increase of the electron population in higher energy bands,where the larger band gap allows electrons to release more energy,and the long electronic paths are suppressed.Additionally,we also investigate the HHG of defective solids by Bohmian trajectories(BT).It is found that the harmonic intensity of the second plateau can be further enhanced.Simultaneously,cutoff order is also extended due to Bohmian particles moving farther away from the defective zone.
基金supported by the Scientific and Technological Innovation Programs of Higher Education Institutions in Shanxi。
文摘We present a comprehensive study on the role of various excited states in high-order harmonic generation of hydrogen atoms driven by a long-wavelength(1500 nm)laser field.By numerically solving the time-dependent Schrodinger equation(TDSE)and performing a time-frequency analysis,we investigate the influence of individual excited states on the harmonic spectrum.Our results reveal that the 2s excited state primarily contributes to the enhancement of high-energy harmonic yields by facilitating long electron trajectories,while the 2p excited state predominantly suppresses harmonic yields in the lower-energy region(20th-50th orders)by altering the contributions of electron trajectories.Our results highlight the critical role of the excited states in the HHG process,even at longer laser wavelengths.
基金Project supported by the National Natural Science Foundation of China (Grant No. 12204214)the National Key Research and Development Program of China (Grant No. 2022YFE0134200)+1 种基金the Fundamental Research Funds for the Central Universities (Grant No. GK202207012), QCYRCXM-2022-241the Guangdong Basic and Applied Basic Research Foundation (Grant No. 2025A1515011117)。
文摘We performed real-time and real-space numerical simulations of high-order harmonic generation in the threedimensional structured molecule methane(CH_(4)) using time-dependent density functional theory. By irradiating the methane molecule with an elliptically polarized laser pulse polarized in the x–y plane, we observed significant even-order harmonic emission in the z-direction. By analyzing the electron dynamics in the electric field and the multi-orbital effects of the molecule, we revealed that electron recombination near specific atoms in methane is the primary source of highorder harmonic generation in the z-direction. Furthermore, we identified the dominant molecular orbitals responsible for the enhancement of harmonics in this direction and demonstrated the critical role played by multi-orbital effects in this process.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.12174228 and 12274271)。
文摘Two types of bound states in continuum(BICs),symmetry-protected and Brillouin zone folding driven,are identified in hollow Si nanorod arrays.By modulating the direction and distance of the air holes from the center of the nanorods,it is possible to achieve either a single quasi-BIC or three quasi-BICs.The transmission spectra exhibit ultra-narrow lines,and the quasi-BICs demonstrate ultra-high Q factors.Additionally,efficient third-harmonic generation occurs at low pump intensities.The results indicate that the proposed nanostructures of two types of BICs with a flexible modulation hold great potential applications for nonlinear photonic devices.
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Project supported by the National Major Scientific Instruments Development Project of China(Grant No.2012YQ120047)the National Natural Science Foundation of China(Grant No.61205130)the Doctor Fund from Southwest University,China(Grant No.SWU110645)
文摘We experimentally demonstrated a diode-pumped Kerr-lens mode-locked femtosecond（fs） laser with a self-frequency doubling Yb：YCa_4O（BO_3）_3 crystal.Sub-40 fs laser pulses were directly generated from the oscillator without extracavity compression.The central wavelength was tunable from 1039 nm to 1049 nm with a typical bandwidth of 35 nm and an average output power of 53 mW.For the first time,a self-frequency doubled second harmonic green laser with tunable range from 519 nm to 525 nm was observed.
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Project supported by the National Natural Science Foundation of China(Grant Nos.11504221,61575077,11404204,and 11447208)the Natural Science Foundation for Young Scientists of Shanxi Province,China(Grant No.2015021023)Program for the Top Young Academic Leaders of Higher Learning Institutions of Shanxi Province,China
文摘The spatial distribution in high-order harmonic generation（HHG） is theoretically investigated by using a few-cycle laser pulse from a two-dimensional model of a hydrogen molecular ion. The spatial distribution in HHG demonstrates that the harmonic spectra are sensitive to the carrier envelope phase and the duration of the laser pulse. The HHG can be restrained by a pulse with the duration of 5 fs in the region from the 90 th to 320th order. This characteristic is illustrated by the probability density of electron wave packet distribution. The electron is mainly located near the nucleus along the positive-x direction from 3.0 o.c. to 3.2 o.c., which is an important time to generate the HHG in the plateau area. We also demonstrate the time-frequency distribution in the region of the positive-and negative-x direction to explain the physical mechanism.
