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 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
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
The third-harmonic generation(THG)coefficient for a spherical quantum dot system with inversely quadratic Hellmann plus inversely quadratic potential is investigated theoretically,considering the regulation of quantum...The third-harmonic generation(THG)coefficient for a spherical quantum dot system with inversely quadratic Hellmann plus inversely quadratic potential is investigated theoretically,considering the regulation of quantum size,confinement potential depth and the external environment.The numerical simulation results indicate that the THG coefficient can reach the order of 10~(-12)m~2V~(-2),which strongly relies on the tunable factor,with its resonant peak experiencing a redshift or blueshift.Interestingly,the effect of temperature on the THG coefficient in terms of peak location and size is consistent with the quantum dot radius but contrasts with the hydrostatic pressure.Thus,it is crucial to focus on the influence of internal and external parameters on nonlinear optical effects,and to implement the theory in practical experiments and the manufacture of optoelectronic devices.展开更多
In high harmonic generation(HHG),Laguerre–Gaussian(LG) beams are used to generate extreme ultraviolet(XUV)vortices with well-defined orbital angular momentum(OAM),which have potential applications in fields such as m...In high harmonic generation(HHG),Laguerre–Gaussian(LG) beams are used to generate extreme ultraviolet(XUV)vortices with well-defined orbital angular momentum(OAM),which have potential applications in fields such as microscopy and spectroscopy.An experimental study on the HHG driven by vortex and Gaussian beams is conducted in this work.It is found that the intensity of vortex harmonics is positively correlated with the laser energy and gas pressure.The structure and intensity distribution of the vortex harmonics exhibit significant dependence on the relative position between the gas jet and the laser focus.The ring-like structures observed in the vortex harmonics,and the interference of quantum paths provide an explanation for the distinct structural characteristics.Moreover,by adjusting the relative position between the jet and laser focus,it is possible to discern the contributions from different quantum paths.The optimization of the HH vortex field is applicable to the XUV,which opens up a new way for exploiting the potential in optical spin or manipulating electrons by using the photon with tunable orbital angular momentum.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
High harmonic generation in ZnO crystals under chirped single-color field and static electric field are investigated by solving the semiconductor Bloch equation(SBE). It is found that when the chirp pulse is introduce...High harmonic generation in ZnO crystals under chirped single-color field and static electric field are investigated by solving the semiconductor Bloch equation(SBE). It is found that when the chirp pulse is introduced, the interference structure becomes obvious while the harmonic cutoff is not extended. Furthermore, the harmonic efficiency is improved when the static electric field is included. These phenomena are demonstrated by the classical recollision model in real space affected by the waveform of laser field and inversion symmetry. Specifically, the electron motion in k-space shows that the change of waveform and the destruction of the symmetry of the laser field lead to the incomplete X-structure of the crystal-momentum-resolved(k-resolved) inter-band harmonic spectrum. Furthermore, a pre-acceleration process in the solid four-step model is confirmed.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
High-order harmonic generation(HHG) of Ar atom in an elliptically polarized intense laser field is experimentally investigated in this work.Interestingly,the anomalous ellipticity dependence on the laser ellipticity(...High-order harmonic generation(HHG) of Ar atom in an elliptically polarized intense laser field is experimentally investigated in this work.Interestingly,the anomalous ellipticity dependence on the laser ellipticity(ε) in the lower-order harmonics is observed,specifically in the 13rd-order,which displays a maximal harmonic intensity at ε ≈ 0.1,rather than at ε = 0 as expected.This contradicts the general trend of harmonic yield,which typically decreases with the increase of laser ellipticity.In this study,we attribute this phenomenon to the disruption of the symmetry of the wave function by the Coulomb effect,leading to the generation of a harmonic with high ellipticity.This finding provides valuable insights into the behavior of elliptically polarized harmonics and opens up a potential way for exploring new applications in ultrafast spectroscopy and light–matter interactions.展开更多
Efficient third-order nonlinearities of the Zinc Oxide and Al-doped Zinc Oxide were studied by Third Harmonic Generation (Third Harmonic Generation) Maker fringes to establish the effect Aluminum of Aluminum doping (A...Efficient third-order nonlinearities of the Zinc Oxide and Al-doped Zinc Oxide were studied by Third Harmonic Generation (Third Harmonic Generation) Maker fringes to establish the effect Aluminum of Aluminum doping (Al-doping) on the cubic nonlinearities. Adding the Al-dopant to the Zinc Oxide crystal structure results in changes that affect the optical and nonlinear characteristics. Presented results indicate that the magnitude of X<sup>(3)</sup> was enhanced at single experimental wavelengths;however, across the broadband experimental spectrum, the effect of Al-doping remained relatively constant. The observed enhancement of third-order nonlinearity was purely from the bound electronic response. The observation is attributed to increased charge carriers and spontaneous polarization in the Zinc Oxide and Al-doped Zinc Oxide crystal structure.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 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 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National Natural Science Foundation of China(Grant Nos.11674312,52174161,51702003,12174161 and 61775087)Anhui University of Science and Technology(Grant No.2023CX2141)。
文摘The third-harmonic generation(THG)coefficient for a spherical quantum dot system with inversely quadratic Hellmann plus inversely quadratic potential is investigated theoretically,considering the regulation of quantum size,confinement potential depth and the external environment.The numerical simulation results indicate that the THG coefficient can reach the order of 10~(-12)m~2V~(-2),which strongly relies on the tunable factor,with its resonant peak experiencing a redshift or blueshift.Interestingly,the effect of temperature on the THG coefficient in terms of peak location and size is consistent with the quantum dot radius but contrasts with the hydrostatic pressure.Thus,it is crucial to focus on the influence of internal and external parameters on nonlinear optical effects,and to implement the theory in practical experiments and the manufacture of optoelectronic devices.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11974137,92250306,and 12304302)the National Key Program for Science and Technology Research and Development(Grant No.2019YFA0307700)+1 种基金the Natural Science Foundation of Jilin Province,China(Grant Nos.YDZJ202101ZYTS157 and YDZJ202201ZYTS314)the Scientific Research Foundation of Jilin Provincial Education Department,China(Grant No.JJKH20230283KJ)。
文摘In high harmonic generation(HHG),Laguerre–Gaussian(LG) beams are used to generate extreme ultraviolet(XUV)vortices with well-defined orbital angular momentum(OAM),which have potential applications in fields such as microscopy and spectroscopy.An experimental study on the HHG driven by vortex and Gaussian beams is conducted in this work.It is found that the intensity of vortex harmonics is positively correlated with the laser energy and gas pressure.The structure and intensity distribution of the vortex harmonics exhibit significant dependence on the relative position between the gas jet and the laser focus.The ring-like structures observed in the vortex harmonics,and the interference of quantum paths provide an explanation for the distinct structural characteristics.Moreover,by adjusting the relative position between the jet and laser focus,it is possible to discern the contributions from different quantum paths.The optimization of the HH vortex field is applicable to the XUV,which opens up a new way for exploiting the potential in optical spin or manipulating electrons by using the photon with tunable orbital angular momentum.
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.
基金supported by the Natural Science Foundation of Jilin Province (Grant No.20220101010JC)the National Natural Science Foundation of China (Grant No.12074146)。
文摘High harmonic generation in ZnO crystals under chirped single-color field and static electric field are investigated by solving the semiconductor Bloch equation(SBE). It is found that when the chirp pulse is introduced, the interference structure becomes obvious while the harmonic cutoff is not extended. Furthermore, the harmonic efficiency is improved when the static electric field is included. These phenomena are demonstrated by the classical recollision model in real space affected by the waveform of laser field and inversion symmetry. Specifically, the electron motion in k-space shows that the change of waveform and the destruction of the symmetry of the laser field lead to the incomplete X-structure of the crystal-momentum-resolved(k-resolved) inter-band harmonic spectrum. Furthermore, a pre-acceleration process in the solid four-step model is confirmed.
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Project supported by the National Natural Science Foundation of China(Grant Nos.92250306,11974137,and 12304302)the National Key Program for Science and Technology Research and Development of China(Grant No.2019YFA0307700)+1 种基金the Natural Science Foundation of Jilin Province,China(Grant Nos.YDZJ202101ZYTS157 and YDZJ202201ZYTS314)the Scientific Research Foundation of the Education Department of Jilin Province,China(Grant No.JJKH20230283KJ)。
文摘High-order harmonic generation(HHG) of Ar atom in an elliptically polarized intense laser field is experimentally investigated in this work.Interestingly,the anomalous ellipticity dependence on the laser ellipticity(ε) in the lower-order harmonics is observed,specifically in the 13rd-order,which displays a maximal harmonic intensity at ε ≈ 0.1,rather than at ε = 0 as expected.This contradicts the general trend of harmonic yield,which typically decreases with the increase of laser ellipticity.In this study,we attribute this phenomenon to the disruption of the symmetry of the wave function by the Coulomb effect,leading to the generation of a harmonic with high ellipticity.This finding provides valuable insights into the behavior of elliptically polarized harmonics and opens up a potential way for exploring new applications in ultrafast spectroscopy and light–matter interactions.
文摘Efficient third-order nonlinearities of the Zinc Oxide and Al-doped Zinc Oxide were studied by Third Harmonic Generation (Third Harmonic Generation) Maker fringes to establish the effect Aluminum of Aluminum doping (Al-doping) on the cubic nonlinearities. Adding the Al-dopant to the Zinc Oxide crystal structure results in changes that affect the optical and nonlinear characteristics. Presented results indicate that the magnitude of X<sup>(3)</sup> was enhanced at single experimental wavelengths;however, across the broadband experimental spectrum, the effect of Al-doping remained relatively constant. The observed enhancement of third-order nonlinearity was purely from the bound electronic response. The observation is attributed to increased charge carriers and spontaneous polarization in the Zinc Oxide and Al-doped Zinc Oxide crystal structure.
