The study of nonlinear optical responses in the mid-infrared(mid-IR)regime is essential for advancing ultrafast mid-IR laser applications.However,nonlinear optical effects under mid-IR excitation are rarely reported d...The study of nonlinear optical responses in the mid-infrared(mid-IR)regime is essential for advancing ultrafast mid-IR laser applications.However,nonlinear optical effects under mid-IR excitation are rarely reported due to the lack of suitable nonlinear optical materials.The natural van derWaals heterostructure franckeite,known for its narrow bandgap and stability in air,shows great potential for developing mid-IR nonlinear optical devices.We have experimentally demonstrated that layered franckeite exhibits a broadband wavelength-dependent nonlinear optical response in the mid-IR spectral region.Franckeite nanosheets were prepared using a liquid-phase exfoliation method,and their nonlinear optical response was characterized in the spectral range of 3000 nm to 5000 nm.The franckeite nanosheets exhibit broadband wavelengthdependent third-order nonlinearities,with nonlinear absorption and refraction coefficients estimated to be about 10^(-7)cm/W and 10^(-11)cm^(2)/W,respectively.Additionally,a passively Q-switched fluoride fiber laser operating around a wavelength of 2800 nm was achieved,delivering nanosecond pulses with a signal-to-noise ratio of 43.6 dB,based on the nonlinear response of franckeite.These findings indicate that layered franckeite possesses broadband nonlinear optical characteristics in the mid-IR region,potentially enabling new possibilities for mid-IR photonic devices.展开更多
Ultrafast optical nonlinearities of N,N-dimethylformamide(DMF)are studied by using polarized light at 400 nm.Both nonlinear refraction(NLR)and stimulated Rayleigh-wing scattering(SRWS)depend on the polarization state ...Ultrafast optical nonlinearities of N,N-dimethylformamide(DMF)are studied by using polarized light at 400 nm.Both nonlinear refraction(NLR)and stimulated Rayleigh-wing scattering(SRWS)depend on the polarization state of incident beam,while two-photon absorption(TPA)changes negligibly with polarization state.The polarization dependence of SRWS originates from that of NLR via self-focusing effect.Third-order susceptibility elements of DMF were determined,and a method to distinguish the multi-photon absorption signal from SRWS in Z-scan is provided.These results are helpful for the nonlinear optical research of the novel materials dissolved in DMF.展开更多
Highly efficient nonlinear optical（NLO） materials with well-defined architectures in the wavelength and subwavelength length scales are of particular importance for next generation of integrated photonic circuits. F...Highly efficient nonlinear optical（NLO） materials with well-defined architectures in the wavelength and subwavelength length scales are of particular importance for next generation of integrated photonic circuits. Fluorenone analogues have been demonstrated to be promising candidates as building blocks for assembly of organic NLO materials thanks to their synergistic supramolecular interactions and brilliant optical properties. Here we have studied the polymorphs of a phenylethynyl functionalized fluorenone derivative, and their controlled self-assembly for microstructures with different morphologies. These polymorphic microcrystals exhibit very distinctive NLO properties, highly related to their supramolecular and electronic structures.展开更多
A series of alkali halide doped chalcohalide glasses （100-x）（0.9GeS2-0.1Sb2S3）-xCsCl （x=5, 10, 15 and 20 mole fraction） were prepared. The absorption spectra and Raman scatting spectra of these glasses were meas...A series of alkali halide doped chalcohalide glasses （100-x）（0.9GeS2-0.1Sb2S3）-xCsCl （x=5, 10, 15 and 20 mole fraction） were prepared. The absorption spectra and Raman scatting spectra of these glasses were measured. The optical band gaps Eopt were obtained from ultraviolet absorption edges. Z-scan technique was utilized to investigate the third-order nonlinear optical properties of GeS2-Sb2S3-CsCl glasses. The value of Eopt increases and the third-order optical nonlinearity decreases with increasing CsCl content. Decreasing lone-pair electron and broadening the band-gap will provide less transition paths for nonlinear process, which play a key role in ultrafast third-order nonlinear optical responses of these chalcohalide glasses.展开更多
The new tetracarbonyl - chromium-triphenyl phosphine complex was synthesized and characterized using ultraviolet（UV）-visible,Fourier transform infrared（FTIR）,and nuclear magnetic resonance（NMR） techniques.The ch...The new tetracarbonyl - chromium-triphenyl phosphine complex was synthesized and characterized using ultraviolet（UV）-visible,Fourier transform infrared（FTIR）,and nuclear magnetic resonance（NMR） techniques.The characterization results confirm the molecular structure of the new complex.The z-scan measurements were done by diode laser[continuous wave（CW）]to estimate the nonlinear optical parameter（X^3）.The results led to calculate three parameters：the groundstate cross sections（σ_g）,the excited-state cross sections（σ_（ex））,and thermo-optic coefficient of the new complex.This study indicated that our complex is a suitable for photonic applications.展开更多
The efficiency of nanoscale nonlinear elements in photonic integrated circuits is hindered by the physical limits to the nonlinear optical response of dielectrics,which cannot be engineered as it is a fundamental mate...The efficiency of nanoscale nonlinear elements in photonic integrated circuits is hindered by the physical limits to the nonlinear optical response of dielectrics,which cannot be engineered as it is a fundamental material property.Here,we experimentally demonstrate that ultrafast optical nonlinearities in doped semiconductors can be engineered and can easily exceed those of conventional undoped dielectrics.The electron response of heavily doped semiconductors acquires in fact a hydrodynamic character that introduces nonlocal effects as well as additional nonlinear sources.Our experimental findings are supported by a comprehensive computational analysis based on the hydrodynamic model.In particular,by studying third-harmonic generation from plasmonic nanoantenna arrays made out of heavily n-doped InGaAs with increasing levels of free-carrier density,we discriminate between hydrodynamic and dielectric nonlinearities.Most importantly,we demonstrate that the maximum nonlinear efficiency as well as its spectral location can be engineered by tuning the doping level.Crucially,the maximum efficiency can be increased by almost two orders of magnitude with respect to the classical dielectric nonlinearity.Having employed the common material platform InGaAs/InP that supports integrated waveguides,our findings pave the way for future exploitation of plasmonic nonlinearities in all-semiconductor photonic integrated circuits.展开更多
Herein,we report the synthesis and third-order nonlinear optical(NLO)properties of a novel cage-based 2D metal-organic framework constructed from Ti_(4)L_(6)(L4-=embonate)cage combined with Mg^(2+)and tris[4-(1H-imida...Herein,we report the synthesis and third-order nonlinear optical(NLO)properties of a novel cage-based 2D metal-organic framework constructed from Ti_(4)L_(6)(L4-=embonate)cage combined with Mg^(2+)and tris[4-(1H-imidazol-1-yl)phenyl]amine(tipa)ligand,whose molecular formula is(Me_(2)CH_(2))_(2)[Mg_(3)(Ti_(4)L_(6))(tipa)(H_(2)O)_(12)](PTC‑378).The Ti_(4)L_(6)tetrahedral cages serve as robust building units,while the Mg^(2+)ions and tipa ligands provide structural stability and tunable optical properties.The resulting PTC‑378 film exhibited intriguing third-order NLO property,which was systematically investigated using Z-scan techniques.Our results demonstrate that the synergistic interaction between Ti_(4)L_(6)cages andπ-conjugated ligands significantly enhances the NLO performance of the materials.CCDC:2453909.展开更多
Sulfates are always promising short-wave ultraviolet(UV)nonlinear optical(NLO)candidates,if their birefringence could be greatly improved.Here,in terms of the insufficient birefringence,the unity of heteroleptic tetra...Sulfates are always promising short-wave ultraviolet(UV)nonlinear optical(NLO)candidates,if their birefringence could be greatly improved.Here,in terms of the insufficient birefringence,the unity of heteroleptic tetrahedral groups and triangular ones was proposed and implemented.Thus,a new semiorganic crystal,[C(NH_(2))_(3)]S_(3)O_(6)(G_(2)S_(3)O_(6)),was obtained,which is composed of[S_(3)O_(6)]^(2-)and[C(NH_(2))_(3)]+groups.It exhibits excellent optical properties with a short absorption cutoff edge of 218 nm,a strong NLO response of 1.4×KH_(2)PO_(4),and more especially,a large birefringence of 0.097@546 nm.This birefringence leap makes the G_(2)S_(3)O_(6) crystal achieve a phase-matching behavior under a 532 nm laser.Thus,the synergy of[S_(3)O_(6)]^(2-)and[C(NH_(2))_(3)]~+groups results in excellent optical performances.This finding opens a new horizon for exploring novel UV NLO crystals.展开更多
Graphene oxide(GO)is a two-dimensional carbon material with a graphene-like structure and many oxygen-containing functional groups,and in recent years from research into the unique optical properties of GO,GO-based co...Graphene oxide(GO)is a two-dimensional carbon material with a graphene-like structure and many oxygen-containing functional groups,and in recent years from research into the unique optical properties of GO,GO-based composite materials formed by combining with other materials have shown improved overall performance.Reported here is an investigation of how doping with Ni,Fe,and Ag nanoparticles affects the linear and nonlinear optical properties of GO films.The morphology and structure of films of GO,GO with Ni nanoparticles,GO with Fe nanoparticles,and GO with Ag nanoparticles were studied by laser scanning confocal microscopy,SEM,energy dispersive spectroscopy,XRD,and Raman spectroscopy.UV-visible absorption spectra were used to study the optical absorption properties,and the optical band gaps of GO and the composites were calculated from those spectra via Tauc plots.The results show that the band gaps of GO films can be effectively regulated by metal nanoparticles,and so the properties of GO composites can be manipulated.The nonlinear optical properties of GO and GO-metal-nanoparticle composite films were studied by femtosecond laser Z-scanning.The results show that the femtosecond laser power can be tuned to the optical limiting behavior of GO.The strong synergistic coupling effect between metal nanoparticles and GO enhances the nonlinear absorption and nonlinear refraction of composite thin films.The nonlinear absorption coefficient of the composite thin films is improved significantly,and the optical limiting properties are excellent.GO-metal-nanoparticle composite materials have potential applications and advantages in improving optical absorption,band-gap control,and optical limiting.They can promote the expansion of GO composite materials in various practical applications and are candidates for good optical materials,opening the way to GO photonics.展开更多
The unique property of chirality is widely used in various fields.In the past few decades,a great deal of research has been conducted on the interactions between light and matter,resulting in significant technical adv...The unique property of chirality is widely used in various fields.In the past few decades,a great deal of research has been conducted on the interactions between light and matter,resulting in significant technical advancements in the precise manipulation of light field wavefronts.In this review,which focuses on current chiral optics research,we introduce the fundamental theory of chirality and highlight the latest achievements in enhancing chiral signals through artificial nano-manufacturing technology,with a particular focus on mechanisms such as light scattering and Mie resonance used to amplify chiral signals.By providing an overview of enhanced chiral signals,this review aims to provide researchers with an indepth understanding of chiral phenomena and its versatile applications in various domains.展开更多
We investigated nonlinear optical properties of ZnO-Nb2O5-TeO2 glass excited by a femtosecond laser with time-resolved four-wave mixing (FWM) technique. The unusual FWM signals were observed in samples with ZnO dopant...We investigated nonlinear optical properties of ZnO-Nb2O5-TeO2 glass excited by a femtosecond laser with time-resolved four-wave mixing (FWM) technique. The unusual FWM signals were observed in samples with ZnO dopant. The mechanism for the optical nonlinearities was discussed.展开更多
The third-order optical nonlinearities of dimethyl sulfoxide （DMSO） are investigated using the optical Kerr effect （OKE） and Z-scan techniques with femtosecond pulses. We are able to fit the OKE signal theoretical...The third-order optical nonlinearities of dimethyl sulfoxide （DMSO） are investigated using the optical Kerr effect （OKE） and Z-scan techniques with femtosecond pulses. We are able to fit the OKE signal theoretically by convolving the autocorrelation of the incident pulse intensity profile with the impulse responses of the samples, illustrating the instantaneous nonlinear response of DMSO. We verify that the purely electronic cloud distortion causes the observed signal for DMSO. The Z-scan technique is used to estimate the third-order susceptibility of DMSO, which is about a quarter of that for CS2 and mainly comes from the nonlinear refraction with an intensity of less than 140 GW/cm^2.展开更多
The design of pnictide nonlinear optical crystals is quite different from chalcogenide and oxide those in which a new paradigm need be developed to regulate the band gap,one of key optical parameters In this work,two ...The design of pnictide nonlinear optical crystals is quite different from chalcogenide and oxide those in which a new paradigm need be developed to regulate the band gap,one of key optical parameters In this work,two non-centrosymmetric halidepnictides,[Cd_(2)P]_(2)[CdBr_(4)](CPB)and[Cd_(2)As]_(2)[CdBr_(4)](CAB) were reported.The complete octet binding electrons of pnictogens were constructed by four Cd-P pola covalent bonds under the anchoring effect of halogens,creating an extremely flat valence band maximum with band dispersion of only 0.17 eV.As expected,the balance of the covalency and ionicity in CPB and CAB was successfully realized,leading to a wide band gap of 2.58 eV and 1.88 eV.Remarkably,CPB no only has a widest band gap among Cd-containing pnictides,but also exhibits a SHG effect of 1.2×AgGaS_(2).moderate birefringence(0.088@visible light and calcd.0.043@2050 nm)and a wide IR transmission range.This is the first time that the octet binding electrons construction strategy was utilized to design non diamond like NLO pnictides with excellent performances.展开更多
We present the measurement of the third-order nonlinearity of Bi203-B^O3-BaO glasses using the single Z-scan method with femtosecond laser pulses at 750 - 850 nm. Both third-order nonlinear refraction γ and two photo...We present the measurement of the third-order nonlinearity of Bi203-B^O3-BaO glasses using the single Z-scan method with femtosecond laser pulses at 750 - 850 nm. Both third-order nonlinear refraction γ and two photon absorption coefficient β are investigated. The γ shows an increasing tendency with increasing BaO content, and the largest value is estimated to be 7.2×10^-14 cm^2/W, which is as large as those of chalcogenide glasses. The dependence of 13 on the normalized photon energy is studied.展开更多
Functional materials with multiple properties are urgent to be explored to reach high requirements for applications nowadays.In this work,a new multifunctional one-dimensional(1D)chain compound[N(C_(3)H_(7))_(4)][Cu(o...Functional materials with multiple properties are urgent to be explored to reach high requirements for applications nowadays.In this work,a new multifunctional one-dimensional(1D)chain compound[N(C_(3)H_(7))_(4)][Cu(ohpma)]·H_(2)O 1(ohpma=deprotonated N-(2-hydoxyphenyl)oxamic acid)exhibiting both 1D antiferromagnetic and nonlinear optical properties,which are both originated from the same polar[Cu(C_(8)H_(4)NO_(4))]magnetic units,has been successfully synthesized by evaporation at room temperature.Bis-polydentate nature of the(ohpma)3−ligand with constrained tridentate and bidentate coordination sites conducts Cu^(2+)ions coordinating in different geometries and forms 1D chains along the c axis,which are further separated by the[N(C_(3)H_(7))_(4)]+cations.And the 1D magnetic chains further exhibit noncentrosymmetric polar arrangement.Nonlinear optical study shows polar compound 1 exhibits a discernible second-harmonic generation(SHG)efficiency and the calculation of the partial density of states indicates that the SHG efficiency of 1 is mainly originated from the polar[Cu(C_(8)H_(4)NO_(4))]magnetic units.Moreover,magnetic susceptibility shows a broad maximum around 70 K with strong intrachain interaction of J/k B=−113.0 K but no long-range order is observed down to 2 K,suggesting that 1 shows a good 1D magnetism.Both good 1D magnetism and SHG activity suggest that 1 could be as a potential multifunctional material,particularly.展开更多
The ultrashort lasers working in pulse-burst mode reveal great machining performance in recent years. The number of pulses in bursts effects greatly on the removal rate and roughness. To generate a more equal amplitud...The ultrashort lasers working in pulse-burst mode reveal great machining performance in recent years. The number of pulses in bursts effects greatly on the removal rate and roughness. To generate a more equal amplitude of pulses in burst with linear polarization output and time gap adjustable, we propose a new method by the harmonic beam combining(HBC).The beam combining is commonly used in adding pulses into the output beam while maintaining the pulse waveform and beam quality. In the HBC, dichroic mirrors are used to combine laser pulses of fundamental wave(FW) into harmonic wave(HW), and nonlinear crystals are used to convert the FW into HW. Therefore, HBC can add arbitrarily more HW pulses to generate pulse-burst in linear polarization with simple structure. The amplitude of each pulse in bursts can be adjusted the same to increase the stability of the burst, the time gap of each pulse can be adjusted precisely by proper time delay. Because HBC adds pulses sequentially, the peak power density of the burst is the same as each pulse, pulses can be combined without concern of back-conversion which often occurs in high peak power density. In the demonstration, the extendibility of HBC was verified by combining two beams with a third beam. The combined efficiency rates were larger than 99%, and the beam quality of each beam was maintained at M^(2)≈1.4.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
It is challenging to cooperatively improve the nonlinear optical(NLO)efficiency and the laser-induced damage threshold(LIDT).This work reports a novel IR NLO materials CsInP_(2)S_(7)(CIPS)designed by combination the s...It is challenging to cooperatively improve the nonlinear optical(NLO)efficiency and the laser-induced damage threshold(LIDT).This work reports a novel IR NLO materials CsInP_(2)S_(7)(CIPS)designed by combination the strategies of alkali metals substitution and microscopic NLO units PS4 introduction based on AgGaS_(2).CIPS was composed of strongly distorted[InS_(6)]^(9-)octahedra and[P_(2)S_(7)]4-dimers constructed by corner-sharing[PS_(4)]^(3-),which increase the NLO efficiency and decrease thermal expansion anisotropy simultaneously.Compared with AgGaS_(2),CIPS exhibited strong phase matchable NLO response ca.1.1×AGS@2.1μm,high LIDT ca.20.8×AgGaS_(2),and IR transparency up to 15.3μm.Structural analysis and theoretical investigation confirmed that large SHG effect and ultrahigh LIDT of CIPS originated from the synergistic contribution of[InS_(6)]^(9-)octahedra and[P_(2)S_(7)]4-dimers.These results indicate that CIPS is a promising NLO candidate in the mid-IR region,and this study provides a new approach for developing potential NLO-LIDT compatible materials.展开更多
Cyclo[18]carbon has received considerable attention thanks to its novel geometric configuration and special electronic structure.Superalkalis have low ionization energy.Doping a superalkali in cyclo[18]carbon is an ef...Cyclo[18]carbon has received considerable attention thanks to its novel geometric configuration and special electronic structure.Superalkalis have low ionization energy.Doping a superalkali in cyclo[18]carbon is an effective method to improve the optical properties of the system because considerable electron transfer occurs.In this paper,the geometry,bonding properties,electronic structure,absorption spectrum,and nonlinear optical(NLO)properties of superalkaline M_(3)O(M=Li,Na)-doped cyclo[18]carbon were studied by using density functional theory.M_(3)O and the C_(18) rings are not coplanar.The C_(18) ring still exhibits alternating long and short bonds.The charge transfer between M_(3)O and C_(18) forms stable[M_(3)O]+[C_(18)]-ionic complexes.C_(18)M_(3)O(M=Li,Na)shows striking optical nonlinearity,i.e.,their first-and second-order hyperpolarizability(βvec andγ||)increase considerably atλ=1907 nm and 1460 nm.展开更多
A Weyl node is characterized by its chirality and tilt.We develop a theory of how nth-order nonlinear optical conductivity behaves under transformations of anisotropic tensor and tilt, which clarifies how chirality-de...A Weyl node is characterized by its chirality and tilt.We develop a theory of how nth-order nonlinear optical conductivity behaves under transformations of anisotropic tensor and tilt, which clarifies how chirality-dependent and-independent parts of optical conductivity transform under the reversal of tilt and chirality.Built on this theory, we propose ferromagnetic Mn Bi2Te4as a magnetoelectrically regulated, terahertz optical device, by magnetoelectrically switching the chiralitydependent and-independent DC photocurrents.These results are useful for creating nonlinear optical devices based on the topological Weyl semimetals.展开更多
基金supported by the National Natural Science Foundation of China(Grant No.61975055)the Natural Science Foundation of Hunan Province,China(Grant No.2023JJ30165)+1 种基金the Natural Science Foundation of Shandong Province,China(Grant No.ZR2022QF005)the Doctoral Fund of University of Heze(Grant No.XY22BS14).
文摘The study of nonlinear optical responses in the mid-infrared(mid-IR)regime is essential for advancing ultrafast mid-IR laser applications.However,nonlinear optical effects under mid-IR excitation are rarely reported due to the lack of suitable nonlinear optical materials.The natural van derWaals heterostructure franckeite,known for its narrow bandgap and stability in air,shows great potential for developing mid-IR nonlinear optical devices.We have experimentally demonstrated that layered franckeite exhibits a broadband wavelength-dependent nonlinear optical response in the mid-IR spectral region.Franckeite nanosheets were prepared using a liquid-phase exfoliation method,and their nonlinear optical response was characterized in the spectral range of 3000 nm to 5000 nm.The franckeite nanosheets exhibit broadband wavelengthdependent third-order nonlinearities,with nonlinear absorption and refraction coefficients estimated to be about 10^(-7)cm/W and 10^(-11)cm^(2)/W,respectively.Additionally,a passively Q-switched fluoride fiber laser operating around a wavelength of 2800 nm was achieved,delivering nanosecond pulses with a signal-to-noise ratio of 43.6 dB,based on the nonlinear response of franckeite.These findings indicate that layered franckeite possesses broadband nonlinear optical characteristics in the mid-IR region,potentially enabling new possibilities for mid-IR photonic devices.
基金the National Natural Science Foundation of China(No.12074202)the Natural Science Foundation of Tianjin City(Nos.22JCYBJC00390 and 20JCQNJC00020)。
文摘Ultrafast optical nonlinearities of N,N-dimethylformamide(DMF)are studied by using polarized light at 400 nm.Both nonlinear refraction(NLR)and stimulated Rayleigh-wing scattering(SRWS)depend on the polarization state of incident beam,while two-photon absorption(TPA)changes negligibly with polarization state.The polarization dependence of SRWS originates from that of NLR via self-focusing effect.Third-order susceptibility elements of DMF were determined,and a method to distinguish the multi-photon absorption signal from SRWS in Z-scan is provided.These results are helpful for the nonlinear optical research of the novel materials dissolved in DMF.
基金the financial supports from the National Natural Science Foundation of China(NSFC) (Nos.21773168, 51503143 and 21761132007)the Tianjin Natural Science Foundation(No. 16JCQNJC05000)+5 种基金the Innovation Foundation of Tianjin University (No. 2016XRX-0017)the China International Science and Technology Projects(No. S2016G3413)The Netherlands Organization for Scientific Research (NWO) with the Veni Grant (No. 680-47-437)The Royal Netherlands Academy of Arts and Sciences(KNAW) with the China-Exchange Program (No. 530-4CDPO2)the Tianjin 1000 Youth Talents Planthe Chinese Scholarship Council (CSC)
文摘Highly efficient nonlinear optical（NLO） materials with well-defined architectures in the wavelength and subwavelength length scales are of particular importance for next generation of integrated photonic circuits. Fluorenone analogues have been demonstrated to be promising candidates as building blocks for assembly of organic NLO materials thanks to their synergistic supramolecular interactions and brilliant optical properties. Here we have studied the polymorphs of a phenylethynyl functionalized fluorenone derivative, and their controlled self-assembly for microstructures with different morphologies. These polymorphic microcrystals exhibit very distinctive NLO properties, highly related to their supramolecular and electronic structures.
基金supported by the National Ba-sic Research Program of China ("973 Project", (No2006CB708607)the Science and Technology Department of Zhejiang Province, China (No 2006C11127)+1 种基金the Science and Technology Foundation of Ningbo, China (No2006B100068)the Natural Science Foundation of Ningbo, China (Nos 2006A610056, 2007A610004)
文摘A series of alkali halide doped chalcohalide glasses （100-x）（0.9GeS2-0.1Sb2S3）-xCsCl （x=5, 10, 15 and 20 mole fraction） were prepared. The absorption spectra and Raman scatting spectra of these glasses were measured. The optical band gaps Eopt were obtained from ultraviolet absorption edges. Z-scan technique was utilized to investigate the third-order nonlinear optical properties of GeS2-Sb2S3-CsCl glasses. The value of Eopt increases and the third-order optical nonlinearity decreases with increasing CsCl content. Decreasing lone-pair electron and broadening the band-gap will provide less transition paths for nonlinear process, which play a key role in ultrafast third-order nonlinear optical responses of these chalcohalide glasses.
文摘The new tetracarbonyl - chromium-triphenyl phosphine complex was synthesized and characterized using ultraviolet（UV）-visible,Fourier transform infrared（FTIR）,and nuclear magnetic resonance（NMR） techniques.The characterization results confirm the molecular structure of the new complex.The z-scan measurements were done by diode laser[continuous wave（CW）]to estimate the nonlinear optical parameter（X^3）.The results led to calculate three parameters：the groundstate cross sections（σ_g）,the excited-state cross sections（σ_（ex））,and thermo-optic coefficient of the new complex.This study indicated that our complex is a suitable for photonic applications.
文摘The efficiency of nanoscale nonlinear elements in photonic integrated circuits is hindered by the physical limits to the nonlinear optical response of dielectrics,which cannot be engineered as it is a fundamental material property.Here,we experimentally demonstrate that ultrafast optical nonlinearities in doped semiconductors can be engineered and can easily exceed those of conventional undoped dielectrics.The electron response of heavily doped semiconductors acquires in fact a hydrodynamic character that introduces nonlocal effects as well as additional nonlinear sources.Our experimental findings are supported by a comprehensive computational analysis based on the hydrodynamic model.In particular,by studying third-harmonic generation from plasmonic nanoantenna arrays made out of heavily n-doped InGaAs with increasing levels of free-carrier density,we discriminate between hydrodynamic and dielectric nonlinearities.Most importantly,we demonstrate that the maximum nonlinear efficiency as well as its spectral location can be engineered by tuning the doping level.Crucially,the maximum efficiency can be increased by almost two orders of magnitude with respect to the classical dielectric nonlinearity.Having employed the common material platform InGaAs/InP that supports integrated waveguides,our findings pave the way for future exploitation of plasmonic nonlinearities in all-semiconductor photonic integrated circuits.
文摘Herein,we report the synthesis and third-order nonlinear optical(NLO)properties of a novel cage-based 2D metal-organic framework constructed from Ti_(4)L_(6)(L4-=embonate)cage combined with Mg^(2+)and tris[4-(1H-imidazol-1-yl)phenyl]amine(tipa)ligand,whose molecular formula is(Me_(2)CH_(2))_(2)[Mg_(3)(Ti_(4)L_(6))(tipa)(H_(2)O)_(12)](PTC‑378).The Ti_(4)L_(6)tetrahedral cages serve as robust building units,while the Mg^(2+)ions and tipa ligands provide structural stability and tunable optical properties.The resulting PTC‑378 film exhibited intriguing third-order NLO property,which was systematically investigated using Z-scan techniques.Our results demonstrate that the synergistic interaction between Ti_(4)L_(6)cages andπ-conjugated ligands significantly enhances the NLO performance of the materials.CCDC:2453909.
基金supported by the National Natural Science Foundation of China(Nos.52172009 and 12275274)the Science and Technology Project of Fujian Province(Nos.2021J01519 and 2021H0043)the Instrument Developing Project of Chinese Academy of Sciences(No.YJKYYQ20210033)。
文摘Sulfates are always promising short-wave ultraviolet(UV)nonlinear optical(NLO)candidates,if their birefringence could be greatly improved.Here,in terms of the insufficient birefringence,the unity of heteroleptic tetrahedral groups and triangular ones was proposed and implemented.Thus,a new semiorganic crystal,[C(NH_(2))_(3)]S_(3)O_(6)(G_(2)S_(3)O_(6)),was obtained,which is composed of[S_(3)O_(6)]^(2-)and[C(NH_(2))_(3)]+groups.It exhibits excellent optical properties with a short absorption cutoff edge of 218 nm,a strong NLO response of 1.4×KH_(2)PO_(4),and more especially,a large birefringence of 0.097@546 nm.This birefringence leap makes the G_(2)S_(3)O_(6) crystal achieve a phase-matching behavior under a 532 nm laser.Thus,the synergy of[S_(3)O_(6)]^(2-)and[C(NH_(2))_(3)]~+groups results in excellent optical performances.This finding opens a new horizon for exploring novel UV NLO crystals.
基金funded by the Henan Key Laboratory of Intelligent Manufacturing Equipment Integration for Superhard Materials(Grant No.JDKJ2022-01)the Key Lab of Modern Optical Technologies of Education Ministry of China,Soochow University。
文摘Graphene oxide(GO)is a two-dimensional carbon material with a graphene-like structure and many oxygen-containing functional groups,and in recent years from research into the unique optical properties of GO,GO-based composite materials formed by combining with other materials have shown improved overall performance.Reported here is an investigation of how doping with Ni,Fe,and Ag nanoparticles affects the linear and nonlinear optical properties of GO films.The morphology and structure of films of GO,GO with Ni nanoparticles,GO with Fe nanoparticles,and GO with Ag nanoparticles were studied by laser scanning confocal microscopy,SEM,energy dispersive spectroscopy,XRD,and Raman spectroscopy.UV-visible absorption spectra were used to study the optical absorption properties,and the optical band gaps of GO and the composites were calculated from those spectra via Tauc plots.The results show that the band gaps of GO films can be effectively regulated by metal nanoparticles,and so the properties of GO composites can be manipulated.The nonlinear optical properties of GO and GO-metal-nanoparticle composite films were studied by femtosecond laser Z-scanning.The results show that the femtosecond laser power can be tuned to the optical limiting behavior of GO.The strong synergistic coupling effect between metal nanoparticles and GO enhances the nonlinear absorption and nonlinear refraction of composite thin films.The nonlinear absorption coefficient of the composite thin films is improved significantly,and the optical limiting properties are excellent.GO-metal-nanoparticle composite materials have potential applications and advantages in improving optical absorption,band-gap control,and optical limiting.They can promote the expansion of GO composite materials in various practical applications and are candidates for good optical materials,opening the way to GO photonics.
基金funded by the National Natural Science Foundation of China(62005168,62075132,and 92050202)the Natural Science Foundation of Shanghai(22ZR1443100).
文摘The unique property of chirality is widely used in various fields.In the past few decades,a great deal of research has been conducted on the interactions between light and matter,resulting in significant technical advancements in the precise manipulation of light field wavefronts.In this review,which focuses on current chiral optics research,we introduce the fundamental theory of chirality and highlight the latest achievements in enhancing chiral signals through artificial nano-manufacturing technology,with a particular focus on mechanisms such as light scattering and Mie resonance used to amplify chiral signals.By providing an overview of enhanced chiral signals,this review aims to provide researchers with an indepth understanding of chiral phenomena and its versatile applications in various domains.
基金This work was supported by Shanghai Priority Academic DisciPline,National Natural Science Foundation (No.10234030),National Key project for Basic Research (No.1999075200),the Key Project sponsored by National Education Ministry of China and the PhosP
文摘We investigated nonlinear optical properties of ZnO-Nb2O5-TeO2 glass excited by a femtosecond laser with time-resolved four-wave mixing (FWM) technique. The unusual FWM signals were observed in samples with ZnO dopant. The mechanism for the optical nonlinearities was discussed.
基金supported by the Heilongjiang Province Science Foundation(No.F201032)the High-Level Professionals and Innovative Teams of Heilongjiang University(No.Hdtd2010-15)the Science and Technique Research Project of the Department of Education of Heilongjiang Province(No.12521423)
文摘The third-order optical nonlinearities of dimethyl sulfoxide （DMSO） are investigated using the optical Kerr effect （OKE） and Z-scan techniques with femtosecond pulses. We are able to fit the OKE signal theoretically by convolving the autocorrelation of the incident pulse intensity profile with the impulse responses of the samples, illustrating the instantaneous nonlinear response of DMSO. We verify that the purely electronic cloud distortion causes the observed signal for DMSO. The Z-scan technique is used to estimate the third-order susceptibility of DMSO, which is about a quarter of that for CS2 and mainly comes from the nonlinear refraction with an intensity of less than 140 GW/cm^2.
基金supported by the National Natural Science Foundation of China(Nos.22305174,22375147,52332001,51890862,51902308 and 21921001)the Natural Science Foundation of Fujian Province(No.2021J05097)the Natural Science Foundation of Tianjin City(No.22JCYBJC01380)。
文摘The design of pnictide nonlinear optical crystals is quite different from chalcogenide and oxide those in which a new paradigm need be developed to regulate the band gap,one of key optical parameters In this work,two non-centrosymmetric halidepnictides,[Cd_(2)P]_(2)[CdBr_(4)](CPB)and[Cd_(2)As]_(2)[CdBr_(4)](CAB) were reported.The complete octet binding electrons of pnictogens were constructed by four Cd-P pola covalent bonds under the anchoring effect of halogens,creating an extremely flat valence band maximum with band dispersion of only 0.17 eV.As expected,the balance of the covalency and ionicity in CPB and CAB was successfully realized,leading to a wide band gap of 2.58 eV and 1.88 eV.Remarkably,CPB no only has a widest band gap among Cd-containing pnictides,but also exhibits a SHG effect of 1.2×AgGaS_(2).moderate birefringence(0.088@visible light and calcd.0.043@2050 nm)and a wide IR transmission range.This is the first time that the octet binding electrons construction strategy was utilized to design non diamond like NLO pnictides with excellent performances.
基金supported by the National Natural Science Foundation of China(Nos.60978058,60908032, and 60972064)the Natural Science Foundation of Zhejiang Province(No.Y1090996)the Scientific Research Foundation of Graduate School of Ningbo University, and the K.C.Wong Magna Fund in Ningbo University
文摘We present the measurement of the third-order nonlinearity of Bi203-B^O3-BaO glasses using the single Z-scan method with femtosecond laser pulses at 750 - 850 nm. Both third-order nonlinear refraction γ and two photon absorption coefficient β are investigated. The γ shows an increasing tendency with increasing BaO content, and the largest value is estimated to be 7.2×10^-14 cm^2/W, which is as large as those of chalcogenide glasses. The dependence of 13 on the normalized photon energy is studied.
基金supported by the National Natural Science Foundation of China(NSFC,No.22101091)the Fundamental Research Funds for the Central Universities(No.2019kfyXKJC016)the Innovation and Talent Recruitment Base of New Energy Chemistry and Device(No.B210003),Knowledge Innovation Program of Wuhan-Basic Research.
文摘Functional materials with multiple properties are urgent to be explored to reach high requirements for applications nowadays.In this work,a new multifunctional one-dimensional(1D)chain compound[N(C_(3)H_(7))_(4)][Cu(ohpma)]·H_(2)O 1(ohpma=deprotonated N-(2-hydoxyphenyl)oxamic acid)exhibiting both 1D antiferromagnetic and nonlinear optical properties,which are both originated from the same polar[Cu(C_(8)H_(4)NO_(4))]magnetic units,has been successfully synthesized by evaporation at room temperature.Bis-polydentate nature of the(ohpma)3−ligand with constrained tridentate and bidentate coordination sites conducts Cu^(2+)ions coordinating in different geometries and forms 1D chains along the c axis,which are further separated by the[N(C_(3)H_(7))_(4)]+cations.And the 1D magnetic chains further exhibit noncentrosymmetric polar arrangement.Nonlinear optical study shows polar compound 1 exhibits a discernible second-harmonic generation(SHG)efficiency and the calculation of the partial density of states indicates that the SHG efficiency of 1 is mainly originated from the polar[Cu(C_(8)H_(4)NO_(4))]magnetic units.Moreover,magnetic susceptibility shows a broad maximum around 70 K with strong intrachain interaction of J/k B=−113.0 K but no long-range order is observed down to 2 K,suggesting that 1 shows a good 1D magnetism.Both good 1D magnetism and SHG activity suggest that 1 could be as a potential multifunctional material,particularly.
基金Project supported by Youth Innovation Promotion Association of the Chinese Academy of Sciences (Grant No.2020029)。
文摘The ultrashort lasers working in pulse-burst mode reveal great machining performance in recent years. The number of pulses in bursts effects greatly on the removal rate and roughness. To generate a more equal amplitude of pulses in burst with linear polarization output and time gap adjustable, we propose a new method by the harmonic beam combining(HBC).The beam combining is commonly used in adding pulses into the output beam while maintaining the pulse waveform and beam quality. In the HBC, dichroic mirrors are used to combine laser pulses of fundamental wave(FW) into harmonic wave(HW), and nonlinear crystals are used to convert the FW into HW. Therefore, HBC can add arbitrarily more HW pulses to generate pulse-burst in linear polarization with simple structure. The amplitude of each pulse in bursts can be adjusted the same to increase the stability of the burst, the time gap of each pulse can be adjusted precisely by proper time delay. Because HBC adds pulses sequentially, the peak power density of the burst is the same as each pulse, pulses can be combined without concern of back-conversion which often occurs in high peak power density. In the demonstration, the extendibility of HBC was verified by combining two beams with a third beam. The combined efficiency rates were larger than 99%, and the beam quality of each beam was maintained at M^(2)≈1.4.
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the Natural Science Foundation of China(No.22105218).
文摘It is challenging to cooperatively improve the nonlinear optical(NLO)efficiency and the laser-induced damage threshold(LIDT).This work reports a novel IR NLO materials CsInP_(2)S_(7)(CIPS)designed by combination the strategies of alkali metals substitution and microscopic NLO units PS4 introduction based on AgGaS_(2).CIPS was composed of strongly distorted[InS_(6)]^(9-)octahedra and[P_(2)S_(7)]4-dimers constructed by corner-sharing[PS_(4)]^(3-),which increase the NLO efficiency and decrease thermal expansion anisotropy simultaneously.Compared with AgGaS_(2),CIPS exhibited strong phase matchable NLO response ca.1.1×AGS@2.1μm,high LIDT ca.20.8×AgGaS_(2),and IR transparency up to 15.3μm.Structural analysis and theoretical investigation confirmed that large SHG effect and ultrahigh LIDT of CIPS originated from the synergistic contribution of[InS_(6)]^(9-)octahedra and[P_(2)S_(7)]4-dimers.These results indicate that CIPS is a promising NLO candidate in the mid-IR region,and this study provides a new approach for developing potential NLO-LIDT compatible materials.
基金Project supported by the Natural Science Foundation of Anhui Province(Grant No.1908085MA12)the National Natural Science Foundation of China(Grant No.21703222)。
文摘Cyclo[18]carbon has received considerable attention thanks to its novel geometric configuration and special electronic structure.Superalkalis have low ionization energy.Doping a superalkali in cyclo[18]carbon is an effective method to improve the optical properties of the system because considerable electron transfer occurs.In this paper,the geometry,bonding properties,electronic structure,absorption spectrum,and nonlinear optical(NLO)properties of superalkaline M_(3)O(M=Li,Na)-doped cyclo[18]carbon were studied by using density functional theory.M_(3)O and the C_(18) rings are not coplanar.The C_(18) ring still exhibits alternating long and short bonds.The charge transfer between M_(3)O and C_(18) forms stable[M_(3)O]+[C_(18)]-ionic complexes.C_(18)M_(3)O(M=Li,Na)shows striking optical nonlinearity,i.e.,their first-and second-order hyperpolarizability(βvec andγ||)increase considerably atλ=1907 nm and 1460 nm.
基金Project supported by the National Key R&D Program of China (Grant Nos.2018YFA, 0305601, and 2021YFA1400100)the National Natural Science Foundation of China (Grant Nos.12274003, 11725415, and 11934001)the Innovation Program for Quantum Science and Technology (Grant No.2021ZD0302600)。
文摘A Weyl node is characterized by its chirality and tilt.We develop a theory of how nth-order nonlinear optical conductivity behaves under transformations of anisotropic tensor and tilt, which clarifies how chirality-dependent and-independent parts of optical conductivity transform under the reversal of tilt and chirality.Built on this theory, we propose ferromagnetic Mn Bi2Te4as a magnetoelectrically regulated, terahertz optical device, by magnetoelectrically switching the chiralitydependent and-independent DC photocurrents.These results are useful for creating nonlinear optical devices based on the topological Weyl semimetals.
