Broadband third-order optical nonlinearities of layered franckeite towards mid-infrared regime

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.

Optical nonlinearities of tetracarbonyl-chromium triphenyl phosphine complex

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.

Study on optical nonlinearities of ZnO-Nb_2O_5-TeO_2 glass with time-resolved four-wave mixing technique

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.

Polarization-dependent ultrafast optical nonlinearities of N,N-dimethylformamide at 400 nm

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.

Ultrafast third-order optical nonlinearities in DMSO

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.

Strong optical nonlinearities of self-assembled polymorphic microstructures of phenylethynyl functionalized fluorenones

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.

CsCl Effected Ultrafast Third-order Optical Nonlinearities of GeS_2-Sb_2S_3 Chalcogenide Glasses

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.

Femtosecond measurement of third-order optical nonlinearities in Bi_2O_3-B_2O_3-BaO glasses

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.

Third-order Optical Nonlinearities of a Series of Compounds Derived from a Keplerate Type Molybdenum-oxide-based Polyoxometalate

Abstract By reacting the unique Keplerate type molybdenum-oxide based polyoxometalate （NH4）42·[MoI320372·（CH3COO）30（H2O）y2]·ca.300H2·ca. 10CH3COONH4（1） with tetramethylammonium bromide, a new derivative （NH4）26[TMA]16{MoI32O372（H2O）72（CH3COO）30}·ca.7NH4CH3COO·ca.189H2O（2, TMA=tetramethylammonium） was prepared. Compound 2 was characterized by Fourier transform infrared spectroscopy（FTIR）, UV-Vis, elemental and thermogravimetric analyses. By the well-established Z-scan technique, investigations on the nonlinear opti- cal（NLO） properties of the series of compounds derived from the Keplerate type molybdenum-oxide-based poly- oxometalate, namely, the newly prepared compound 2, the three previously reported compounds, included compound 1, （NH4hs（TBA）24{Mo132O372（H2O）72（CH3COO）30}·ca.7NH4CH3COO·ca. 173H2O（3, TBA=tetrabutylammonium） and （DODA）40（NH4）2[（H2O）nMo132O372（CH3COO）3o（H20）72]（4, DODA=dimethyldioctadecylammonium）, reveal that the third-order nonlinearity[x（3）] values of compounds 1, 2 and 3 in the DMF/H2O solution and compound 4 in chloro- form are almost the same, which indicates that the counter cations with different length of alkyl chains show ignora- ble impacts on the NLO susceptibility. In other words, the remarkable third-order nonlinearities[x（3）≈10 19 m2/V2] mainly come from the [MoI32O372（CH3COO）30（H2O）72]42 anions. This fact reveals that the applications of the NLO active polyoxometalates in various environments（such as hydrophilic, hydrophobic, polar, apolar, etc.） can be achieved by simply varying cations to meet the demands in the design of diverse devices. Keywords Keplerate type polyoxometalate; Nonlinear optical property; Z-Scan technique; Self-defocusing; Reverse saturable absorption

Using harmonic beam combining to generate pulse-burst in nonlinear optical laser

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.

Structure,electronic,and nonlinear optical properties of superalkaline M_(3)O(M=Li,Na)doped cyclo[18]carbon

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.

Symmetry transformation of nonlinear optical current of tilted Weyl nodes and application to ferromagnetic MnBi_(2)Te_(4)

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.

Electrical and nonlinear optical properties of TGZO transparent conducting films deposited by magnetron sputtering

Thin transparent oxide conducting films(TCOFs)of titanium and gallium substituted zinc oxide(TGZO)were fabricated via radio frequency(RF)magnetron sputtering technique.The effects of RF power on electrical,linear and nonlinear optical characteristics were investigated by Hall tester,Ultraviolet(UV)-visible spectrophotometer and optical characterization method.The results indicate that RF power significantly influences the electrical and optical properties of the deposited films.As RF power raises,the resistivity and Urbach energy fall initially and then rise,while the figure of merit,mean visible transmittance and optical bandgap show the reverse variation trend.At RF power of 190 W,the TGZO sample exhibits the highest electro-optical properties,with the maximum figure of merit(1.14×10^(4)Ω^(-1)∙cm^(-1)),mean visible transmittance(86.9%)and optical bandgap(3.50 eV),the minimum resistivity(6.26×10^(-4)Ω∙cm)and Urbach energy(174.23 meV).In addition,the optical constants of the deposited films were determined by the optical spectrum fitting method,and the RF power dependence of nonlinear optical properties was studied.It is observed that all the thin films exhibit normal dispersion characteristics in the visible region,and the nonlinear optical parameters are greatly affected by the RF power in the ultraviolet region.

Microstructure and Nonlinear Optical Properties of Very Small Size GaAs Nanogranulae Embedded in SiO_2 Matrix by Magnetron Co-Sputtering

Microstructure of GaAs/SiO 2 nanogranular thin films fabricated by radio frequency magnetron co sputtering technique and postannealing are investigated via atomic force microscope,X ray diffraction,and Rutherford backscattering spectroscopy.The results show that GaAs nanocrystals with average diameters from 1 5nm to 3 2nm (depending on the annealing temperature) are uniformly dispersed in the SiO 2 matrices.GaAs and SiO 2 are found in normal stoichiometry in the films.The nonlinear optical refraction and nonlinear optical absorption are studied by Z scan technique using a single Gaussian beam of pulse laser.The third order nonlinear optical refractive index and nonlinear absorption coefficient are enhanced due to the quantum confinement effects and estimated to be 4×10 -12 m 2/W and 2×10 -5 m/W respectively in nonresonant condition,while 2×10 -11 m 2/W and -1×10 -4 m/W respectively in quasi resonant condition.

SYNTHESIS AND CHARAOTERIZATION OF NOVEL THERMOTROPIO LIQUID ORYSTALLINE POLYESTERS BEARING NONLINEAR OPTICAL AZOBENZENE SIDE GROUP

A series of novel thermotropic liquid crystalline polyesters bearing nonlinear optical azobenzene side group were synthesized by high temperature solution polycondensation and their structures,thermal stability, phase transition behavior and crystallinity were characterized by IR,elemental analysis, TG-DTA, polarizing optical microscope (POM) equipped with a hot stage and X-ray diffraction techniques. The results demonstrate that all the synthesized polyesters exhibit nematic liquid crystalline phases and show relatively high glass transition temperatures and good thermal stability.

Nonlinear optical properties of Au/PVP composite thin films

Colloidal Au and poly（vinylpyrrolidone） （PVP） composite thin films are fabricated by spin-coating method. Linear optical absorption measurements of the Au/PVP composite films indicate an absorption peak around 530 nm due to the surface plasmon resonance of gold nanoparticles. Nonlinear optical properties are studied using standard Z-scan technique, and experimental results show large optical nonlinearities of the Au/PVP composite films. A large value of χ^（3）/α up to 0.56× 10-^10esu·cm is obtained, which is comparable to the best values reported in metal/oxlde composite films.

Optical nonlinearity measurement of 4-(N-methyl,N-hydroxyethl)amino,4'-nitroazobenzene using a transmittance technique with a phase object(T-PO) with top-hat beams at 600-nm wavelength

The transmittance technique with a phase object（T-PO）,for measuring optical nonlinear coefficients is proposed with a top-hat beam.The sensitivity of the T-PO with a top-hat beam is a factor of 4 greater than that with a Gaussian beam.The validity of this method is verified by measuring the nonlinearity of a well-characterized liquid,CS 2 at 532-nm wavelength.The ease of use of this method has been proved by measuring a new compound 4-（N-methyl,N-hydroxyethyl）amino,4＇-nitroazobenzene（ANAB） at 600-nm wavelength,indicating that this method can be extended to the measurement of optical nonlinearities in a wide-band spectrum.

Nonlinear Optical Spatial Filtering for Medical Image Processing

The nonlinear properties of Tris(acetylacetonato) Manganese(III) are used to manipulate the spatial frequencies at the Fourier plane using 4f-z scan. The technique is a simple self-adaptive all-optical system, which performs image processing and nonlinear optical measurements at the same time. Preferred spatial frequencies can be selected by shifting the nonlinear sample through the focus. Edge enhancement was demonstrated by filtering of low frequency with the nonlinear material at the Fourier plane.

Crystal Growth and Structure of Novel Tolane Nonlinear Optical Materials

A novel tolane 4-methoxy-4'-nitro-diphenyl-acetylene (MONA) has been prepared quantitatively by reacting cuprous p-methoxy phenyl-acetylene with p-iodonitrobenzene. A single crystal of the Moan was grown by solution growth method. The crystal was then characterized by X-ray diffraction structure analysis and second-harmonic generation(SHG)investigation. Polymorphous crystal forms of the MONA were grown from different solvents having different nonlinear optical properties depending on their different crystal structures. The relationship between the crystal growth and crystal structure is discusse.

All-optical switching and nonlinear optical properties of HBT in ethanol solution

This paper demonstrates an all-optical switching model system comprising a single pulsed pump beam at 355 nm and a CW He-Ne signal beam at 632.8 nm with 2-（2＇-hydroxyphenyl）benzothiazole （HBT） in ethanol solution. The origins of the optical switching effect were discussed. By the study of nonlinear optical properties for HBT in ethanol solvent, this paper verified that the excited-state intramolecular proton transfer （ESIPT） effect of HBT and the thermal effect of solvent worked on quite different time scales and together induced the change of the refractive index of HBT solution, leading to the signal beam deflection. The results indicated that the HBT molecule could be an excellent candidate for high-speed and high-sensitive optical switching devices.