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.

PREPARATION AND SECOND-ORDER OPTICAL NONLINEARITY OF NOVEL PHENOXYSILICON NETWORKS BY SOL-GEL PROCESS

Four phenoxysilicon networks for nonlinear optical (NLO) applications were designed and prepared by an extended sol-gel process without additional H2O and catalyst. All poled polymer network films possess high second-order nonlinear optical coefficients (d(33)) Of 10(-7)similar to 10(-8) esu. The investigation of NLO temporal stability at room temperature and elevated temperature (120 degreesC) indicated that these films exhibit high d(33) stability because the orientation of the chromophores are locked in the phenoxysilicon organic/inorganic networks.

Influence of optical nonlinearity on combining efficiency in ultrashort pulse fiber laser coherent combining system

The influence of optical nonlinearity on combining efficiency in ultrashort pulse fiber laser coherent combining system is investigated theoretically and experimentally.In the theoretical work,a new theoretical algorithm is presented for the coherent combining efficiency,which can be used to quantify the spectral coherence decay induced by optical nonlinearity imbalance between the sub-beams.The spectral information of the sub-beam is obtained by numerically solving the nonlinear Schrödinger equation(NLSE)in this algorithm to ensure an accurate prediction.In the experimental work,the coherent combining of two all-fiber picosecond lasers is achieved,and the influence of imbalanced optical nonlinearity on the combining efficiency is studied,which agrees with the theoretical prediction.This paper reveals the physical mechanism for the influence of optical nonlinearity on the combining efficiency,which is valuable for the coherent combining of ultrashort pulse fiber laser beams.

Enhanced optical nonlinear absorption of graded Au-TiO_2 composite films

This paper reports that single-layer and graded Au-TiO2 granular composite films with Au atom content 15%- 66% were prepared by using reactive co-sputtering technique. The third-order optical nonlinearity of single-layer and graded composite films was investigated by using s- and p-polarized Z-scans in femtosecond time scale. The nonlinear absorption coefficient βeff of single-layer Au-TiO2 films is measured to be -2.3×10^3-0.76×10^3 cm/GW with Au atom content 15%-66%. The βeff value of the 10-layer Au-TiO2 graded film is enhanced to be -2.1×10^4cm/GW calculated from p-polarized Z-scans, which is about ten times the maximum βeff of single-layer films. Broadened response in the wavelength region 730-860 nm of the enhanced optical nonlinearity of graded Au-TiO2 composite films was also investigated.

Ultrafast third-order optical nonlinearity of several sandwich-type phthalocyaninato and porphyrinato europium complexes

The third-order optical nonlinearity of two sandwich-type phthalocyaninato and porphyrinato europium com- plexes, including double- and triple-deckers （Eu[Pc（OC5H11）8]2, Eu2（Pc）（TPP）2, Pc=phthalocyanine, TPP=5, 10, 15, 20- tetraphenylporphyrinate）, was investigated by using the femtosecond time-resolved optical Kerr gate method at 830 nm wavelength. Their second-order hyperpolarizability is estimated to be 0.74× 10^-30esu and 3.0× 10^-3esu respectively. This exhibits an evident enhancement in comparison with 0.47×10^-30esu for one-decker Eu（Pc）（acac） （acac=acetylacetonate）, which is also measured under the same conditions. The enhancement is attributed to the introduction of lanthanide metal to the large π-conjugated system, intermacrocycle interaction and two-photon resonance etc.

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.

Studies of Optical Nonlinearity Behaviors of Ultrafine PbS Particles in Perfluorocarboxylated Cation-exchanged Films

Ultrafine PbS particles with different sizes have been prepared in perfluorocarboxylated cation-exchanged films. The variation of PbS particle size was clarified by absorption spectra and TEM graphs. Time-resolved optical Kerr effects were measured by femtosecond pump-probe techniques. Optical Kerr effect response time was estimated to be less than 165 fs. A third-order optical nonlinearity of χ(3)10-12 esu for PbS particles was obtained and it was found that it increases with the decrease of particle sizes, showing the influence of quantum confined effect on optical nonlinear behaviour of ultrafine particles.

The Synthesis of Third-order Optical Nonlinear Organic Polyheterocyclic Materials

Synthesis of the third-order nonlinear materials: bis (1,4-dihydroxynaphthalene) tetrathiafulvalene and bis (1,4-dialkoxylnaphthalene) tetrathiafulvalene has been achieved in four steps, starting from 2,3-dichloro-1,4-naphthaquinone. The materials exhibit larger third-order nonlinear optical susceptibilities c(3) .

Research progress of third-order optical nonlinearity of chalcogenide glasses

Chalcogenide glasses （ChGs） are a promising candidate for applications in nonlinear photonic devices. In this paper, we review the research progress of the third-order optical nonlinearity （TONL） of ChGs from the following three aspects： chemical composition, excitation condition, and post processing. The deficiencies in previous studies and further research of the TONL property of ChGs are also discussed.

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.

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.

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.

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.

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.

Optical Nonlinearity in a Novel Optical Signal Regeneration System Based on Cross-Gain Modulation Using Cascaded Semiconductor Optical Amplifiers

We propose a novel optical signal regeneration system based on wavelength converters by use of cross gain modulation in cascaded semiconductor optical amplifiers. The nonlinearity in optical input/output characteristics and eye opening using NRZ signal were archived.

Nonlinear optical properties in double-sided nonlinear media with Z-scan technique based on the Huygens-Fresnel principle

We present a theoretical model to analyse the propagation of a Gaussian laser beam through double-sided nonlinear media. This model is based on the Huygens-Fresnel diffraction integral method. This theoretical model is not only consistent with the cascade structure model for a small nonlinear phase-shift but also can be used for a large nonlinear phase-shift. It has been verified that it is suitable to characterize the double-sided nonlinear media compared with the cascade structure model. A good agreement between the experimental data and the results from the theoretical model is obtained. It will be useful for the design of multi-sided nonlinear materials.

Nonlinear optical properties of [（CH3）4N]Au（dmit）2 using Z-scan technique

The third-order optical nonlinearities of [（CH3）4N]Au（dmit）2 （dmit = 4,5-dithiolate-1,3-dithiole-2-thione） at 532 nm and 1064 nm are investigated using the Z-scan technique with pulses of picoseconds duration. The Z-scan spectra reveal a strong nonlinear absorption （reverse saturable absorption） and a negative nonlinear refraction at 532 nm. No nonlinear absorption is observed at 1064 nm. The molecular second-order hyperpolarizability γ for the [（CH3）4N]Au（dmit）2 molecule at 532nm is estimated to be as high as （2.1 ±0.1） × 10^-31 esu, which is nearly three times larger than that at 1064 nm. The mechanism responsible for the difference between the results is analysed. Nonlinear transmission measurements suggest that this material has potential applications in optical limiting.

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.

Dispersive Nonlinearity in Er-Doped Optical Fiber

Optical dispersive nonlinearities in Er-doped optical fiber are discussed and measured at the third window wavelength 1.55 μm for optical communications firstly. The experimental method, which is developed by us, is based on dynamic scanning for fixed-point-interference (DSFPI) of two fiber beams. The real part and complex value of the third-order susceptibility at the wavelength are also obtained from the measured Kerr coefficient and nonlinear-absorption coefficient reported elsewhere.