Third-Order Optical Nonlinearity of a Novel Material：（Tetramethylammonium） bis （1,3-dithiole-2-thione-4,5-dithiolato） Copper

A novel dmit^2- salt： （tetramethylammonium）bis（1,3-dithiole-2-thione-4,5-dithiolato） copper, abbreviated as MECu, is synthesized and its third-order optical nonlinearity is characterized by Z-scan technique at a wavelength of 1064nm with laser duration of 30ps. Z-scan curves reveal a negative Kerr coefficient at 1064nm and no nonlinear absorption is observed. The nonlinear refraction coefficient n2 and the second hyperpolarizability γ have been determined to be as large as 2.15 × 10^-11 esu and 3.23 × 10^-31 esu, respectively, suggesting MECu is a potential material for optical device applications.     

Nonlinear and saturable absorption properties of PbS nanocrystalline thin films

The structural, morphological, optical, and nonlinear optical properties of a lead sulfide （PbS） thin film grown by chemical bath deposition （CBD） are investigated by X-ray diffraction （XRD）, scanning electron microscope （SEM）, ultraviolet-visible （UV-Vis）, and open aperture Z-scan experiments. The band gap energy of the PbS nanocrystalline film is 1.82 eV~ higher than that of bulk PbS at 300 K. The nonlinear absorption properties of the film are investigated using the open aperture Z-scan technique at 1064 nm and pulse durations of 4 ns and 65 ps. Intensity-dependent switching of the film from nonlinear absorption to saturable absorption is observed. The nonlinear absorption coefficient increases monotonically with increasing pulse duration from 65 ps to 4 ns.     

Observation of Two-Photon Absorption and Nonlinear Refraction in AlN

Two-photon absorption(TPA) and nonlinear refraction in AlN single crystals are revealed with the single beam Z-scan technique.A large TPA coefficient of 13±3 cm/GW at 355 nm and third-order nonlinear refractive indices of-1.91±0.38 x 10~(-13) cm~2/W at 355 nm,1.79±0.36×10~(-13) cm~2/Wat 532 nm and 1.61±0.32× 10~(-12) cm~2/W at 1064 nm are derived.It is inferred that the TPA-generated free carriers are responsible for the large negative nonlinear refractive index at 355 nm,while the oxygen impurity induced bandgap narrowing may account for the large third-order nonlinear refractive indices at 532 nm and 1064 nm.The large nonlinear optical responses of AlN promise wide applications in the deep ultraviolet nonlinear optical devices.     

Off-Resonant Third-Order Optical Nonlinearity of Au Nanoparticle Array by Femtosecond Z-scan Measurement

A periodic triangular-shaped Au nanoparticle array is fabricated on a quartz substrate using nanosphere lithography and pulsed laser deposition, and the linear and nonlinear optical properties of metal particles are studied. The morphology of the polystyrene nanosphere mask （D = 820 nm） and the Au nanoparticle array are investigated by scanning electron microscopy. The surface plasmon resonance absorption peak is observed at 606 nm, which is in good agreement with the calculated result using the discrete dipole approximation method. By performing the Z-scan method with femtosecond laser （800 nm, 50 fs）, the optical nonlinearities of A u nanoparticle array are determined. The results show that the Au particles exhibit negative nonlinear absorption and positive nonlinear refractive index with the effective third-order optical nonlinear susceptibility Xeff^（3） can be up to （8.8 ± 1.0）× 10^-10 esu under non-resonant femtosecond laser excitation.     

Nonlinear optical properties of polyaniline composite materials

The nonlinear optical properties of polyaniline composite materials (PANI/Au) were studied using the single-beam Z-scan technique.These molecules exhibited a strong reverse saturable absorption and an interesting optical limiting performance with a nanosecond Nd:YAG laser pulses at 532 nm.     

Large Third-Order Optical Nonlinearity of Cadmium Sulphide Nanoparticles Embedded in Polymer Thin Films

A simple method for synthesis of well dispersed cadmium sulphide nanoparticles embedded in a polyethylene glycol matrix （PEG 400） in thin film form is presented. The large blue shift of the band gap energy of the CdS nanoparticles compared to the bulk semiconductors is observed via UV-vis absorption spectra. Photoluminescence spectra of CdS nanocomposite films show that the emission peaks shift towards the longer wavelength with the increase of annealing temperature. Transmission electron microscopic images as well as Raman scattering studies confirm the CdS nanometer size particle formation within the polymer matrix. The particle size is about 8 nm. Selected area electron diffraction （SAED） shows the cubic zinc blende polycrystalline rings. Third-order optical nonlinearity of the CdS nanopartieles embedded in polymer thin films is studied with the Z-scan technique under 1064 nm excitation. The results show that the CdS nanocomposite film exhibits negative nonlinear refraction index and positive absorption coefficient. The film shows large optical nonlinearity, and the magnitude of the third-order nonlinear susceptibility of the film is calculated to be 1.73 × 10^-9 esu. The corresponding mechanism is discussed.     

Nonlinear optical behaviors in a silver nanoparticle array at different wavelengths

The optical nonlinearities of an Ag nanoparticle array are investigated by performing Z-scan measurements at the selected wavelengths (400, 600, 650, and 800 nm). The nonlinear refraction index in the resonant region (around 400 nm) exhibits a significant enhancement by two orders compared with that in the off-resonant region (around 800 nm)), and exhibits an sign alternation of the resonant nonlinear absorption, which results in a negligible nonlinear absorption at a certain excitation intensity. Moreover, a low degree of nonlinear absorption was measured at the edges of the resonant region (600 and 650 nm), which is attributed to the competition of the saturated absorption and the two-photon absorption processes.     

Effect of Fe concentration on the nonlinear refraction and reverse saturable absorption in ferroelectric X-cut LiNbO_3 crystal

In this Letter, the effects of the iron(Fe) dopant concentration on the nonlinear optical properties of iron-doped ferroelectric X-cut Li Nb O3 crystals plates are studied by using the Z-scan technique with a cw laser at the wavelength of 532 nm. The amount of iron in the compound is varied from 0 to 0.15 mol%. Measurements of nonlinear refractive index n2 and the nonlinear absorption coefficient β are determined. The sign of the nonlinear refractive index is found to be negative and the magnitude is on the order of 10-8cm2∕W. This nonlinear effect increases as the concentration increases from 0 to 0.15 mol%. A good linear relationship is obtained between nonlinear refractive index, nonlinear absorption coefficient, and concentration.     

Multi-wavelength measurements of aerosol optical absorption coefficients using a photoacoustic spectrometer

The atmospheric aerosol absorption capacity is a critical parameter determining its direct and indirect effects on cli- mate. Accurate measurement is highly desired for the study of the radiative budget of the Earth. A multi-wavelength （405 rim, 532 nm, 780 nm） aerosol absorption meter based on photoacoustic spectroscopy （PAS） invovling a single cylin- drical acoustic resonator is developed for measuring the aerosol optical absorption coefficients （OACs）. A sensitivity of 1.3 Mm-l （at 532 nm） is demonstrated. The aerosol absorption meter is successfully tested through measuring the OACs of atmospheric nigrosin and ambient aerosols in the suburbs of Hefei city. The absorption cross section and absorption Angstrom exponent （AAE） for ambient aerosol are determined for characterizing the component of the ambient aerosol.     

Nonlinear Optical Properties of Novel Polymeric Rare Earth Phthalocyanine Studied Using Picosecond Z-Scan Technique

Three novel tri-dimensional phthalocyanine polymers, with lanthanum （LaPPc）, gadolinium （GdPPc） and ytterbium （YbPPc） as centric atoms, have been synthesized from a tetranuclear phthalonitrile. Third-order optical nonlinearities of these compounds in DMF solution are measured by a picosecond Z-sacn technique at 532 nm. It is found that all the compounds show reverse saturation absorption and nonlinear self-focus refraction effect. The second-order molecular hyperpolarizabilities are calculated to be 1.82×10^-23, 1.48×10^-23 and 1.45×10^-23 esu for LaPPc, GdPPc and YbPPc, respectively. The differences among their nonlinear optical properties are attributed to the special tri-dimensional structure and the variation in rare earth atoms.     

Enhanced optical nonlinear absorption of graded Au--TiO2 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.     

Study on nonlinear optical absorption properties of [(CH3)4N]2[Cu(dmit)2] by Z-scan technique

The third-order optical nonlinearities of an organo-metallic compound, [(CH₃)₄N]₂[Cu(dmit)₂] (dmit²⁻=4,5-dithiolate-1,3-dithiole-2-thione), abbreviated as MeCu, dissolved in acetone are characterized by Z-scan technique with picosecond and nanosecond laser pulses in the near-infrared region. Two-photon absorption has been found when the sample solution is irradiated by 40 ps pulse width at 1064 nm and the two-photon absorption (TPA) coefficient β_TPA is 4×10⁻¹³ m/W. While excited by 15 ns laser pulses at 1053 nm, the Z-scan spectra reveal strong reverse saturable absorption (RSA) and the nonlinear absorption coefficient β_RSA is estimated to be as high as 7.07×10⁻¹¹ m/W which is much larger than β_TPA. An explanation for this enhancement is given. All the results suggest that MeCu may be a promising candidate for the application to optical limiting in the near-infrared region.     

Short pulse Z -scan investigations of optical nonlinearities of a novel organometallic complex: [(C2H5)4N]2[Cu(dmit)2] at 532 and 1064?nm

A novel dmit organometallic complex: [(C₂H₅)₄N]₂[Cu(dmit)₂] (dmit^2-=1,3-dithiole-2-thione-4,5-dithiolate), abbreviated as EtCu, was synthesized. Afterwards its optical nonlinearities in acetone solution at 532 nm and 1064 nm were studied by the Z-scan technique with laser pulses of picosecond duration. The two-photon absorption at 1064 nm and the saturable absorption at 532 nm were observed. The Z-scan curves also revealed that EtCu sample solutions exhibited self-defocusing effects at both wavelengths. The origins were analyzed for the differences between the results. All the outcomes suggest that this material is potential for nonlinear optical device applications. PACS 42.65.An; 42.65.Hw; 42.65.Jx; 81.20.Ka; 78.30.Jw     

First-principles study on the electronic structure and optical properties of T12Cd2（SO4）3 and Rb2Cd2（SO4）3

With the help of ab initio full-potential linearized augmented plane wave （FPLAPW） method, calculating the electronic structure and linear optical properties is carried out for XCd2（SO4）3 （X =Tl, Rb）. The results show that Tl2Cd2（SO4）3 （TlCdS） has a larger band gap than Rb2Cd2（SO4）3 （RbCdS） and the energy bands for RbCdS are more dispersive than those of TlCdS. From their partial densities of states （PDOS）, we have observed that the hybridization between S ionic 2p and O atomic 2p orbitals forms SO4 ionic groups. The remarkable difference between RbCdS and TlCdS is, however, the degree of hybridization between cation （Tl and Rb） and its surrounding oxygen atoms. In the view of quantum chemistry, the strong p-d hybridization indicates the existence of their cation ionic bonds （Cd-O, Rb-O, and Tl-O）. The calculations of TlCdS and RbCdS show their optical properties to be less anisotropic. Their anisotropies in the optical properties mainly occur in a low photon energy region of 5-16 eV.     

Elastic scattering of two H（^2Sg） and N（^4Su） atoms at low temperatures and accurate spectroscopic parameters of NH （X^3∑^-） radical

This paper reports that the interaction potential for the X3Z- state of NH radical is constructed at the CCSD（T）/ cc-PV6Z level of theory. Using this potential, this paper calculates the spectroscopic parameters （De, Re, ωe, ωeχe, αe and Be） and their values are of 3.578eV, 0.10368nm, 3286.833cm^-1, 78.433cm^-1, 0.6469cm^-1 and 16.6735cm^-1 respectively, which are in excellent agreement with the experiments. Then the total of 14 vibrational states has been found when J=0 by solving the radial Schrodinger equation of nuclear motion. For each vibrational state, the vibrational manifolds are reported for the first time. And last, the total cross sections, s-wave, p-wave and d-wave cross sections are computed for the elastic collisions between two ground-state atoms （hydrogen and nitrogen） at low temperatures. It finds that the total elastic cross sections are dominated by s-wave scattering when the collision energy is below 10^-6a.u. The pronounced shape resonance is found at energy of 6.1 × 10^-6a.u. Calculations have shown that the shape resonance comes from the p-wave contributions.     

Experimental Study on Optical Limiting and Transient All-optical Switching Properties of a Cubanelike Transition-metal Cluster Compound (n-Bu4N)3[MoAg3BrI3S4]

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Investigation of the nonlinear absorption and optical limiting properties of two [Q]2[Cu(C3S5)2] compounds

The nonlinear absorption properties of two organometallic compounds, [(C₂H₅)₄N]₂[Cu(C₃S₅)₂] (DCu1) and [(C₄H₉)₄N]₂[Cu(C₃S₅)₂] (DCu2), have been investigated using an open-aperture Z-scan technique at 1064 nm with 40 ps pulse width and at 1053 nm with 18 ns pulse width. The reverse saturable absorption (RSA) which was observed in both samples with nanosecond pulse excitation was much larger than that observed with picosecond pulse excitation. The nonlinear absorption properties were analyzed theoretically by a five-level model. Optical limiting based on RSA was performed and limiting thresholds were evaluated for both samples under three conditions. DCu1 exhibited the better limiting characteristics because of its stronger RSA response.     

Third-order nonlinearity and optical limiting of dichloromethane solutions of cis-Mo(CO)4(PPh3)2

Oxidized dichloromethane solutions of cis-Mo(CO)₄(PPh₃)₂ stabilized by the addition of excess PPh₃ exhibit unusual large molecular second-order hyperpolarizabilities with minimal linear absorption. To better understand the mechanism by which this occurs, DFWM, Z-scan and optical limiting experiments have been carried out on oxidized dichloromethane solutions of cis-Mo(CO)₄(PPh₃)₂ using 5.8 ns laser pulses at 532 nm. Our results demonstrate that the mechanism by which the oxidized species enhance the third-order nonlinear response is not dominated by thermal effects, but is instead due to the strong nonlinear absorption and nonlinear refraction of the oxidized species. Moreover, the oxidized species shows very strong optical limiting properties. Such complexes would be very interesting third-order nonlinear optical materials for optical limiting applications.     

Te/TeO2-SiO2复合薄膜的吸收和非线性光学特性研究

应用分光光度计测量Te/TeO₂-SiO₂复合薄膜的透射光谱和吸收光谱, 在480nm附近观察到Te颗粒引起的等离子体共振吸收峰; 采用Z扫描技术研究了共振(激发波长为532 nm)和非共振情况下(激发波长1064 nm) 不同电位制备薄膜的Te颗粒状态与复合薄膜的三阶非线性极化率的关系. 基于有效介质理论对复合薄膜的三阶非线性效应进行分析, 研究Te颗粒大小对Te/TeO₂-SiO₂复合薄膜的非线性光学性质的影响及其产生机理. 结果表明薄膜制备过电位增大, Te的粒径减小, 颗粒数量多, 颗粒分布趋于均匀, 使得金属颗粒的表面等离子体共振峰红移, 吸收强度增强, 导致三阶非线性光学效应增强, χ⁽³⁾由1064 nm的5.12×10^-7 esu增大为532 nm的8.11×10^-7 esu. 关键词： 碲 二氧化碲 复合薄膜 三阶非线性     

Measurement of wurtzite ZnO/rutile TiO2 heterojunction band offsets by x-ray photoelectron spectroscopy

Four novel dmit complexes: [(C₂H₅)₄N][Ni (dmit)₂], [(C₃H₇)₄N][Ni(dmit)₂], [(C₂H₅)₄N][Au(dmit)₂] and [(C₃H₇)₄N][Au(dmit)₂], abbreviated as EtNi, PrNi, EtAu, and PrAu, were synthesized. The third-order nonlinear optical properties of them in acetonitrile solutions were investigated by using the Z-scan technique with 20 ps pulses width at 1064 nm. When the on-axis irradiance at focus I ₀ was 5.025 GW/cm², the nonlinear refraction coefficient n ₂, the third-order nonlinear susceptibility χ ⁽³⁾, the molecular second-order hyperpolarizability γ of the four types of material were obtained with subject to Z-scan curves, and these indexes were with the magnitudes of 10⁻¹⁸ m²/W, 10⁻¹³ esu, and 10⁻³¹ esu, respectively. The nonlinear absorption coefficient β of Ni samples had the 10⁻¹² m/W scale. The impact of different metals and cations on the third-order nonlinear optical properties of materials was analyzed. Through the derivation, the result suggests that these dmit complexes are promising candidates for applications to nonlinear optical devices manufacture in the near-infrared waveband.