Third-order optical nonlinearity of a novel material: [(C<Subscript>4</Subscript>H<Subscript>9</Subscript>)<Subscript>4</Subscript>N][Co(dmit)<Subscript>2</Subscript>]

A novel dmit organometallic complex—[(C₄H₉)₄N][Co(dmit)₂] (dmit^2? = 4,5-dithiolate-1,3-dithiole-2-thione), abbreviated as BuCo, is synthesized and its third-order optical nonlinearity of the acetone solution is characterized using the Z-scan technique with a 40-ps pulse width at 1064 nm. Z-scan curves show that BuCo sample solution possesses the negative nonlinear refraction, exhibiting a self-defocusing effect. In addition, the two-photon absorption has been observed in BuCo. The effective molecular second-order hyperpolarizability γ_eff of the BuCo molecule was estimated to be as large as 5.60 × 10^?31 esu, suggesting BuCo is a potential material for optical device applications.     

适用于全光开关的[(C3H7)4N][Au(C3S5)2]三阶非线性光学性质研究

合成了一种金属有机配合物[(C3H7)4N][Au(C3S5)2].配制了浓度为1×10－3 mol/L的[(C3H7)4N][Au(C3S5)2]/乙腈溶液,并用旋涂法制备了掺杂浓度质量比为1%的[(C3H7)4N][Au(C3S5)2]/PMMA复合薄膜.运用Z扫描方法,分别研究了样品溶液和薄膜在波长为1 064 nm,脉宽为20 ps条件下的三阶非线性光学性质.研究发现薄膜的三阶非线性极化率χ(3)比溶液高出三个数量级.其中,薄膜的非线性折射率n2为－1.76×10－15 m2/W、三阶非线性极化率χ(3)为9.37×10－10 esu.结果表明,该材料在全光开关方面具有潜在的应用价值.     

Investigation of third-order nonlinear optical properties of NNDC-doped PMMA thin films by Z-scan technique

A novel chalcone derivative, (2E)-1-(2,4-di- chloro-5-fluorophenyl)-3-[4-dimethylamino)phenyl]prop-2-en-1-one, abbreviated as NNDC, was prepared and characterized by elemental analyses, infrared (IR) and proton nuclear magnetic resonance (¹H NMR) spectrum, and thermal analyses. The NNDC-doped poly(methyl methacrylate) (PMMA) thin films with five different doping concentrations by weight were prepared by using a spin-coating method. Their linear optical properties were investigated by using a prism coupling measuring system. The third-order nonlinear optical properties of NNDC in 1,2-dichloroethane (NNDC/1,2-dichloroethane) solution and NNDC-doped PMMA (NNDC/PMMA) films were investigated by using the laser Z-scan technique with 20 ps pulses at 532 nm. A self-focusing effect was observed from the Z-scan curves for solution and thin films and the nonlinear refractive index of the film increases with the increase of the doping concentration. In addition, nonlinear absorption was negligible for all samples. The magnitude of third-order nonlinear refraction index n ₂ and the third-order nonlinear susceptibility χ ⁽³⁾ for thin films were 10⁻¹⁵ m²/W and 10⁻⁹ esu, respectively, which are about three orders larger than that of NNDC/1,2-dichloroethane solution. Some necessary analyses were presented. The results show that this material is a promising candidate for application in the nonlinear optical devices at 532 nm.     

Large optical nonlinearity in CaCu<Subscript>3</Subscript>Ti<Subscript>4</Subscript>O<Subscript>12</Subscript> thin films

CaCu₃Ti₄O₁₂ (CCTO) thin films were successfully prepared on LaAlO₃ substrates by pulsed laser deposition technique. We measured the nonlinear optical susceptibility of the thin films using Z-scan method at a wavelength of 532 nm with pulse durations of 25 ps and 7 ns. The large values of the third-order nonlinear optical susceptibility, χ ⁽³⁾, of the CCTO film were obtained to be 2.79×10⁻⁸ esu and 3.30×10⁻⁶ esu in picosecond and nanosecond time regimes, respectively, which are among the best results of some representative nonlinear optical materials. The origin of optical nonlinearity of CCTO films was discussed. The results indicate that the CCTO films on LaAlO₃ substrates are promising candidate materials for applications in nonlinear optical devices.     

Studies on third-order nonlinear optical properties and reverse saturable absorption in polythiophene/poly (methylmethacrylate) composites

We report here the studies on third-order nonlinear optical properties of two novel polythiophene composite films investigated using the Z-scan technique. The measurements were carried out using a Q-switched, frequency doubled Nd:YAG laser producing 7 nanosecond laser pulses at 532 nm. Z-scan results reveal that the composite films exhibit self-defocusing nonlinearity. The real and imaginary parts of the third-order nonlinear optical susceptibility were of the order 10⁻¹² esu. The effective excited-state absorption cross section was found to be larger than the ground state absorption cross section, indicating that the operating nonlinear mechanism is reverse saturable absorption (RSA). The polythiophene composite films also exhibit good optical power limiting of the nanosecond laser pulses. The nonlinear optical parameters are found to increase on increasing the strength of the electron-donor group, indicating the dependence of χ ⁽³⁾ on the electron-donor/acceptor units of polythiophenes.     

The nonlinear optical property and photoinduced anisotropy of?a?novel azobenzene-containing fluorinated polyimide

A novel azobenzene-containing fluorinated polyimide was synthesized. The nonlinear optical property and photoinduced birefringence of a polyimide thin film were investigated. Large third-order nonlinear refraction (n ₂=−4.49×10⁻¹¹ cm²/W) was observed in the polyimide thin film by carrying out Z-scan measurement. The polyimide thin film exhibited larger nonlinear refraction than that of a mono-azo dye doped PMMA thin film (n ₂=−1.63×10⁻¹² cm²/W). The photoinduced birefringence of the polyimide thin film (▵ n∼10⁻²) under different pump intensities was investigated; it was much larger than that of the mono-azo dye doped PMMA thin film (▵ n∼10⁻³). Moreover, the time constants for birefringence growth and relaxation processes were determined.     

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     

Third harmonic generation of laser radiation in Fe- and Zn-doped polyvinylpyrrolidone

The results of third-order nonlinear susceptibilities studies of Fe- and Zn-doped polyvinylpyrrolidone (PVP) aqueous solution in processes of third harmonic generation of Nd:YAG laser radiation are presented. Nonlinear susceptibilities of PVP:Fe and PVP:Zn were calculated to be 5×10^-13 esu and 3×10^-13 esu respectively. Third harmonic conversion efficiencies in these metallocomplexes were measured to be 8×10^-7 and 5×10^-7 respectively. The Z-scan method was applied to determine Kerr effect influence on frequency conversion process. The value of nonlinear refractive index of PVP:Fe at the wavelength of λ = 1064 nm was measured to be n ₂ = - 6.7×10^-13 esu. Received 30 November 2001 / Received in final form 27 March 2002 Published online 28 June 2002     

Anharmonic force constants of GaSb from the measured third order elastic constants at 300°K

The third-order elastic constants of single crystal GaSb are determined using ultrasonic pulse interferometer at 10 MHz. The constants at 300°K, in units of 10¹¹ N.m.⁻², are C_l11 = ™ 4 ·75 ± 0·06 C₁₄₄ = + 0·50 ± 0·25 C₁₁₃ = ™ 3 ·08 ± 0·02 C₁₆₆ = ™ 2·16 ± 0·13 C₁₂₃ = ™ 0 ·44 ± 0·29 C₄₅₆ = ™ 0·25 ± 0·15 These constants are used to evaluate the three anharmonic first and second neighbour force constants based on modified Keating’s model. The constants are (in units of 10¹¹ N.m⁻²)γ=− 2·406;δ=0·407;ε=−0·222.     

Third-order nonlinear optical response of newly synthesized accepter/donor substituted propylidene aryloxy acet hydrazide

A class of organic compounds namely propylidene aryloxy acet hydrazide derivatives were synthesized. The third-order nonlinear optical properties and optical limiting studies of the compounds were investigated using the single beam Z-scan technique at 532 nm. The Z-scan study reveals that the compounds exhibit a self-defocusing effect at 532 nm. The calculated values of nonlinear refractive index, third-order nonlinear optical susceptibility and second order molecular hyperpolarizability are of the order of 10^?11 esu, 10^?13 esu and 10^?31 esu, respectively. The compounds exhibit good optical limiting properties at the wavelength used.     

Nonlinear optical absorption studies of an organo-metallic complex by Z-scan technique

An organo-metallic complex, [(CH₃)₄N][Ni(dmit)₂] (dmit²⁻ = (1,3-dithiole-2-thione-4,5-dithiolate), abbreviated as MeNi, is synthesized. The nonlinear optical absorption properties of MeNi dissolved in acetone have been studied using the open-aperture Z-scan technique with 40 ps pulse width at 1064 nm and 1 ns, 15 ns pulse width at 1053 nm, respectively. Strong saturable absorption has been found when the sample solution is irradiated by 40 ps and 1 ns laser pulses. While irradiated with 15 ns laser pulse, a stronger reverse saturable absorption has been found. The nonlinear optical absorption coefficients are −1.03 × 10⁻¹¹ m/W, −1.85 × 10⁻¹¹ m/W and 3.84 × 10⁻¹⁰ m/W, respectively. The mechanism responsible for the difference between the results is analyzed. All the results suggest that this material may be a promising candidate for the application to laser pulse compression in the near-infrared waveband.     

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.     

三-α-(2,4-二甲基-3-戊氧基)溴硼亚酞菁的三阶非线性光学性质研究

应用Z扫描技术，在波长为532nm、脉宽为8ns条件下，对一种新型亚酞菁配合物三-α-(2,4-二甲基-3-戊氧基)溴硼亚酞菁的三阶非线性光学特性进行了研究，结果发现，该新化合物有较强的反饱和吸收(β=3.7×10^-10 m/W)效应和非线性自聚焦折射效应(n₂=7.2×10^-11esu)，其三阶非线性极化率χ⁽³⁾=1.1×10^-11esu.分析了溴硼亚酞菁配合物特殊的锥形分子结构和重原子溴的轴向配位等因素对其三阶非线性光学性质的重要影响. 关键词： 亚酞菁 Z扫描 三阶光学非线性     

Nonlinear optical study of palladium Schiff base complex using femtosecond differential optical Kerr gate and Z-scan techniques

A femtosecond differential optical Kerr gate (DOKG) and Z-scan techniques, have been applied to investigate the third-order optical nonlinearity of composite film of the coordination complex [PdLPPh₃] (L=N-(2-pyridyl)-N′-(salicylidene)hydrazine, PPh₃=triphenylphosphine). Film exhibits superior nonlinear optical properties in the near-infrared spectral region. The nonlinear response time and third-order nonlinear optical susceptibility of complex were found to be≤90 fs and 3.9×10^?10 esu, respectively. The Z-scan result shows that saturable absorption property of the film and its nonlinear absorption coefficient of the sample was found to be ?23 cm/GW.     

Third-order nonlinear optical properties in [(C4H9)4N]2[Cu(C3S5)2]-doped PMMA thin film using Z-scan technique in picosecond pulse

An organometallic complex, [(C₄H₉)₄N]₂[Cu(C₃S₅)₂], abbreviated as BuCu, was synthesized. Then the BuCu-doped polymethylmethacrylate (PMMA) thin film with a doping concentration 1% by weight (1 wt.%) was fabricated using a spin-coating method and its third-order nonlinear optical properties were characterized using the Z-scan technique with 20 ps pulse duration at 532 and 1064 nm, respectively. The Z-scan curves have revealed that the material exhibits a self-defocusing effect at both wavelengths. Saturable absorption at 532 nm and two-photon absorption at 1064 nm were also found, respectively. Additionally, the calculated results of the material in film were compared with that of acetone solution, which indicated that the values in film were larger than that of acetone solution for about two orders in magnitude. The origins were analyzed of the difference between the two wavelengths. Our results suggest that considerable nonlinear optical properties were confirmed in BuCu-doped PMMA film. The material can easily be doped into PMMA film and forms a waveguide mode. So this material should be considered to be manufactured into devices and applied in all-optical switching, laser locking-mode, optical limiting fields etc.     

Third-order nonlinear optical properties of Bi2S3 and Sb2S3 nanorods studied by the Z-scan technique

Bismuth sulfide (Bi₂S₃) and antimony sulfide (Sb₂S₃) nanorods were synthesized by hydrothermal method. The products were characterized by UV-vis spectrophotometer, X-ray powder diffraction (XRD) and transmission electron microscope (TEM). Bi₂S₃ and Sb₂S₃ nanorods were measured by Z-scan technique to investigate the third-order nonlinear optical (NLO) properties. The result of NLO measurements shows that the Bi₂S₃ and Sb₂S₃ nanorods have the behaviors of the third-order NLO properties of both NLO absorption and NLO refraction with self-focusing effects. The third-order NLO coefficient χ⁽³⁾ of the Bi₂S₃ and Sb₂S₃ nanorods are 6.25×10⁻¹¹ esu and 4.55×10⁻¹¹ esu, respectively. The Sb₂S₃ and Bi₂S₃ nanorods with large third-order NLO coefficient are promising materials for applications in optical devices.     

Nonlinear optical properties of Cu nanocluster composite fabricated by 180 keV ion implantation

Metal nanocluster composite glass prepared by 180 keV Cu ions into silica with dose of 5×10¹⁶ ions/cm² has been studied. The microstructural properties of the nanoclusters has been verified by optical absorption spectra and transmission electron microscopy (TEM). Third-order nonlinear optical properties of the nanoclusters were measured at 1064 and 532 nm excitations using Z-scan technique. The nonlinear refraction index, nonlinear absorption coefficient, and the real and imaginary parts of the third-order nonlinear susceptibility were deduced. Results of the investigation of nonlinear refraction by the off-axis Z-scan configuration were presented and the mechanisms responsible for the nonlinear response were discussed. Third-order nonlinear susceptibility χ⁽³⁾ of this kind of sample was determined to be 8.7×10⁻⁸ esu at 532 nm and 6.0×10⁻⁸ esu at 1064 nm, respectively.     

Electrical characterization of the [N(CH<Subscript>3</Subscript>)<Subscript>4</Subscript>][N(C<Subscript>2</Subscript>H<Subscript>5</Subscript>)<Subscript>4</Subscript>]ZnCl<Subscript>4</Subscript> compound

The [N(CH₃)₄][N(C₂H₅)₄]ZnCl₄ compound has been synthesized by a solution-based chemical method. The X-ray diffraction study at room temperature revealed an orthorhombic system with P2₁2₁2 space group. The complex impedance has been investigated in the temperature and frequency ranges 420–520 K and 200 Hz–5 MHz, respectively. The grain interior and grain boundary contribution to the electrical response in the material have been identified. Dielectric data were analyzed using the complex electrical modulus M ^* for the sample at various temperature. The modulus plots can be characterized by full width at half height or in terms of a non-exponential decay function ϕ(t) = exp[(−t/τ) ^β ]. The detailed conductivity study indicated that the electrical conduction in the material is a thermally activated process. The variation of the AC conductivity with frequency at different temperatures obeys the Almond and West universal law.     

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