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.     

Generation of nanosecond terahertz pulses by the optical rectification method

The possibility of the generation of quasi-cw terahertz radiation by the optical rectification method for broad-band Fourier unlimited nanosecond laser pulses has been experimentally demonstrated. The broadband radiation of a LiF dye-center laser is used as a pump source of a nonlinear optical oscillator. The energy efficiency of terahertz optical frequency conversion in a periodically polarized lithium niobate crystal is 4 × 10⁻⁹ at a pump power density of 7 MW/cm².     

Laser ablation of gallium arsenide in different solutions

The optical, structural, and nonlinear optical characteristics of GaAs nanoparticles obtained by laser ablation in different liquids were investigated. Thermally induced self-defocusing in GaAs solutions was observed using both a high pulse repetition rate and nanosecond pulses. In studying the nonlinear optical characteristics of GaAs solutions using picosecond and femtosecond pulses, two-photon absorption was observed. The nonlinear absorption coefficient of an aqueous GaAs solution measured by the Z-scan technique and the nonlinear susceptibility of GaAs nanoparticles were, respectively, 0.7 × 10^?9 cm W^?1 and 2 × 10^?9 esu at a wavelength of 795 nm.     

Laser ablation of GaAs in liquids: structural, optical, and nonlinear optical characteristics of colloidal solutions

We investigated the optical, structural, and nonlinear optical properties of GaAs nanoparticles prepared by laser ablation in various liquids at the wavelengths of 795 nm and 1,054 nm. The slow-thermal-effect-induced self-defocusing processes were dominating both in the cases of high pulse repetition rate and nanosecond pulses. The two-photon absorption was observed in these colloidal solutions in the case of low pulse repetition rate of picosecond and femtosecond radiation. The nonlinear susceptibility of GaAs nanoparticles ablated in water was measured to be 2× 10^–9 esu.     

Laser ablation of silver in different liquids: Optical and nonlinear optical properties of silver nanoparticles

The optical, structural, and nonlinear optical properties of silver nanoparticles prepared using the method of laser ablation in various liquids at wavelengths of 397, 532, and 795 nm with laser pulses of different duration are studied. An analysis of the dimensional and spectral characteristics of the silver nanoparticles revealed a time dynamics of the nanoparticle size distribution in solutions. It is shown that thermal self-defocusing is observed for the case of nanosecond or shorter pulses generated with a high repetition rate. For picosecond and femtosecond pulses with a low repetition rate, the effects of self-focusing (γ = 3 × 10^?13 cm² W^?1) and saturated absorption (β = ?1.5 × 10^?9 cm W^?1) were observed in the solutions under study. The third-order nonlinear susceptibility of the silver nanoparticles was found to be 5 × 10^?8 esu at a wavelength of 397 nm.     

Z-scan studies and optical limiting of nanosecond laser pulses in neutral red dye

The nonlinear optical absorption, refraction and optical limiting behaviour of an organic dye, neutral red, were investigated under excitation with nanosecond laser pulses at 532 nm. The nonlinear optical responses of the material were studied both in solution and solid film, made in methanol and polyvinyl alcohol, respectively, using single-beam Z-scan technique. The open aperture Z-scans of the solution samples displayed a switch over from saturable absorption to enhanced absorption with increase in input intensity. Theoretical fit to the experimental data indicated that the dominant mechanism of nonlinear absorption is two-photon absorption. The closed aperture Z-scans of both the samples denoted positive nonlinearity, which was three orders larger in magnitude in solid film, compared with that in solution. The results of optical limiting experiments revealed that neutral red exhibited strong optical limiting of nanosecond laser pulses with a threshold lower than that of C₆₀ in toluene.     

3,3′-Benzene-1,4-diylbis[1-(substituted)phenylprop-2-en-1-one] derivatives: A new class of materials for third-order nonlinear optical applications

We have investigated the third-order nonlinear optical parameters of Bischalcones embedded in DMF solution and in solid PMMA matrix, by Z-scan technique using nanosecond laser pulse trains at 532 nm. Z-scan results reveal that the Bischalcones exhibits negative nonlinear refractive index as high as 10⁻¹¹ esu. The molecular two-photon absorption cross-section of Bischalcones were of the order 10⁻⁴⁶ cm⁴ s/photon, which is nearly two orders of magnitude larger than that of Rhodamine 6G which is 10⁻⁴⁸ - 10⁻⁵⁰ cm⁴ s/photon. We found that, the two-photon absorption (TPA) is the dominating nonlinear process leading to nonlinear absorption in both the cases in solution and as well as in solid medium. Based on TPA process, the Bischalcones exhibit good optical power limiting of nanosecond laser pulses at the input wavelength. The nonlinear optical parameters found to increase on enhancing the strength of the electron donor groups indicating the dependence and importance of electron donor/acceptor units on third-order nonlinear optical susceptibility χ⁽³⁾.     

Third-order optical nonlinearities of α,ω-dithienylpolyenes and oligo(thienylvinylene)

α,ω-Dithienylpolyenes and oligo(thienylvinylene) are interesting third-order nonlinear optical materials for a variety of device applications. To better understand the third-order nonlinear response of these materials, the third-order susceptibilities (χ⁽³⁾) and nonlinear absorption behaviors of two α,ω-dithienylpolyenes with different conjugation length and two oligo(thienylvinylene) with different substituents on the thiophene rings have been studied using degenerate four wave mixing (DFWM) and nonlinear transmission techniques at 532 nm. The χ⁽³⁾ values of 1×10⁻³ mol/l solutions are all of the order of 10⁻¹³ esu. The χ⁽³⁾ values increase with the increase of the linear absorption coefficient. In addition, these compounds exhibit reverse saturable absorption for nanosecond laser pulses. The strength of reverse saturable absorption varies when the conjugation length and substituents change. Moreover, the nonlinear absorption characteristics of these compounds in the picosecond regime differ from those in the nanosecond regime. The different nonlinear absorption behavior is due to the relative contributions from excited singlet–singlet and triplet–triplet absorption. The strong reverse saturable absorption characteristics of two of the compounds suggest that they could be potential candidates for optical limiting applications in the nanosecond regime.     

Nonlinear optical properties of organic dye dimer-monomer systems

An analysis is provided for the discussion of nonlinear optical properties of aggregated dye systems. The intensity-dependent transmission of fluorescein solutions excited by nanosecond dye laser pulses is shown to fit a monomer-dimer equilibrium shifted towards monomer formation by excitation. The implications for spatial light modulation and other nonlinear optical applications are discussed.     

Nonlinear optical characteristics of a pseudoisocyanine solution

The saturated nonlinear absorption and Kerr nonlinearities of an aqueous pseudoisocyanine solution are investigated at the wavelengths of 532 and 529 nm with the use of pulsed laser radiation of different duration (8 ns and 475 fs). The measured values of the nonlinear refractive indices amount to ?6×10^?12 (t=8 ns) and ?8×10^?14 cm²W^?1 (t=475 fs). The change in self-action effects in pseudoisocyanine from self-defocusing to self-focusing revealed in the case of increasing intensity of femtosecond laser pulses is attributed to the effect of a fifth-order nonlinear optical process. The nonlinear refractive index responsible for this process amounts to 4×10^?24 cm⁴ W^?2. The imaginary part of the third-order nonlinear susceptibility, responsible for the induced transparency of the pseudoisocyanine solution, is Imχ ⁽³⁾=?2×10^?12 esu. Temporal changes in the shape of nanosecond laser pulses due to the nonlinear refraction induced by a thermal process are analyzed.     

Self-Q-switched Er-Brillouin fiber source with extra-cavity generation of a Raman supercontinuum in a dispersion-shifted fiber

Brillouin mirrors based on a single-mode optical fiber provide the simplest, completely passive, and most universal way to produce nanosecond pulses with extensive wavelength tunability. We propose an all-fiber solution, where a passively Q-switched Er-doped Briilouin fiber laser pumped by a low-power laser diode produces pulses with a peak/average power contrast of 500 W/25 mW and, in association with a conventional dispersion-shifted fiber employed as an extracavity nonlinear medium, causes the generation of a nanosecond supercontinuum extending from 900 to over 1800 nm. Expanding evolution of the spectrum kicked off by the multicascade Brillouin process is reported.     

Interband phototransitions involving free electrons: III. Transmission of light through crystals

It has been shown that the two-electron mechanism of nonlinear optical absorption considered in the first two parts of our study, even at laser radiation intensities j ～ 10³-10⁴ W/cm² in the case of nanosecond pulses, can lead to almost complete absorption of light by crystals that are transparent to weak radiation of the same wavelength. A number of materials that can exhibit the considered effects have been described.     

Time resolved spectra of optical and electrical transient response induced by nanosecond laser pulses in amorphous AgInSbTe films

The phase transition dynamics of amorphous Ag₈In₁₄Sb₅₅Te₂₃ (AIST) thin films induced by single nanosecond laser pulses were studied by transient optical reflectivity and electrical resistance measurements with nanosecond resolution. Phase transition driven by nanosecond laser pulses can be achieved in a proper fluence range on AIST thin films. The results show that phase transition dynamics driven by nanosecond laser pulses was a multi-stage optical evolution process involving melt, solidification, recalescence, and recrystallion. However, it was found that the real-time responses of optical and electrical signals were quite different under the same irradiated condition. The recalescence process reflected by the second rising of optical reflectivity will not result in obvious changes in electrical resistance. The dependence of saturated time determined by optical and electrical evolution curve on laser pulse fluence was compared and analyzed. A two-dimensional percolation model was employed to explain the difference between electrical and optical transient responses.     

Properties of optical limitation of radiation in π-conjugated organic systems doped with fullerenes (The COANP-C70 system)

The effect of optical limitation of laser radiation in 2-cyclooctylamino-5-nitropyridine (COANP-C₇₀) doped with fullerene is experimentally studied. The energy density of the incident beam is measured to be ～4–4.5 J cm^?2 and the attenuation coefficients and the absorption spectrum of a new structure are determined. The photoinduced variation of the refractive index of the COANP-fullerene system and its influence on the optical limitation is studied in the visible range upon irradiation by nanosecond laser pulses. The mechanisms of optical limitation of radiation in these structures are specified. The nonlinear optical coefficients n ₂ and χ⁽³⁾ of the fullerene-doped π-conjugated COANP system are measured for the first time by the methods of dynamic holography.     

Nonlinear optical studies of 1-3-diaryl-propenones containing 4-methylthiophenyl moieties

The third-order nonlinear optical properties of chalcone derivatives have been studied using the single beam Z-scan technique. The dependence of χ⁽³⁾ on different donor and acceptor type substituents demonstrates the electronic nonlinearity of compounds. The largest value of nonlinear refractive index, n₂, measured for a high electron donor substituted molecule is −2.033 × 10⁻¹¹ esu. These molecules exhibit a strong two-photon absorption and interesting optical limiting of nanosecond laser pulses at 532 nm.     

Optical limiting effect based on stimulated Brillouin scattering in CCl4

The optical limiting effect based on stimulated Brillouin scattering (SBS) in a nonlinear medium was investigated. We numerically treated the nonlinear propagation process with a theoretical model, which includes the spontaneous nature of the initiation of SBS, and obtained optical limiting effect in the process. Energy limiting, pulse reshaping and stabilization have been demonstrated on SBS mechanism with the nonlinear medium CCl_4. The input optical signals were Nd:YAG nanosecond laser pulses with width varying from 16ns to 7ns then to 2ns, the relationship between the transmitted signal and launched pump signal was shown. In the experimental regime, the most stable pulse and a superior energy stabilization of the transmitted pulse were obtained when the laser pulse-width became as short as 2ns. For the energy variation of laser pulses in a wide range of 14－88mJ, the output energy was limited in a quite narrow range 4.5－5.5mJ.     

Comparison of Solutions of the General Nonlinear Amplitude Equation and a Modified Schrӧdinger Equation

We review the dynamics of narrow and broad-band optical pulses in nonlinear dispersive media. A major problem that arises during the development of theoretical models, which describe accurately and correctly the behavior of these pulses, is the limited application of the nonlinear Schr?dinger equation. It describes very well the evolution of nanosecond and picosecond laser pulses. However, when we investigate the propagation of femtosecond and attosecond light pulses, it is necessary to use the more general nonlinear amplitude equation. We show that in this equation two additional terms are included and they have a significant impact on the phase of the pulse. We perform numerical simulations and show the temporal shift of the position of fundamental solitons. This effect depends on the initial duration of the laser pulses. To clarify the influence of the additional terms on the parameters of the optical pulses, we consider the nonlinear amplitude equation, which is a modified nonlinear Schr?dinger equation.     

受激布里渊散射对纳秒激光脉冲光限幅规律

 研究了受激布里渊散射对纳秒激光脉冲的光限幅效应。针对四氯化碳介质研究了受激布里渊散射对2ns激光脉冲的光限幅和稳定输出能量的特性,给出了光限幅特性及输出能量与光限幅介质的结构参数之间的关系。对于输入能量波动范围在 13%的激光脉冲,实验获得输出能量波动范围为 7%,与理论分析的结果基本符合。     

Optical Performance and Nonlinear Scattering of Soluble Polystyrene Grafted Multi-Walled Carbon Nanotubes

Three soluble polystyrene grafted multi-walled carbon nanotube （MWNT） samples are synthesized, and their optical performance and nonlinear scattering properties are investigated by z-scan method using nanosecond pulses of 532 nm from a frequency-doubled Q-switched Nd： YLF laser. Analysis of the experimental results shows that other than nonlinear scattering, nonlinear absorption plays a major role in optical limiting performance of these stable and well-dispersed suspensions. These new synthesized materials which can be better dispersed in common organic solvents than MWNT itself can be considered as potential sources for further optical applications.     

抽运能量对受激布里渊散射光限幅特性的影响

采用布里渊噪声起源模型,数值模拟了受激布里渊散射介质CCl4对波长1064nm的Nd：YAG纳秒激光脉冲的传输特性及光限幅特性。入射抽运脉冲能量较低时,非线性介质对纳秒激光脉冲呈光学透明。入射抽运脉冲能量高于受激布里渊散射产生阈值后,透射脉冲峰值受限,脉宽压缩,能量趋于饱和,说明该光学系统同时具有光功率限幅和能量限幅的光限幅特性。利用理论模型模拟了如下光限幅参量：透射脉冲峰值功率、透射能量、能量透射率、脉宽压缩率依赖抽运光能量的变化关系。相应的理论模拟计算结果由实验进行验证,实验结果与理论模拟相符合。