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 susceptibilities χ of nitridosilicate powders

Nitridosilicates are of interest as novel nonlinear materials due to their extraordinary chemical and thermal stability. Unfortunately, large nitridosilicate single crystals are presently not available for the investigation of their nonlinear optical properties. The first experiments are presented in which an averaged nonlinear susceptibility χ⁽²⁾ for several nitridosilicates is studied by using two different powder techniques, the Kurtz Perry method and the SHEW method (Second Harmonic Wave generated by an Evanescent Wave). We observe nonlinearities of the new materials which are comparable to those of LiIO₃. The highest averaged M_eff=(χ_eff⁽²⁾)²/4n_2ωn_ω² values found are ∼0.9 pm²/V². The refractive indices of the materials are determined to be between n=2 and 3.     

色散磁导率对异向介质中的调制不稳定性的影响

基于Drude模型研究了异向介质的色散磁导率对调制不稳定性的影响. 结果表明,在反常色散情形,赝五阶非线性在异向介质的负折射区中增大了调制频谱的范围及增益值,这与常规正折射介质中出现的现象正好相反;自陡峭效应在异向介质中有可能为负值,但无论正负,也无论在正折射区还是负折射区,它都抑制调制不稳定性的产生;二阶非线性色散效应在正、负折射区中分别促进和抑制调制不稳定性的产生. 在正常色散情形,由于二阶非线性色散效应的作用,使本来在常规正折射介质中不可能出现的调制不稳定性现象也能出现,这一特性为在正常色散区形成孤 关键词： 异向介质 调制不稳定性 色散磁导率 二阶非线性色散     

Ag:Bi2O3复合膜的线性和非线性光学性质

从实验和理论两个方面，探讨了金属Ag不同掺杂浓度对Ag:Bi₂O₃复合膜线性和非线性光学性质的影响. 用吸收光谱研究了Ag浓度与Ag:Bi₂O₃复合膜表面等离子体共振带之间的关系；用皮秒Z-扫描技术研究了共振和非共振情况下(激发光波长分别为532nm和1064nm)，金属Ag浓度与复合膜三阶非线性极化率的关系. 基于表面等离子体共振理论和局域场增强理论对复合膜进行了分析，得到了不同Ag浓度时Ag:Bi₂O₃复合膜的三阶非线性效应，研究了激发波长和金属浓度对复合膜线性和非线性光学性质的影响. 结果表明，等离子体共振增强和合适的金属掺杂浓度使得三阶极化率增强二个量级，在Ag浓度为35％左右和接近等离子体共振频率(相应吸收带位于560nm—622nm)的532nm激发时，χ⁽³⁾具有最大值2.4×10^-9esu. 关键词： 金属纳米颗粒 复合膜 三阶非线性 表面等离子体共振     

Au:TiO2和Au:Al2O3纳米颗粒复合膜的线性和非线性光学特性

主要从实验和理论两个方面,探讨了不同Au颗粒尺寸和不同基质对Au：TiO₂和Au：Al₂O₃复合膜线性和非线性光学性质的影响.用吸收光谱研究了Au颗粒尺寸和基质与Au复合膜表面等离子体共振带之间的关系;用皮秒Z扫描技术研究了共振和非共振情况下(激发光波长分别为532nm和1064nm),Au颗粒尺寸和基质与复合膜三阶非线性极化率的关系.基于表面等离子体共振理论和局域场增强理论对复合膜进行了分析,得到了不同Au颗粒大小和不同基质时Au复合膜的 关键词： 金属纳米颗粒 复合膜 三阶非线性 表面等离子体共振     

Enhanced nonlinear optical responses in metal-glass nanocomposites

The “engineered” nonlinear nanocomposite materials with extremely large values of optical Kerr susceptibility and fast temporal responses that can be precisely tuned to satisfy the requirements of switching applications is of current interest in photonics. Metal quantum-dot composite glasses can exhibit enhanced optical susceptibility, χ⁽³⁾, whose real and imaginary parts are related to the intensity-dependent refractive index and two-photon absorption coefficient, respectively. Classical (dielectric) and quantum confinement effects come into play in the nonlinear optical responses of these nanocomposites. Metal nanocluster-glass composites have been synthesized by 200 keV Cu⁺ and 1.5 MeV Au⁺ ion implantations in fused silica glasses at a dose of 3 × 10¹⁶ ions/cm², followed by thermal annealing in reducing atmosphere to promote cluster growth. UV-Visible spectroscopy has revealed prominent linear absorption bands at characteristic surface plasmon resonance (SPR) frequencies signifying appreciable formation of copper and gold colloids in glass matrices. Third-order optical properties of the composite materials have been studied by Z-Scan and Anti-Resonant Interferometric Nonlinear Spectroscopy (ARINS) measurements. The sign of nonlinear refraction is readily obtained from the Z-Scan signatures. The ARINS technique utilizes the dressing of two unequal-intensity counter-propagating pulsed light beams with differential nonlinear phases, which occur upon traversing the sample if it exhibits nonlinear optical response. This difference in phase manifests itself in the intensity-dependent transmission. The nonlinear refractive index, nonlinear absorption coefficient, the real and imaginary parts of the third-order optical susceptibility have been extracted.     

Investigation of third-order nonlinear optical susceptibility in polymer complexes of diarylidenealkanones

The third-order nonlinear optical susceptibility in polymer complexes of diarylidenealkanones has been investigated by the third harmonic generation technique at a wavelength of 1.06 μm. The macroscopic nonlinear susceptibility χ ⁽³⁾ measured is compared with the calculated γ values of the second-rank molar hyperpolarizability tensor. It is demonstrated that low-molecular chromophores can be used in syntheses of the stable polymer composite systems with a high nonlinear optical susceptibility. A further improvement in the nonlinear optical properties of complexes between deprotonated chromophores and high-basicity polymers can be achieved using the proposed methods. __________ Translated from Fizika Tverdogo Tela, Vol. 42, No. 11, 2000, pp. 2099–2102. Original Russian Text Copyright ? 2000 by Ten’kovtsev, Yakimanski, Lukoshkin, Dudkina, Boehme.     

Study of the maximum conversion efficiency of the four-wave mixing process based on the Hamiltonian approach

In the four-wave mixing process, since the intensity of the generated coherence field is related closely to the third-order nonlinear susceptibility. With the help of a Hamiltonian approach, we obtain the expression of third-order nonlinear susceptibility χ⁽³⁾, and the special relation between χ⁽³⁾ and the nonlinear conversion coefficient. They are very useful to analyze the phase mismatch due to the Kerr effect and linear refraction contributions, which affect the maximum conversion efficiency under the condition taking account into pump field depletion. The investigative results show that energy conversion efficiency from the weak idler field to the generated field may exceed 100% when the phase mismatch induced by linear refraction is compensated, though the phase mismatch contribution from the Kerr effect can not be compensated simultaneously. Moreover, the conversion efficiency of the photon numbers fast reaches a plateau value.     

Detection of a new SRS‐promoting phonon mode and cross‐cascaded χ(3)‐nonlinear lasing in single crystals of calcite (trigonal CaCO3)

For calcite (CaCO₃), one of the pioneer crystals in nonlinear optics, new results of stimulated Raman scattering (SRS) spectroscopy are presented. Among them are the discovery of a new SRS‐promoting vibration mode with ω_SRS2 ≈︁ 282 cm^‐1 and its participation, together with the main SRS mode ω_SRS1 ≈︁ 1086.5 cm^‐1, in cross‐cascaded (χ⁽³⁾ ↔ χ⁽³⁾) nonlinear‐lasing generation, as well as the observation of efficient self‐upconversion via cascaded parametric four‐wave processes of one‐micron Stokes and anti‐Stokes χ⁽³⁾‐lasing into the UV‐region of third harmonic generation. The investigations show that calcite is able to generate a χ⁽³⁾‐lasing comb of more than two octaves bandwidth. The article also gives a brief review on the discovery and study of the SRS‐effect in natural crystals (minerals), which have expanded our ability to study the photon‐phonon nonlinear‐laser interactions in crystalline materials. A short summary of information about χ⁽³⁾‐lasing properties of the triangular planar structure units in SRS‐active crystals is included.     

Comparative analysis of multi-wave mixing and measurements of the higher-order nonlinearities in resonant media

The features of degenerate multi-wave mixing in resonant media (dye solutions) have been studied theoretically and experimentally. It has been demonstrated that thermal nonlinearity due to the induced absorption from the excited level contributes significantly to the efficiency of four-wave mixing, but results in lower efficiency of higher-order interactions. The measurement results obtained for the energy efficiency of four-, six- and eight-wave mixing enable calculations of the third-, fifth- and seventh-order nonlinear optical susceptibilities, respectively. Experimentally, the method proposed for measurements of the higher-order nonlinearities has been realized with the use of the multi-wave mixing at second harmonic λ = 532 nm of monopulse YAG:Nd³⁺ laser radiation in a Rhodamine 6G dye solution. The ratios ∣χ⁽⁵⁾∣/∣χ⁽³⁾∣ and ∣χ⁽⁷⁾∣/∣χ⁽⁵⁾∣ are determined to be of the order of 10⁻⁵ cm³/erg.     

Enhanced optical nonlinearities of superlattices within the Kronig-Penney model incorporating inherent bulk nonlinearities

Third order nonlinear optical susceptibilities χ⁽³⁾ of GaAs/Ga_1?xAlAs superlattices have been predicted which are two orders of magnitude larger than those of bulk GaAs. This enhancement is due to the band nonparabolicity arising from the additional periodicity of the superlattice. These predictions, based on a tight-binding model of the superlattice dispersion, are here extended to the more realistic Kronig-Penney (KP) model. Corrections to tight-binding are non-negligible; however, enhancements of χ⁽³⁾ are still large but reduced approximately 30%–50% over previous estimates. The KP model is also here applied to superlattices employing InSb as the quantum well material. Because of the smaller effective mass of InSb, and taking account of its bulk nonparabolicity, the minibands move to higher energy, enhancing the interwell overlap and increasing χ⁽³⁾ by about one order of magnitude over that of bulk InSb. The role of the barrier material in this case is important and is discussed. The interplay between the bulk nonparabolicity and that arising from the superlattice is also addressed.     

Characterization of nonlinear optical parameters of KDP,LiNbO3 and BBO crystals

Third-order nonlinear susceptibilities (χ⁽³⁾) and nonlinear refractive indices (n₂) of KDP, BBO and LiNbO₃ crystals are measured at the wavelengths of 1064 nm and 532 nm by Z-scan technique. The measurements were carried out at different pulse energies, focusing conditions, and crystals’ lengths. It was shown that the increase of phase-matching angle leads to the decreasing of χ⁽³⁾ of KDP crystals. The parameters of multi-photon absorption in KDP, BBO and LiNbO₃ crystals are determined. The analysis and comparison of experimental and theoretical values of nonlinear susceptibilities are presented.     

Nonlinear electrostatic response of strongly correlated one-dimensional electron systems

We investigate the nonlinear response of the strongly correlated one-dimensional electron systems to the static electric field with using the one-dimensional Hubbard model in the half-filled case. We adopt the variational Monte Carlo method with the Gutzwiller wave function to describe the strong correlation effects. In the weak correlation region U/t≤4, where U is the one-site Coulomb repulsion energy and t is the transfer integral between the nearest neighbor sites, the response can be described within the band picture, and the third order nonlinear susceptibility χ⁽³⁾ increases slowly with increasing U/t. For U/t≤4, χ⁽³⁾ increases rapidly with increasing U/t, and χ⁽³⁾ at U/t=10 is more than ten times larger than that at U/t=2. This large value of χ⁽³⁾ originates from the exotic properties of carriers in the strongly correlated one-dimensional electron systems.     

Z-scan and optical limiting properties of Hibiscus Sabdariffa dye

The intensity-dependent refractive index n ₂ and the nonlinear susceptibility χ ⁽³⁾ of Hibiscus Sabdariffa dye solutions in the nanosecond regime at 532 nm are reported. More presicely, the variation of n ₂, β, and real and imaginary parts of χ ⁽³⁾ versus the natural dye extract concentration has been carried out by z-scan and optical limiting techniques. The third-order nonlinearity of the Hibiscus Sabdariffa dye solutions was found to be dominated by nonlinear refraction, which leads to strong optical limiting of laser.     

Third-order nonlinear optical response in double-walled carbon nanotubes

Resonant behavior and magnitudes of third-order nonlinear optical susceptibilities in double-walled carbon nanotubes (DWNTs) have been investigated by means of femtosecond pump-probe spectroscopy with different pump-photon energies. With the selective excitation of the E₂₂ exciton transition of the inner tubes labeled by the chiral vector indices (7,5) and (7,6), the imaginary part of nonlinear susceptibility Imχ⁽³⁾ has shown the resonant enhancement compared with the case of the nonresonant excitation of the specific tube. The nonlinear response signal at the E₂₂ transition energy of the (8,7) tube has been also enhanced for the excitation of the G-band phonon sideband of its E₂₂ transition. This result is consistent with the phonon-mediated nonlinear optical process observed for the E₂₂ transitions in single-walled carbon nanotubes (SWNTs). It has been also found that the values of the figure of merit Im χ⁽³⁾/α (α: absorption coefficient) of the inner tubes in DWNTs are smaller than those of the corresponding SWNTs, which is interpreted in terms of decay time shortening due to the energy relaxation between the inner and outer tubes.     

Fast nonlinear optical mechanism of photoconversion in systems of lyotropic ionic liquid crystals–viologen impurities

We study a new nonlinear optical mechanism of reversible photoconversion between excited dimers and cation radicals, the reduction products of electrochromic molecules (viologens), in lyotropic ionic liquid crystals of metal alkanoates. The results of the theoretical study are compared with experimental data obtained from dynamic holographic recordings as well as nonlinear absorption measurements. The estimated value of the photoconversion probability is higher than the probability of non-radiative relaxation of excited molecules. The value of the cubic nonlinearity is χ ^(3)?～?4?·?10^?7?esu for colored cells of these materials.     

The nonlinear optical susceptibilities of polydiacetylenes

We present a general formalism of the NLO susceptibilities by using the Genkin-Mednis approach for a one-dimensional electron-lattice system. Based on the SSH model, we obtained an analytic expression for the third-order nonlinear optical susceptibilities χ⁽³⁾(ω) for polydiacetylenes (PDAs) after considering the case of conjugated chains, in which there is no adjustable parameter. The results are in good agreement with experiments on PDAs. Furthermore, the origin of the second peak in the χ⁽³⁾(ω) spectrum of PDAs is discussed, and a transition mechanism is proposed. It is believed that when the external light field is applied along the centrosymmetric polymer backbone, the parity symmetry of the system is broken, there occurs a mixing between the even- and odd-parity exciton states, leading to the transition from the ground state to the A_g excited state, and accordingly a second sharp peak appears in the χ⁽³⁾(ω) spectrum which could be attributed to the three-photon resonance with the A_g exciton generation process at around 2.2 eV.     

CdSe量子点的线性和非线性光学特性

主要从实验和理论两个方面,探讨了强受限尺寸区域内不同尺寸对CdSe量子点线性和非线性光学性质的影响.用吸收光谱研究了量子点尺寸与吸收峰之间的关系,用皮秒Z扫描技术研究了共振和非共振情况下(激发光波长分别为532和1064nm),尺寸与三阶非线性极化率之间的关系.基于电子能量状态理论和局域场增强理论对量子点进行分析,得到了CdSe不同尺寸的三阶非线性效应,研究了尺寸对量子点非线性光学性质的影响.结果表明,由激发态粒子数布局改变和纳米颗粒增大引起的非线性共振增强效应相当,二者共同作用使得三阶极化率增强20倍左右,且用532nm的共振频率激发4.3nm CdSe量子点时,χ⁽³⁾具有最大值2.0×10^-11esu. 关键词： CdSe量子点 三阶非线性 Z扫描')" href="#">Z扫描 量子限域效应     

Nonlinear optical properties of Au/ZnO nanoparticle arrays

The triangular-shaped Au/ZnO nanoparticle arrays were fabricated on fused quartz substrate using nanosphere lithography. The structural characterization of the Au/ZnO nanoparticle arrays was investigated by atomic force microscopy. The absorption peak due to the surface plasmon resonance of Au particles at the wavelength of about 570 nm was observed. The nonlinear optical properties of the nanoparticle arrays were measured using the z-scan method at a wavelength of 532 nm with pulse duration of 10 ns. The real and imaginary part of third-order nonlinear optical susceptibility, Re χ⁽³⁾ and Im χ⁽³⁾, were determined to be 1.15 × 10⁻⁶ and −5.36 × 10⁻⁷ esu, respectively. The results show that the Au/ZnO nanoparticle arrays have great potential for future optical devices.     

Diagnostic study of the roughness surface effect of zirconium on the third-order nonlinear-optical properties of thin films based on zinc oxide nanomaterials

Zinc oxide (ZnO) and zirconium doped zinc oxide (ZnO:Zr) thin films were deposited by reactive chemical pulverization spray pyrolysis technique on heated glass substrates at 500 °C using zinc and zirconium chlorides as precursors. Effects of zirconium doping agent and surface roughness on the nonlinear optical properties were investigated in detail using atomic force microscopy (AFM) and third harmonic generation (THG) technique. The best value of nonlinear optical susceptibility χ⁽³⁾ was obtained from the doped films with less roughness. A strong third order nonlinear optical susceptibility χ⁽³⁾ = 20.12 × 10⁻¹² (esu) of the studied films was found for the 3% doped sample.