Third-Order Nonlinear Optical Susceptibility of Indium Phosphide Nanocrystals

InP nanocrystals synthesized by refluxing and annealing of organic solvent are determined from XRD measurements to have an averse granularity of 25 nm. The nonlinear optical properties of the InP nanocrystals studied by using laser Z-scan technique with 50 ps pulses at 532nm are found to reveal strong nonlinear optical properties and two-photon absorption phenomenon. Also, the nonlinear absorption coeffcient, the nonlinear refractive index and the third-order nonlinear optical susceptibility are determined by experiments, in which the nonlinear refractive index is three orders of magnitude larger than that of bulk InP.     

Large third-order optical nonlinearities in brilliant green solutions induced by CW He-Ne laser

Laser induced third-order nonlinear optical responses of Brilliant Green solution (which belongs to triphenylmethane organic dye group) was investigated by utilizing single beam Z-scan technique using a continuous wave He-Ne laser at the wavelength of 632.8 nm. It was observed that the material exhibits self-defocusing and saturation absorption type optical nonlinearity behavior. The measurements of the real and imaginary parts of the third-order nonlinear optical susceptibility were carried out at several incident laser irradiations and different dye concentrations. It was found that the increase in any of the incident laser intensity or solution concentration leads to the linear increase of the nonlinear refractive index. The obtained values of the third-order nonlinearities of Brilliant Green solutions are amongst the highest reported CW regimes, to the best of our knowledge. This study shows a great potential of the Brilliant Green for the application in nonlinear optical devices.     

Enhancement of optical switching parameter and third-order optical nonlinearities in embedded Si nanocrystals: A theoretical assessment

Third-order bound-charge electronic nonlinearities of Si nanocrystals (NCs) embedded in a wide band-gap matrix representing silica are theoretically studied using an atomistic pseudopotential approach. Nonlinear refractive index, two-photon absorption and optical switching parameter are examined from small clusters to NCs up to a size of 3 nm. Compared to bulk values, Si NCs show higher third-order optical nonlinearities and much wider two-photon absorption-free energy gap which gives rise to enhancement in the optical switching parameter.     

Lead sulfide colloidal nanocrystals with strong optical nonlinearity

Colloidal PbS nanocrystals have been synthesized by a developed procedure. UV–Vis absorption and Z-scan technique was also applied to study the nonlinear optical properties of prepared lead sulfide nanocrystals at 532 nm wavelength. The nonlinear refractive (n₂) and absorption (β) were determined which are confirming the strong nonlinearity at 532 nm of colloidal PbS nanocrystals. The obtained results have not been reported before. In this study, only a weak thermal optical nonlinearity was observed and the dominating nonlinear response is resulted by the electronic origin. The nonlinear optical properties of prepared sample supported wide applications in nanophotonics.     

Quantum crystallites and nonlinear optics

This is a review and analysis of the optical properties of quantum crystallites, with principal emphasis on the electro-optic Stark effect and all optical third order nonlinearity. There are also introductory discussions on physical size regimes, crystallite synthesis, quantum confinement theory, and linear optical properties. The experiments describe CdSe crystallites, exhibiting strong confinement of electrons and holes, and CuCl crystallites, exhibiting weak confinement of the exciton center of mass. In the CdSe system, neither the Stark effect nor the third order nonlinearity is well understood. The Stark shifts appear to be smaller than calculated, and field inducted broadening also occurs. The third order nonlinearity is only modestly stronger than in bulk material, despite theoretical prediction. Unexpectedly large homogeneous widths, due to surface carrier trapping, in the nominally discrete crystallite excited states appear to be involved. The CuCl system shows far narrower spectroscopic homogeneous widths, and corresponds more closely to an ideal quantum dot in the weak confinement limit. CuCl also exhibits exciton superradiance at low temperature. Surface chemistry and crystallite encapsulation are critical in achieving the predicted large Stark and third order optical effects in II-VI and III-V crystallites.     

CuO薄膜的三阶非线性光学特性研究

采用脉冲激光沉积技术在Si(100)和熔石英基片上制备了单相的CuO薄膜.通过X射线衍射仪,拉曼光谱仪,场发射扫描电镜和紫外可见光光度计对薄膜的结构,表面形貌和光学性质进行了表征. 场发射扫描电镜结果表明CuO薄膜中晶粒排列致密且分布均匀,其尺寸约为45nm.结合飞秒激光(800nm,50fs)和Z扫描方法测量了薄膜的三阶非线性光学特性,结果表明CuO薄膜具有超快的非线性光学响应且非线性折射率和非线性吸收系数均为负值,其大小分别为-3.96×10^-17 m^{2< 关键词： CuO薄膜 Z-扫描')" href="#">Z-扫描 三阶光学非线性}     

A sensitive method for measurements of complex third-order susceptibilities in waveguides

A method for measuring complex fast nonlinear optical nonlinearities χ ⁽³⁾ in waveguides is demonstrated. It is based on a comparison between the optical nonlinearities of two different samples under identical experimental circumstances and thus is independent of laser pulse parameters. Heterodyne detected four-wave mixing is employed to achieve information about both amplitude and phase of χ ⁽³⁾. To increase the sensitivity, a procedure for suppression of the limiting parasitic signals due to the photodiode nonlinearity is suggested. Results obtained from a short piece of hollow-core photonic bandgap fiber are presented.     

Absorption spectroscopy of uranium plasma for remote isotope analysis of next-generation nuclear fuel

CdSe/Se multilayer thin films were prepared using sequential thermal evaporation technique by varying the thickness of selenium sublayers. Identifying the prominent peaks observed in the XRD spectra of the top layer CdSe which corresponds to the (100) plane with wurtzite structure, the average size of the crystallites was calculated for the CdSe nanocrystals. Experimentally measured band gaps are larger than bulk band gap of CdSe. This confirms the presence of spin-orbit splitting of energy levels. Size of the crystallites was then calculated with the theoretical prediction of the effective mass approximation model (i.e., Brus model). It resulted in that the diameters of crystallites were much smaller than the Bohr exciton diameter (11.2 nm) of CdSe. Thus the structural and optical properties of CdSe/Se multilayer thin films reveal the effect of quantum confinement of CdSe crystallites in Se matrix for various sublayer thicknesses. Confinement effect is more pronounced while sublayer thickness of selenium increases.     

Stable helical solitons in optical media

We present a review of new results which suggest the existence of fully stable spinning solitons (self-supporting localised objects with an internal vorticity) in optical fibres with self-focusing Kerr (cubic) nonlinearity, and in bulk media featuring a combination of the cubic self-defocusing and quadratic nonlinearities. Their distinctive difference from other optical solitons with an internal vorticity, which were recently studied in various optical media, theoretically and also experimentally, is that all the spinning solitons considered thus far have been found to be unstable against azimuthal perturbations. In the first part of the paper, we consider solitons in a nonlinear optical fibre in a region of parameters where the fibre carries exactly two distinct modes, viz., the fundamental one and the first-order helical mode. From the viewpoint of application to communication systems, this opens the way to doubling the number of channels carried by a fibre. Besides that, these solitons are objects of fundamental interest. To fully examine their stability, it is crucially important to consider collisions between them, and their collisions with fundamental solitons, in (ordinary or hollow) optical fibres. We introduce a system of coupled nonlinear Schrödinger equations for the fundamental and helical modes with nonstandard values of the cross-phase-modulation coupling constants, and show, in analytical and numerical forms, results of collisions between solitons carried by the two modes. In the second part of the paper, we demonstrate that the interaction of the fundamental beam with its second harmonic in bulk media, in the presence of self-defocusing Kerr nonlinearity, gives rise to the first ever example of completely stable spatial ring-shaped solitons with intrinsic vorticity. The stability is demonstrated both by direct simulations and by analysis of linearized equations.     

Determination of optical Kerr nonlinearity of a photonic bandgap structure by Z-scan measurement

Through analysis of the dispersion relation in a photonic bandgap structure, the effective optical Kerr nonlinearity that determines a Z-scan profile particularly near the stop-band edges, is derived. Near and inside the stop band, the nonlinear optical phase change that originates from an off-resonant response is converted into a change in nonlinear optical intensity through Bragg reflection. The Z-scan measurement of a cholesteric liquid-crystal photonic bandgap structure confirmed that off-resonant Kerr nonlinearity is responsible for the characteristic open-aperture Z-scan profiles near the stop-band edges.     

玻璃中CdSSe纳米晶体的光谱性能

对掺有镉、硒、硫的玻璃在650—800℃退火4?h，生长了不同尺寸的CdS0.13Se0.87纳米晶体，测量了纳米晶体的吸收光谱、光致发光（PL）谱和电调制光谱，确定了纳米晶体部分电子态的能量，讨论了CdSSe纳米晶体的光学性质与其尺寸之间的依赖关系.随着纳米晶体尺寸的增大，对应激子的吸收峰、PL峰及电吸收信号发生红移，表现出明显的量子尺寸效应.小尺寸纳米晶体的电吸收表现为量子受限的Stark效应，而大尺寸纳米晶体的电吸收线形与体材料的相似；随着纳米晶体尺寸的增大，电吸收信号增强.所有尺寸的纳米晶体都表现 关键词： CdSSe纳米晶体 吸收光谱 光致发光谱 电光响应     

The nonlinear optical response of a fluorine-containing azoic dye

The nonlinear optical nonlinearities of a fluorine-containing azoic dye in tetrahydrofuran have been investigated by using Z-scan technique with picosecond and nanosecond lasers. The experimental results reveal that the azoic dye has large optical nonlinearity under the excitations of picosecond and nanosecond 532 nm. At the picosecond 532 nm the solution presents negative nonlinear refraction due to the electronic effect, while the larger nonlinear refraction under nanosecond laser excitation is induced by thermal effect. Moreover, the different nonlinear absorption behavior under picosecond and nanosecond excitations is analyzed.     

Effect of thickness on the optical nonlinearity of gold colloidal nanoparticles prepared by laser ablation

The effect of thickness on the nonlinear optical properties of Au nanoparticles which produced by laser ablation of high purity gold bulk in distilled water were investigated by employing different optical techniques. Experiments were performed on the 0.3, 0.6, and 1 mm thickness cells of Au nanoparticles-fluid. The effect of nonlinear refractive index of samples on the laser beam broadening was observed. The optical limiting behavior of samples is investigated by measuring the transmitted intensity of the laser beam through the samples. The third order nonlinearity of Au nanoparticles-fluid was measured by using Z-scan data. Results show a positive second order refractive index and absorption coefficient for Au nanoparticles-fluid that are increased in due of increasing the thickness of the cells. The magnitudes of both real and imaginary parts of third order susceptibility of samples are increased by increasing the thickness.     

Third-Order Nonlinear Optical Response near the Plasmon Resonance Band of Cu_(2-x)Se Nanocrystals

The third-order nonlinear optical properties of water-soluble Cu_(2-x)Se nanocrystals are studied in the near infrared range of 700-980 nm using a femtosecond pulsed laser by the Z-scan technique. It is observed that the nonlinear optical response of Cu_(2-x)Se nanocrystals is sensitively dependent on the excitation wavelength and exhibits the enhanced nonlinearity compared with other selenides such as ZnSe and CdSe. The W-shaped Z-scan trace, a mixture of the reversed saturated absorption and saturated absorption, is observed near the plasmon resonance band of Cu_(2-x)Se nanocrystals, which is attributed to the state-filling of free carriers generated by copper vacancies(self-doping effect) of Cu_(2-x)Se nanocrystals as well as the hot carrier thermal effect upon intense femtosecond laser excitation. The large nonlinear optical response and tunable plasmonic band make Cu_(2-x)Se nanocrystals promising materials for applications in ultra-fast all-optical switching devices as well as nonlinear nanosensors.     

Low-frequency four-photon spectroscopy of surface waves in semiconductors: A new mechanism of optical nonlinearity

A new mechanism of optical nonlinearity of intrinsic semiconductors is proposed, which is based on bandgap modulation due to the four-wave mixing of interacting waves on the semiconductor surface. This phenomenon is theoretically considered within a one-dimensional model. The corresponding resonances are experimentally found in Ge and Si samples.     

Size and dielectric dependence of the third-order nonlinear optical response of Au nanocrystals embedded in matrices

The third-order nonlinear optical response of Au nanocrystals embedded in BaTiO(3) and ZrO(2) matrices was investigated through the off-resonance femtosecond optical Kerr effect. Compared with pristine films, the nonlinearity of composite films shows an enhancement that depends on the sizes of Au particles and the refractive index of the matrices. We performed a calculation based on Lorenz-Mie scattering theory to explain the experimental results. Additionally, the nonlinearity was optimized by determination of the values of the particle size and the refractive index of the matrix.     

Optical soliton perturbation in non-Kerr law media: Traveling wave solution

This paper analyses the dynamics of soliton propagation through optical fibers with non-Kerr law nonlinearities. The governing nonlinear Schrödinger equation is integrated in the presence of perturbation terms. The traveling wave hypothesis is used to carry out the integration. Domain restrictions on the soliton parameters are identified in the process. The five forms of nonlinearity that are studied are Kerr-law, power-law, parabolic-law, dual-power law and the log-law nonlinearity. Numerical simulations are presented for each of these nonlinear media.     

Theory of multi-exciton states in semiconductor nanocrystals

In this article, the fundamental physics of multi-exciton states in semiconductor nano-crystals is reviewed focusing on the mesoscopic enhancement of the excitonic radiative decay rate and the excitonic optical nonlinearity and the mechanism of their saturation with increase of the nanocrystal size. In the case of the radiative decay rate the thermal excitation of excited exciton states having small oscillator strength within the homogeneous linewidth of the exciton ground state is essential in determining the saturation behavior. The weakly correlated exciton pair states are found to cause a cancellation effect in the third-order nonlinear optical susceptibility at the exciton resonance, providing the first consistent understanding of the experimentally observed saturation of the mesoscopic enhancement of the excitonic optical nonlinearity. The presence of the weakly correlated exciton pair states is confirmed convincingly from the good correspondence between theory and experiments on the induced absorption spectra from the exciton state in CuCl nanocrystals. Furthermore, ultrafast relaxation processes of biexcitons are discussed in conjunction with the observed very fast rise of the biexciton gain in nanocrystals. In prospect of future progress in research, the theoretical formulation to calculate the triexciton states as one of the multi-exciton states beyond the biexciton is presented for the first time including the electron-hole exchange interaction.