Nonlinear properties of composites based on dielectric layers containing copper and silver nanoparticles

Nonlinear optical characteristics of copper and silver nanoparticles in glass host matrices are studied by the Z-scan method at the wavelength of a Nd:YAG laser (λ=1064 nm) in a field of picosecond pulses. It is found that the third-order nonlinear susceptibility is more pronounced in glasses with copper nanoparticles than in glasses with silver nanoparticles. On the basis of experimental data obtained for samples with copper nanoparticles synthesized by ion implantation, it is shown for the first time that the nonlinear absorption of laser radiation with a wavelength lying out of the plasmon resonance region can be caused by a two-photon effect in metal particles. The character of the optical limiting process in the samples with copper nanoparticles when two-photon absorption is involved is discussed.     

Synthesis of Cu 2 O,CuCl, and Cu 2 OCl 2 nanoparticles by ultrafast laser ablation of copper in liquid media

Copper complex nanoparticles were fabricated from bulk copper using picosecond laser ablation in water and chloroform. We found that composition of the nanoparticles was CuCl and Cu₂OCl₂ in chloroform at three different input fluences; Cu₂O in water which was confirmed from the data of EDAX, UV-Visible absorption spectra, and selected area electron diffraction pattern. We have also performed nonlinear optical studies of colloidal nanoparticles using Z-scan technique at 800 nm and ～2 ps laser pulses. Cu₂O NPs exhibited two-photon absorption at lower peak intensities while three-photon absorption was observed at higher peak intensities. Other samples exhibited two-photon absorption at all peak intensities.     

Nonlinear optical characteristics of colloidal solutions of metals

Results of the study of nonlinear optical parameters of colloidal solutions of silver, gold, platinum, and copper by the Z-scan method are presented. The nonlinear refractive indices of these solutions at the wavelength of the Nd:YAG laser (λ=1064 nm) and its second harmonic (λ=532 nm) were measured. The two-photon absorption of these solutions and their nonlinear susceptibilities were studied.     

The features of nonlinear absorption during resonance one- and two-photon excitation of the basic exciton transition in colloidal CdSe/ZnS quantum dots

The features of the nonlinear absorption of CdSe/ZnS quantum dots (colloidal solution) in the case of resonant one- and two-photon excitation of the basic exciton transition by powerful ultra-short laser pulses were determined. In one-photon excitation, with an increasing intensity of impulses, a decrease in absorption (bleaching) is relayed by an increase in absorption, which is associated with the process of the filling of the states (saturation) of a two-level system with the lifetime of the excited state depending on the light intensity. The arising Fresnel or Fraunhofer diffraction of the laser ray that pass through a colloidal solution with a high concentration of quantum dots is associated with the formation of the transparency channel and self-diffraction of laser ray on an induced diaphragm. In two-photon excitation, the features of the nonlinear absorption and luminescence tracks (the dependence of luminescence intensity on distance) were explained by the influence, in addition to the two-photon absorption, of the processes that are responsible for the slower growth of nonlinear absorption and luminescence quenching at high intensities of laser pulses.     

Au纳米颗粒阵列中双光子吸收的饱和过程

采用纳米球蚀刻法制备了Au纳米颗粒阵列.并通过扫描电子显微镜观测了其表面形貌,表明三角形的Au纳米颗粒呈阵列状分布.采用Z扫描方法(800 nm, 50 fs)测量了Au纳米颗粒阵列的三阶非线性光学特性.在较小的激发功率下,结果呈现出双光子吸收效应,随着激发功率不断增加,出现了双光子吸收饱和的过程;非线性折射则呈现出自散焦效应.这种高效率的非线性响应机理使得该种Au纳米颗粒阵列在高速全光开关中有潜在的应用价值. 关键词： 纳米球蚀刻技术 Au纳米颗粒 三阶光学非线性     

Z-Scan studies of KYW, KYbW, KGW, and Ba(NO3)2 crystals

We present the studies of nonlinear refraction and nonlinear absorption in promising crystals which are extensively used in Raman lasers or as solid-state laser host materials: Ba(NO₃)₂, KGW, KYW, and KYbW. The single-beam z-scan technique with 1 ps laser pulses at 790 and 395 nm has been applied for the study. Nonlinear refraction-index intensity-coefficients and two-photon absorption coefficients have been determined for the crystals. The considerable enhancement of nonlinear refraction is observed in the crystals at 395 nm.     

Microfabrication of gold dots in SiO2/TiO2 glass films by two-photon absorption

Photogeneration of Au nanoparticles in SiO₂/TiO₂ glass films was carried out by two-photon absorption with a femtosecond pulse laser. Exquisite microdot-arrays of Au with micrometer spatial resolution were achieved by scanning of the focused laser beam. These structures were constructed in SiO₂/TiO₂ glass films by a sol–gel method. The sol–gel method demonstrated that Au dots microarray are fabricated at any position by two-photon absorption in the glass. The results show the utility of a two-photon absorption technique in the fabrication of complicated patterns with metal particles.     

Flow imaging by use of femtosecond-laser-induced two-photon fluorescence

A novel technique is demonstrated for the imaging of turbulent flows in which a single window to the flow is the only optical access required. A femtosecond laser is used to excite two-photon fluorescence in a disodium-fluorescein-seeded water jet. The fluorescence signal is generated at only the focal point of the laser because of the highly nonlinear nature of the two-photon absorption, and it is collected in a direction counterpropagating to the excitation beam. Tight focusing of the laser is used to limit the probe volume, and the two-dimensional mean and rms concentration images are collected by raster scanning the laser.     

Measurement of the third order nonlinear optical coefficients of GaP and chirp parameter of laser pulse

The spectral resolved femtosecond pump-probe experiment is applied to measure the third order nonlinear refractive index coefficient, two-photon absorption coefficient of GaP crystal, and the chirp parameter of the input laser pulses. The results show that nonlinear refractive index coefficient is 2× 10-18 m2/W, twophoton absorption coefficient is 2× 10-11 m/W at wavelength of 783.5 nm, and the chirp parameter of laser pulse is l× 1025 s-2. Furthermore, the mechanism of nonlinear refraction due to two-photon absorption in GaP crystal and experimental results are discussed.     

Nonlinearly limited saturable-absorber mode locking of an erbium fiber laser

We describe an erbium fiber laser that is passively mode locked by a novel, precision antireflection-coated semiconductor saturable-absorber mirror that incorporates an additional two-photon absorber. It is shown that passive mode locking evolves from a Q-switching instability. The results are achieved by use of saturable absorbers that provide a large (15%) nonlinear (saturable) loss. Exploiting two-photon absorption can substantially reduce the peak power of the Q-switched pulses, which results in improved reliability of the laser. Moreover, two-photon absorption can be used to produce an optimal stability range for saturable-absorber mode locking.     

Methods of measuring the nonlinear-optical coefficients of the refractive index of nonlinear media

A cousistent analysis of a method of measuring the coefficient n ₂ of the Kerr nonlinearity and the two-photon absorption coefficient in presented. The method is based on the study of the dependence of the nonlinear transmittance with respect to the far-field axial intensity of the laser beam on the position of the layer of the nonlinear medium on the z (longitudinal) coordinate of this beam (z scanning). The possibility for the measurement of n ₂ and the two-photon (multiphoton) absorption coefficient based on the study of the far-field variations in the spatial profile of the beam having passed through the nonlinear medium is also analyzed. The calculations prove the efficiency of the new method for measuring n ₂ and the two-photon (multiphoton) absorption coefficient.     

Investigation of optical nonlinearities in Pd(po)2 by Z-scan technique

With nanosecond scale at a 532 nm wavelength, we firstly measured the nonlinear optical absorption and refraction coefficients of Pd(po)₂ complex by using Z-scan technique, here Hpo=1-hydioxy-2-pyridone. We describe an empirical expression for the case when nonlinear refraction is accompanied by nonlinear absorption to separately evaluate the nonlinear refraction and the nonlinear absorption by performing straightforward measurements with the aperture removed. The nonlinear optical response of Pd(po)₂ was determined by the linear decreasing irradiance-dependence. The nonlinear absorption originates from the near resonant two-photon absorption while the mechanism of the nonlinear refraction is the near resonant two-photon absorption transition enhancement. The linear increasing dependences of the optical nonlinearities on the incident irradiance arise from the population redistribution due to the near resonant two-photon absorption.     

Picosecond Z-scan study of bound electronic Kerr effect in LiNbO3 crystal associated with two-photon absorption

3 crystal have been measured using Z-scan technique with picosecond pulses at 532 nm. The nonlinear absorption coefficient and nonlinear refractive index are determined to be 2.5×10^-10 cm/W and 5.3×10^-15 cm²/W, respectively. Both sign and magnitude of the measured refractive nonlinearity are considerably different from the reported Z-scan results in LiNbO₃ obtained with cw laser beam at 514 nm. The nonlinearities in LiNbO₃ induced by 532 nm picosecond pulses are believed to be mainly due to two-photon absorption and bound electronic Kerr effect associated with the two-photon absorption. Received: 4 July 1996     

Rapid pulse shaping with homodyne detection for measuring nonlinear optical signals

We have designed a common-mode interferometric acousto-optic pulse shaper that is capable of shaping individual pulses differently from a mode-locked laser. The design enables the measurement of weak nonlinear optical signals such as two-photon absorption and self-phase modulation at megahertz rates. The experimental apparatus incorporates homodyne detection as a means of resolving the phase of the detected signals. The fast data acquisition rate and the ability to perform measurements in scattering media make this experimental apparatus amenable to imaging applications analogous to measurements of two-photon fluorescence using a mode-locked laser.     

Nonlinear optics of nontoxic nanomaterials

We studied the linear and nonlinear optical properties of halloysite nanotubes using Z-scan technique. Halloysite is alumina silicate clay rolled into 50 nm diameter hollow cylinders, where the silica layer is at the outer surface of the tube and alumina layer is in the inner surface. Optical absorption spectra show an absorption peak around 600 nm. Open aperture Z-scan measurements using 3 ns laser pulses at 532 nm reveal two-photon induced absorption. The closed aperture Z-scan indicates a positive nonlinear refractive index. As these nanotubes are nontoxic and biocompatible, they have advantages over conventional carbon nanotubes for biomedical applications.     

Nonlinear optical parameters and optical limitation in cobalt-doped polyvinylpyrrolidone solutions

Nonlinear optical parameters (nonlinear refractive indices and nonlinear absorption coefficients) of solutions of polyvinylpyrrolidone doped by cobalt to various concentrations are measured at the lasing and second-harmonic wavelengths of a picosecond Nd:YAG laser (λ=1064 and 532 nm, respectively, and τ=35 ps). Data on optical limitation in these solutions are presented. The absence of nonlinear absorption in the IR spectral range and its significant effect in the visible range are demonstrated. Optical limitation at a wavelength of 1064 nm is related to defocusing, whereas at 532 nm, this effect is caused by two-photon absorption and partially by inverse saturated absorption and defocusing. Nonlinear optical parameters of metal-polymer complexes are reported.     

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.     

Orientation of the AD-1 azo-dye molecules in solid nanostructured films upon the two-photon excitation

The orientation of the AD-1 azo-dye molecules in solid nanostructured films is studied upon the nonlinear excitation using femtosecond laser pulses. A significant dichroism resulting from the irradiation is due to the two-photon absorption. The optical anisotropy induced by the two-photon absorption is proven to be related only to the reorientation of the azo-dye molecules and is not caused by alternative effects (e.g., photobleaching).     

Polarization control of multi-photon absorption under intermediate femtosecond laser field

It has been shown that the femtosecond laser polarization modulation is a very simple and well-established method to control the multi-photon absorption process by the light–matter interaction. Previous studies mainly focused on the multiphoton absorption control in the weak field. In this paper, we further explore the polarization control behavior of multiphoton absorption process in the intermediate femtosecond laser field. In the weak femtosecond laser field, the secondorder perturbation theory can well describe the non-resonant two-photon absorption process. However, the higher order nonlinear effect(e.g., four-photon absorption) can occur in the intermediate femtosecond laser field, and thus it is necessary to establish new theoretical model to describe the multi-photon absorption process, which includes the two-photon and four-photon transitions. Here, we construct a fourth-order perturbation theory to study the polarization control behavior of this multi-photon absorption under the intermediate femtosecond laser field excitation, and our theoretical results show that the two-photon and four-photon excitation pathways can induce a coherent interference, while the coherent interference is constructive or destructive that depends on the femtosecond laser center frequency. Moreover, the two-photon and fourphoton transitions have the different polarization control efficiency, and the four-photon absorption can obtain the higher polarization control efficiency. Thus, the polarization control efficiency of the whole excitation process can be increased or decreased by properly designing the femtosecond laser field intensity and laser center frequency. These studies can provide a clear physical picture for understanding and controlling the multi-photon absorption process in the intermediate femtosecond laser field, and also can provide a theoretical guidance for the future experimental realization.     

Two-photon absorption in V2O5 single crystals with Q-switched ruby laser pulses

New experimental results concerning the nonlinear absorption of V₂O₅ single crystals are reported. A Q-switched ruby laser have been used to measure the two-photon absorption coefficient at 694.3 nm. The results are analysed and interpreted with respect to the second-order attenuation of the light propagating through a plane-parallel medium.