Large and Ultrafast Third-Order Nonlinear Optical Properties of Ge-S Based Chalcogenide Glasses

We report ultrafast third-order nonlinear optical （NLO） properties of several chalcogenide glasses GeSx （x = 1.8, 2.0, 2.5） measured by femtosecond time-resolved optical Kerr gate technique at 82Ohm. The third-order nonlinear susceptibility of GeS1.8 glass is determined to be as large as 1.41 ×10^-12 esu, which is the maximum value of the third order nonlinear susceptibility Х^（3） for the three compositions investigated. The symmetric Gauss profiles of optical Kerr signals reveal the nature of ultrafast nonlinear response of these samples, which are originated from the ultrafast polarization of the electron clouds. By detailed microstructural analysis of these glasses based on the chain-crossing model （CCM） and the random-covalent-network model （RCNM）, it can be concluded that Х^（3） value of GeSx glasses can be enhanced greatly by S-S covalent bonds or S3 Ge-GeS3 ethane-l＆e units.     

Third-Order Nonlinear Optical Properties of a Series of Polythiophenes

The third-order nonlinear optical properties of a series of polythiophenes are investigated with the Z-scan method under picosecond pulse laser irradiation at 532nm. The copolymers exhibit a good nonlinear response： large nonlinear refraction coefficients without nonlinear absorption. The signs of nonlinear refraction coefficients are positive, which are opposite to the negative signs of the polythiophene reported before. The mechanism accounting for the process of nonlinear refraction under pulse laser excitation is analyzed from the viewpoint of the electrondonor/acceptor units of polythiophenes. Moreover, changes of nonlinearity according to the lengths of main chains in polythiophene molecules are discussed.     

Large Third-Order Optical Nonlinearity of a Novel Copper Phthalocyanine--Ferrocene Dyad

Third-order optical nonlinearity of a novel copper phthalocyanine-ferrocene dyad is measured by femtosecond forward degenerate four-wave mixing （DFWM） technique at 800 nm. The second-order hyperpolarizability of the novel copper phthalocyanine-ferrocene dyad is measured to be 1.74 ×10^-30 esu. This large and ultrafast thirdorder optical nonlinear response is mainly enhanced by the formation of intramolecular charge-transfer which can enhance the delocalized movements of the large π-electrons in the molecules.     

Cleavage Luminescence from Cleaved Indium Phosphide

We outline the experiments performed to gain further information about the structure and properties of cleaved InP surfaces. The experiments involved detecting the luminescence produced after cleaving thin InP plates within a high vacuum, by a process of converting the luminescence to an electrical signal which could be amplified and measured accurately. The experimental results show that the detected luminescence durations from cleaved InP are usually only about 10μs. It is believed that this time represents the time of travel of the crack with the actual recombination time being much shorter. Strong signals could also be picked up from cleaved InP in air.     

Enhancement of Second- and Third-Order Nonlinear Optical Susceptibilities in Magnetized Semiconductors

Using electromagnetic treatment, an expression of effective nonlinear optical susceptibility χe [= χe^（2） ＋ χe^（3） E] is obtained for Ⅲ-Ⅴ semiconducting crystals in an applied transverse dc magnetic fieM under off-resonant transition regime. The origin of nonlinear interaction lies in nonlinear polarization arising from the crystal properties such as piezoelectricity and electrostriction. Numerical estimates have been made by a representative n-InSb crystal at 77K duly irradiated by a pulsed 10.6-μm CO2 laser under off-resonant transition regime. Efforts are dedicated to optimizing doping level and externally applied dc magnetic field to achieve maximum χe^（2） and χ3^（3）. The results are found to be in good agreement with the available literature. The analysis shows that χe^（2） and χe^（3） can be significantly enhanced in doped Ⅲ-Ⅴ semiconductors by the proper selection of doping concentration and dc magnetic field, which confirms its potential as a candidate material for the fabrication of nonlinear optical devices.     

Nonlinear Optical Properties of Novel Polymeric Rare Earth Phthalocyanine Studied Using Picosecond Z-Scan Technique

Three novel tri-dimensional phthalocyanine polymers, with lanthanum （LaPPc）, gadolinium （GdPPc） and ytterbium （YbPPc） as centric atoms, have been synthesized from a tetranuclear phthalonitrile. Third-order optical nonlinearities of these compounds in DMF solution are measured by a picosecond Z-sacn technique at 532 nm. It is found that all the compounds show reverse saturation absorption and nonlinear self-focus refraction effect. The second-order molecular hyperpolarizabilities are calculated to be 1.82×10^-23, 1.48×10^-23 and 1.45×10^-23 esu for LaPPc, GdPPc and YbPPc, respectively. The differences among their nonlinear optical properties are attributed to the special tri-dimensional structure and the variation in rare earth atoms.     

Third-Order Optical Nonlinearity in Novel Porphyrin Dimers

We investigate the third-order optical nonlinearities in four novel porphyrin dimers （dimers A to D） and a monomeric porphyrin H2 CPTPP measured by using the single-beam z-scan technique with a pulsed Q-switched Nd：YAG nanosecond laser at 532nm. All the samples show strong excited state absorption （ESA） and high value of Х^（3） in the ns domain at this wavelength. We perform a comparison between dimer A and its monomer H2 CPTPP in their third-order optical nonlinearity, and discuss the relationships between the values of Х^（3） and the different bridging groups for all the dimers.     

Optical phonon frequencies and damping in AlAs, GaP, GaAs, InP, InAs and InSb studied by oblique incidence infrared spectroscopy

The transverse (TO) and longitudinal (LO) optical phonons in AlAs, GaP, GaAs, InP, InAs and InSb have been measured at room temperature by infrared spectroscopy using an oblique incidence reflectance method. The spectra obtained were then fitted using a novel approach to determine the TO and LO phonon frequencies and damping. The results obtained are found to be more precise than in earlier reflectivity measurements using near-normal angles of incidence and provide information on the damping of both phonons. Apart from the GaAs LO mode, the observed damping parameters are found to be quite different from those predicted by theory. From these results the Lowndes condition governing the relative magnitudes of the TO and LO phonon line widths is found to be violated for all these zincblende semiconductors.     

Effects of Coupling Lens on Optical Refrigeration of Semiconductors

Optical refrigeration of semiconductors is encountering efficiency difficulties caused by nonradiative recombination and luminescence trapping. A commonly used approach for enhancing luminescence efficiency of a semiconductor device is coupling a lens with the device. We quantitatively study the effects of a coupling lens on optical refrigeration based on rate equations and photon recycling, and calculated cooling emciencies of different coupling mechanisms and of different lens materials. A GaAs/GalnP heterostructure coupled with a homo-epitaxial GalnP hemispherical lens is recommended.     

Multilayer Au/TiO2Composite Films with Ultrafast Third-Order Nonlinear Optical Properties

We report on the ultrafast third-order optical nonlinearity in multilayer Au/TiO2 composite films fabricated on quartz substrates by pulsed laser deposition technique. The linear optical properties of the films are determined and optical absorption peaks due to surface plasmon resonance of Au particles are observed at about 590hm. The third-order optical nonlinearities of the films are investigated by z-scan method using a femtosecond laser （50 fs） at the wavelength of 800 nm. The sample showed fast nonlinear optical responses with nonlinear absorption coefficient and nonlinear refractive index being -3.66 × 10^-10 m/W and -2.95 × 10^-17 m^2/W, respectively. The results also show that the nonlinear optical effects increase with the increasing Au concentration in the composite films.     

Nonlinear Optical Properties of Novel C60 Derivatives under Picosecond Laser Excitation

We investigate the third-order nonlinear optical properties of six novel fullerene derivatives under picosecond laser excitation by Z-scan technique. The experimental results reveal that all the derivatives have very large nonlinear absorption coefficient under 532 nm pulses excitation and great third-order nonlinear refraction index under 1064 nm pulses excitation. The molecular second hyperpolarizabilities are obtained from the experimental results.     

Synthesis and red-shifted photoluminescence of single-crystalline ZnO nanowires

Local-oriented single-crystalline ZnO nanowires have been synthesized in large scale by a simple microemulsion method in the presence of sulfonate-polystyrene (S-PS) and dodecyl benzene sulfonic acid sodium salt (DBS). The as-prepared product is characterized by using X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), high-resolution TEM (HRTEM), infrared (IR) spectra and photoluminescence (PL) spectrum. The nanowires exhibit a local congregation and preferentially grow along the [0 0 2] facet. FT-IR spectrum indicates that S-PS is adsorbed on the surface of ZnO nanowires. The PL spectrum shows evidently red-shifted ultraviolet (UV) emission.     

Pulse Temporal Cleaner Based on Nonlinear Ellipse Rotation by Using BK7 Glass Plate

We report a new pulse cleaning technique to enhance the contrast ratio of intense ultra-short laser pulses. A pulse temporal cleaner based on nonlinear ellipse rotation by using BK7 glass plate is developed, and a contrast ratio improvement of two orders of magnitude for the milli-joule level femtoseeond input pulses is demonstrated, the total transmission effieiency of the pulse cleaner is 16. 7%.     

Effect of ZnS shell on the Raman spectra from CdSe nanorods

We investigated the influence of an epitaxially grown ZnS shell on the phonon spectra of CdSe nanorods of different sizes. The CdSe related Raman peaks shift with addition of a ZnS shell. The longitudinal optical phonon shifts slightly due to strain and the low‐energy shoulder shifts stronger, which can be explained within a model for surface optical phonons. (© 2007 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

Growth of AlN nanostructures by a rapid thermal process

Aluminum nitride nanorods were grown during rapid thermal annealing of multi-layered Al₂S₃ /BaS thin films. Depending on the thickness ratio between the BaS and Al₂S₃ layers, nanowires or straight nanorods were obtained. Typical dimensions for the nanorods were a diameter in the range of 50-100 nm and a length of 2-5 μm. The nanostructures are formed upon annealing at a relatively low temperature of 900 ^°C when aluminum evaporates from the thin film, but remains trapped between the thin film surface and the Si wafer, which is used as a support during the annealing. The nitrogen is provided by N₂ gas flushed through the annealing chamber. High-resolution transmission electron microscopy showed crystalline, wurtzite-structured AlN nanorods. The growth mechanism in terms of thin film composition, annealing parameters and the role of catalysts is discussed.     

Third-Order Nonlinear Optical Susceptibility of Special Asymmetric Quantum Wells

A detailed procedure for the calculation of the third-harmonic-generation susceptibility tensor is given in special asymmetric quantum wells, and an analytic formula for the third-harmonic-generation susceptibility is obtained by the compact density matrix approach and the iterative procedure. Finally, the numerical results are presented for typical GaAs/AlGaAs asymmetric quantum wells. The calculated results show that the origin of the large thirdharmonic-generation susceptibility is due to the increase in asymmetry of the quantum well.     

Effective Dielectric Response of Nonlinear Composites of Coated Metal Inclusions

The effective dielectric response of the composites in which nondilute coated metal particles are randomly embedded in a linear host is investigated. Two types of coated particles are considered, one is that the core is nonlinear, the other is that the shell is nonlinear. We derive general expressions for the effective linear dielectric function and the effective third-order nonlinear susceptibility, and take one step forward to perform numerical calculations on the coated metal/dielectric composites. Numerical results show that the effective linear and nonlinear dielectric responses can be greatly enhanced near the surface plasmon resonant frequency. Moreover, the resonant peaks are found within a range from 0.46ωp to 0.57ωp for spherical particles and from 0.59ωp to 0.70ωp for cylindrical inclusions. In the frequency region, the resonant peak can achieve the maximum, according to an optimal structural parameter and volume fraction. The resonant frequency exhibits a redshift with the increasing structural parameter k or volume fraction f or dimensionality factor D.     

Optical limiting in cobalt-doped polyvinylpyrrolidone

The results of optical limiting investigations of cobalt-doped polyvinylpyrrolidone solutions are presented. The optical limiting studies have shown that this process is due to self-defocusing at the wavelength of 1064 nm and also due to reverse saturable absorption and self-defocusing at the wavelength of 532 nm. The results of measurements on the non-linear optical characteristics of organometallic complexes are presented. Received: 10 July 2001 / Revised version: 15 October 2001 / Published online: 29 November 2001     

Effect of Ag Nanoparticles on Optical Properties of R6G Doped PMMA Films

The composite PMMA films containing Ag nanoparticles and rhodamine 6G are prepared. We investigate the fluorescence properties and nonlinear optical properties of R6G/PMMA films influenced by Ag nanoparticles. The fluorescence enhancement factor is about 3.3. The corresponding nonlinear refractive index is measured to be -2.423 ×10^-8 esu using the Z-scan technique, which is much enhanced compared with the R6G/PMMA film. The results indicate that these enhancements are attributed to surface plasmon resonance of Ag nanoparticles.     

Quantum-chemistry simulations of second-harmonic and sum-frequency generation of organic layers

By using quantum-chemistry approaches, the second-order nonlinear optical responses of molecules and two-dimensional molecular arrays containing the p-nitroaniline chromophore are evaluated in order to highlight key features of the simulation of the second-harmonic and sum-frequency generation spectra of organic layers. For the electronic component, which dominates the second-harmonic generation response and which constitutes the weakly frequency-dependent background contribution to the vibrational sum-frequency generation phenomenon, the time-dependent Hartree–Fock scheme based on the semi-empirical AM1 parameterization is suitable for predicting the microscopic responses as well as for accounting for the surrounding effects within a simple multiplicative scheme. For the vibrational resonant part of the sum-frequency generation response, ab initio density functional theory approaches turn out to be necessary for locating the resonances and estimating their intensities. Received: 16 October 2001 / Published online: 29 May 2002