Effect of the electrostatic interactions of chromophores on the macroscopic second-order nonlinear optical properties of the polymer films

The polyetherketone (PEK-c) guest-host system thin films doped with 3-(1,1-dicyanothenyl)-1-phenyl-4,5-dihydro-1H-pryazole (DCNP) were prepared. Their second-order nonlinear optical (NLO) coefficients chi(33)((2)) were measured by using Maker fringe method for the polymer films doped with different weight percents of DCNP. Experimental results indicate that the second-order NLO properties of the poled polymer films could decrease with the chromophore loading increasing when the chromophore loading reaches a fairly high level. In this paper, the relationship between the macroscopic second-order NLO coefficient and the chromophore number density was modified under considering the role of the electrostatic interactions of chromophores in the polymer film. According to the modified relationship, the macroscopic second-order NLO coefficient is no longer in direct proportion with the chromophore number density in the polymer film. The effect of the electrostatic interactions of chromophores on second-order NLO properties was discussed. The attenuation of the macroscopic second-order NLO activity can be demonstrated by the role of the chromophore electrostatic interactions at high loading of chromophore in the polymer systems.

Two-photon asymmetric color-locking second-order stochastic correlation of attosecond polarization beats

Based on the phase-conjugation polarization interference between two two-photon processes, we theoretically investigated the attosecond scale asymmetry sum-frequency polarization beat in four-level system (FASPB). The field correlation has weak influence on the FASPB signal when the laser has narrow bandwidth. Conversely, when the laser has broadband linewidth, the FASPB signal shows resonance-nonresonance cross correlation. The two-photon signal exhibits hybrid radiation-matter detuning terahertz; damping oscillation, i.e., when the laser frequency is off resonance from the two-photon transition, the signal exhibits damping oscillation and the profile of the two-photon self-correlation signal also exhibits zero time-delay asymmetry of the maxima. We have also investigated the asymmetry of attosecond polarization beat caused by the shift of the two-photon self-correlation zero time-delay phenomenon, in which the maxima of the two two-photon signals are shifted from zero time-delay point to opposite directions. As an attosecond ultrafast modulation process, FASPB can be intrinsically extended to any level-summation systems of two dipolar forbidden excited states.

Second-Order Raman Scattering from n- and p-Type 4H-SiC

The results of second-order Raman-scattering experiments on n- and p-type 4H-SiC are presented,covering the acoustic and the optical overtone spectral regions.Some of the observed structures in the spectra are assigned to particular phonon branches and the points in the Brillouin zone from which the scattering originates.There exists a doublet at 626/636cm-1 with energy difference about 10cm-1 in both n- and p-type 4H-SiC,which is similar to the doublet structure with the same energy difference founded in hexagonal GaN,ZnO, and AlN.The cutoff frequency at 1926cm-1 of the second-order Raman is not the overtone of the A1(LO) peak of the n-type doping 4H-SiC,but that of the undoping one.The second-order Raman spectrum of 4H-SiC can hardly be affected by doping species or doping density.

Thermally stable interpenetrating polymer networks for second-order nonlinear optical materials

We report several kinds of interpenetrating polymer networks (IPNs) with nonlinear optical (NLO) properties. DMA spectra show that the two components of the IPNs have good compatibility with each other. The NLO materials have good optical transparency. The thermal stability of alignment was improved and the poled order remained very high. (C) 1999 John Wiley & Sons, Inc.

A ZINDO-SOS study on the nonlinear second-order optical properties of substituted silanes series molecules

On the basis of ZINDO methods,according to the sum - over - states( SOS) expression, we divise the program for the calculation of nonlinear second - order optical susceptibilities beta(ijk) and study how the different substituents on the phenyl ring attached to the atom silicon influence or; the nonlinear second - order optical properties for substituted silanes series molecules. The property of (CH3)(3)Si is Studied particularly. The effect of length of silica chains on the calculated beta values is studied too. The regularity summarized from calculated results has been explained micromechanically.

A theoretical study on the nonlinear optical second-order properties of azobenzene series molecules

On the basis of AM1 and INDO/CI methods, we devise the program for the calculation of nonlinear second-order optical susceptibilities beta(ijk) and perform systematic theoretical studies on the nonlinear optical second-order properties of azobenzene series molecules, i. e. on the basis of [GRAPHICS] we induced different donors on the left side of phenyl ring, and different accepters on the right side of phenyl ring, and examined the rule of beta variation. The regularity summarized from the calculated results has been explained micromechanically. Finally, a molecule having a big nonlinear second-order optical susceptibility has been designed.

Second-order Stokes solutions for internal waves in three-layer density-stratified fluid

In this paper, internal waves in three-layer stratified fluid are investigated by using a perturbation method, and the second-order asymptotic solutions of the velocity potentials and the second-order Stokes solutions of the associated elevations of the interfacial waves are presented based on the small amplitude wave theory. As expected, the first-order solutions are consistent with ordinary linear theoretical results, and the second-order solutions describe the second-order modification on the linear theory and the interactions between the two interfacial waves. Both the first-order and second-order solutions derived depend on the depths and densities of the three-layer fluid. It is also noted that the solutions obtained from the present work include the theoretical results derived by Umeyama as special cases.

Second-order solutions for random interfacial waves under steady uniform currents

In the present research, the study of Song (2004) for random interfacial waves in two-layer fluid is extended to the case of fluids moving at different steady uniform speeds. The equations describing the random displacements of the density interface and the associated velocity potentials in two-layer fluid are solved to the second order, and the wave-wave interactions of the wave components and the interactions between the waves and currents are described. As expected, the extended solutions include those obtained by Song (2004) as one special case where the steady uniform currents of the two fluids are taken as zero, and the solutions reduce to those derived by Sharma and Dean (1979) for random surface waves if the density of the upper fluid and the current of the lower fluid are both taken as zero.

Representation of microscale ocean wavenumber spectrum correct to the second order

In this paper, the analytical representations of four wave source functions in high-frequency spectrum range are given on the basis of ocean wave theory and dimensional analysis, and the perturbation method is used to solve the governing equations of ocean wave high-frequency spectrum on the basis of the temporally stationary and locally homogeneous scale relations of microscale wave. The microscale ocean wavenumber spectrum correct to the second order has an explicit structure, its first order part represents the equilibrium between different source functions, and its second order part represents the contribution of microscale wave propagation.

Statistical distribution of wave-surface elevation for second-order random directional ocean waves in finite water depth

Based on the second-order random wave solutions of water wave equations in finite water depth, a statistical distribution of the wave-surface elevation is derived by using the characteristic function expansion method. It is found that the distribution, after normalization of the wave-surface elevation, depends only on two parameters. One parameter describes the small mean bias of the surface produced by the second-order wave-wave interactions. Another one is approximately proportional to the skewness of the distribution. Both of these two parameters can be determined by the water depth and the wave-number spectrum of ocean waves. As an illustrative example, we consider a fully developed wind-generated sea and the parameters are calculated for various wind speeds and water depths by using Donelan and Pierson spectrum. It is also found that, for deep water, the dimensionless distribution reduces to the third-order Gram-Charlier series obtained by Longuet-Higgins [J. Fluid Mech. 17 (1963) 459]. The newly proposed distribution is compared with the data of Bitner [Appl. Ocean Res. 2 (1980) 63], Gaussian distribution and the fourth-order Gram-Charlier series, and found our distribution gives a more reasonable fit to the data. (C) 2002 Elsevier Science B.V. All rights reserved.

Second-order solutions for random interfacial waves in N-layer density-stratified fluid with steady uniform currents

In the present paper, the random inter facial waves in N-layer density-stratified fluids moving at different steady uniform speeds are researched by using an expansion technique, and the second-order a symptotic solutions of the random displacements of the density interfaces and the associated velocity potentials in N-layer fluid are presented based on the small amplitude wave theory. The obtained results indicate that the wave-wave second-order nonlinear interactions of the wave components and the second-order nonlinear interactions between the waves and currents are described. As expected, the solutions include those derived by Chen (2006) as a special case where the steady uniform currents of the N-layer fluids are taken as zero, and the solutions also reduce to those obtained by Song (2005) for second-order solutions for random interfacial waves with steady uniform currents if N=2.

Second-order Stokes wave solutions for intefacial waves in three-layer stratified fluid with background current

In this paper, interfacial waves in three-layer stratified fluid with background current are investigated using a perturbation method, and the second-order asymptotic solutions of the velocity potentials and the second-order Stokes wave solutions of the associated elevations of the interfacial waves are presented based on the small amplitude wave theory, and the Kelvin-Helmholtz instability of interfacial waves is studied. As expected, for three-layer stratified fluid with background current, the first-order asymptotic solutions (linear wave solutions), dispersion relation and the second-order asymptotic solutions derived depend on not only the depths and densities of the three-layer fluid but also the background current of the fluids, and the second-order Stokes wave solutions of the associated elevations of the interfacial waves describe not only the second-order nonlinear wave-wave interactions between the interfacial waves but also the second-order nonlinear interactions between the interfacial waves and currents. It is also noted that the solutions obtained from the present work include the theoretical results derived by Chen et al (2005) as a special case. It also shows that with the given wave number k (real number) the interfacial waves may show Kelvin-Helmholtz instability.

Typability and Type Checking in the Second-Order Λ-Calculus Are Equivalent and Undecidable (Preliminary Draft)

We consider the problems of typability[1] and type checking[2] in the Girard/Reynolds second-order polymorphic typed λ-calculus, for which we use the short name "System F" and which we use in the "Curry style" where types are assigned to pure λ -terms. These problems have been considered and proven to be decidable or undecidable for various restrictions and extensions of System F and other related systems, and lower-bound complexity results for System F have been achieved, but they have remained "embarrassing open problems"[3] for System F itself. We first prove that type checking in System F is undecidable by a reduction from semi-unification. We then prove typability in System F is undecidable by a reduction from type checking. Since the reverse reduction is already known, this implies the two problems are equivalent. The second reduction uses a novel method of constructing λ-terms such that in all type derivations, specific bound variables must always be assigned a specific type. Using this technique, we can require that specific subterms must be typable using a specific, fixed type assignment in order for the entire term to be typable at all. Any desired type assignment may be simulated. We develop this method, which we call "constants for free", for both the λK and λI calculi.

A Direct Algorithm for the Type Interference in the Rank 2 Fragment of the Second--Order λ-Calculus

We study the problem of type inference for a family of polymorphic type disciplines containing the power of Core-ML. This family comprises all levels of the stratification of the second-order lambda-calculus by "rank" of types. We show that typability is an undecidable problem at every rank k ≥ 3 of this stratification. While it was already known that typability is decidable at rank ≤ 2, no direct and easy-to-implement algorithm was available. To design such an algorithm, we develop a new notion of reduction and show how to use it to reduce the problem of typability at rank 2 to the problem of acyclic semi-unification. A by-product of our analysis is the publication of a simple solution procedure for acyclic semi-unification.

First- and second-order phase transitions in the adlayer of biadipate on Au(111)

The adsorption of biadipate on Au(111) was studied by cyclic voltammetry and chronocoulometry. The biadipate adlayer undergoes a potential-driven phase transition. It is shown that the phase transition can be either of the first- or second-order depending on the biadipate concentration. At low surfactant concentrations, the first-order transition is characterised by a discontinuity in the charge density-potential curve and by the presence of very sharp peaks in the voltammetric response. At higher concentrations, these peaks are no longer observed but a discontinuity in the capacity curve is still noticeable, in agreement with a second-order transition. © the Owner Societies.