Nonlinear optical response of nc-Si-SiO2 films studied with femtosecond four-wave mixing technique

Nonlinear optical properties of silicon nanocrystals (nc-Si) embedded in SiO2 films are investigated using time-resolved four-wave mixing technique with a femtosecond laser. the off-resonant third-order nonlinear susceptibility chi((3)) is observed to be 1.3 x 10(-10) esu at 800 nm. The relaxation time of the film is fast as short as 50 fs. The off-resonant nonlinearity is predominantly electronic in origin and enhanced due to quantum confinement.

Nonlinear Optical Properties of AI-Doped nc-Si-SiO_2 Composite Films

The nonlinear optical properties of Al-doped nc-Si-SiO_2 composite films have been investigated using the time-resolved four-wave mixing technique with a femtosecond laser. The off-resonant third-order nonlinear susceptibility is observed to be 1.0 × 10~(-10) esu at 800nm. The relaxation time of the optical nonlinearity in the films is as short as 60fs. The optical nonlinearity is enhanced due to the quantum confinement of electrons in Si nanocrystals embedded in the SiO_2 films. The enhanced optical nonlinearity does not originate from Al dopant because there are no Al clusters in the films.

Preparation and nonlinear optical properties of ultrathin composite films containing both a polyoxometalate anion and a binuclear phthalocyanine

An ultrathin composite film containing both polyoxometalate anion [PMo12O40](3-) ( PMo12) and a planar binuclear phthalocyanine, bi-CoPc, has been prepared by the electrostatic layer-by-layer self-assembly method. UV-vis measurements revealed regular film growth with each four-layer {PMo12/bi-CoPc/PSS/PAH} adsorption. The lm structure was characterized by small-angle X-ray reflectivity measurements, X-ray photoelectron spectra, and AFM images. The nanothick film shows a third-order nonlinear optical response of chi((3)) = 4.21 x 10(-12) esu. Experimental investigations also indicate that the combination of polyoxometalate anions [PMo12O40](3-) with the phthalocyanine bi-CoPc in multilayer films can enhance the third-order NLO susceptibility and modify the third-order NLO absorption of bi-CoPc.

The role of Li-O bonds in calculations of nonlinear optical coefficients of LiXO3-type complex crystals

The second-order nonlinear optical (NLO) tenser coefficients of LiXO3 (X = I; Nb or Ta) type complex crystals have been calculated using the chemical bond theory of complex crystals. Contributions of each type of bond to the total second-order NLO coefficient d(ij) and the linear susceptibility X are quantitatively determined. All tensor values thus calculated are in good agreement with experimental data. The Li-O bonds are found to be an important group in the contributions to the total NLO tenser coefficient, especially for those in LiNbO3 and LiTaO3. The importance of Li-O bonds depends on the environment of Li atom in these crystals.

Bond-charge calculation of nonlinear optical susceptibilities of LiXO3 type complex crystals

Second order nonlinear optical (NLO) tensor coefficients of LiXO3 (X = I, Nb, Ta) type crystals have been evaluated on the basis of the dielectric theory of complex crystals and the modified bond charge model. The current method is capable of calculating single bond contributions to the total second order NLO susceptibility. The tenser values thus calculated agree well with experimental data. By introducing the subformula equation and the concept of the effective charge of one valence electron, we are able to successfully treat such complex crystals as LiXO3 type compounds. In addition, the bond charge expression is modified to a more reasonable form for complex crystals. (C) 1998 Elsevier Science B.V.

The effect of stoichiometry on nonlinear optical properties of LiNbO3

From the chemical bond viewpoint, second-order nonlinear optical (NLO) tensor coefficients of LiNbO3 have been investigated. The single-bond contributions to the second-order NLO susceptibility and the linear susceptibility were determined. The tensor values thus calculated are in good agreement with experimental data. Based on theoretical results of LiNbO3 with Li/Nb = 1, we also have calculated linear and nonlinear optical properties of nonstoichiometric samples with Li/Nb < 1. In the calculation, we find that the Li-O bond is an important type of chemical bond in these LiNbO3 samples, which have large NLO contributions to the total nonlinearities. The refractive indices and second-order NLO tensor coefficients have been determined as a function of the stoichiometry.

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.

Nonlinear optical properties and thermal stability of the poled polymer NTAB/PEK-c

Films of high glass' transition temperature polymer polyetherketone doped with chromophore 2,2'[4-[(5-nitro-2-thiazolyl)azophenyl]-amino]-bisethanol NTAB) were prepared, poled by the corona-onset poling setup which includes a grid voltage making the surface-charge distribution uniform at elevated temperature. The thickness of the films was measured by the Model 2010 Prism Coupler system. Second harmonic generation d(33) was measured by the second harmonic generation method, and the d33 is 38.12 pm/V at 1064 nm under the absorption correction. The nonlinear optical activity maintains is 80% of its initial value. (C) 2002 Elsevier Science B.V. All rights reserved.

Side radical influence on the nonlinear optical properties and thermal stability of poled polymer films

Films of polyetherketone doped with the chromophores Disperse Red 1 (DR1) and Disperse Red 13 (DR13) were prepared by spin-coating method. By the in situ Second-harmonic Generation (SHG) signal intensity measurement, the optimal poling temperatures were obtained. For the investigated polyetherketone polymer doped with DR1 (DR1/PEK-c) and polyetherketone polymer doped with DR13 (DR13/PEK-c) films, the optimal poling temperatures were 150degreesC and 140degreesC, respectively. Under the optimal poling conditions, the high second-order nonlinear optical coefficient chi(33)((2)) = 11.02 pm/V has been obtained for the DR1/PEK-c; and for DR13/PEK-c at the same conditions the coefficient is 17.9 pm/V. The SHG signal intensity DR1/PEK-c could maintain more than 80% of its initial value when the temperature was under 100degreesC, and the SHG signal intensity of the DR13/PEK-c could maintain more than 80% of its initial value when the temperature was under 135degreesC. (C) 2002 Kluwer Academic Publishers.

Thermally stable chromophores for nonlinear optical applications

Three thermal organic second-order nonlinear optical chromophores were synthesized. The decomposition temperature was determined by DSC, and the absorption spectra was measured. The second-order polarizabilities at zero energy and the dispersion of second-order polarizabilities were measured by solvatochromic method. (C) 2002 Elsevier Science Ltd. All rights reserved.

Investigation on the nonlinear optical properties of the DCNP/PEK-c guest-host polymer films

The polyetherketone (PEK-c) guest-host polymer thin films doped with 3-(1,1-dicyanothenyl)-1-phenyl-4,5-dihydro-1H-pryazole (DCNP) were prepared. The polymer films were investigated with in situ second-harmonic generation (SHG) measurement. The corona poling temperature was optimized by the temperature dependence of the in situ SHG signal intensity under the poling electric field applying. The temporal and temperature stability of the second-order properties of the poled polymer film were measured by the in situ SHG signal intensity probing. The second-order NLO coefficient chi ((2))(33) = 32.65 pm/V at lambda = 1064 nm was determined by using the Makel fringe method after poling under the optimal poling condition. The dispersion of the NLO coefficient of the guest-host polymer system was determined by the measured value of chi ((2))(33) at 1064 nm and the two-level model.

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.

Refractive index dispersion measurement on nonlinear optical polymer using V-prism refractometer

By using V-prism refractometer, the refractive indices of a polyetherketone (PEK-c) guest-host polymer system were measured with the polymer in solutions. The Lorenz-Lorentz local field formalism was used in the calculation of the refractive indices of the polymers from the measured indices of the polymer solutions and the pure solvent by using V-prism refractometer. The refractive index dispersions of the polymers were obtained by fitting the measured indices of the polymers to Sellmeyer equation. The method allows for an accuracy in index of 0.7% in the determination of the polymer indices. In addition, a large difference between the indices of the polymer and the solvent, and a higher polymer volume fraction in the measured polymer solution are favorable for a high accuracy. (C) 2000 Elsevier Science Ltd. All rights reserved.