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.

Optimization and characterization of the guest-host polyetherketone polymer films for application in integrated optical devices

In order to optimize the loading of 3-(1, 1-dicyanothenyl)-1-phenyl-4, 5-dihydro-1H-pryazole (DCNP) in polyetherketone (PEK-c) guest-host polymer films, ten kinds of DCNP/PEK-c thin films, in which the weight per cent of DCNP changes from 5 to 50, were prepared. Their second-order nonlinear optical coefficients chi(33)((2)) at 1064 nm were measured by Using Maker fringe method after poling under the optimal poling condition. Their optical waveguide transmission losses were measured at 632.8 nm. Optimal weight per cent of the chromophore for the DCNP/PEK-c guest-host polymer system has been determined as about 20 for use in the integrated optical devices.

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.

Transient photoconductivity and its light-induced change of lightly boron-doped a-Si : H films

Transient photoconductivity and its light-induced change were investigated by using a Model 4400 boxcar averager and signal processor for lightly boron-doped a-Si : H films. The transient photoconductivities of the sample were measured at an annealed state and light-soaked states. The transient decay process of the photoconductivity can be fitted fairly well by a second-order exponential decay function, which indicates that the decay process is related with two different traps. It is noteworthy that the photoconductivity of the film increases after light-soaking. This may be due to the deactivity of the boron acceptor B-4(-), and thus some of the boron atoms can no longer act as acceptors and drives E-F to shifts upward. Consequently, the number of effective recombination centers may be reduced and so the photoconductivity increases.

Determination of the macroscopic optical properties for the NAEC/PEK-c guest-host polymer films

The polyetherketone (PEK-c) guest-host polymer films doped with (4'-nitro)-3-azo-9-ethyl-carbazole (NAEC) were prepared. The films were poled by corona-onset poling at elevated temperature (COPET). The orientational order parameter of the chromophores NAEC in poled polymer film was determined by measuring the absorption spectra of the films before and after being poled. By using the two-level model, the measured dispersion of the refractive index of the polymer film, and the dispersion of the first hyperpolarizability of chromophore NAEC, the dispersion of the macroscopic second-order nonlinear optical (NLO) and linear electrooptic (EO) coefficients was evaluated for the NAEC/PEK-c guest-host polymer film. (C) 2001 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.

Raman scattering of nanocrystalline silicon embedded in SiO2

Raman scattering of nanocrystalline silicon embedded in SiO2 matrix is systematically investigated. It is found that the Raman spectra can be well fitted by 5 Lorentzian lines in the Raman shift range of 100-600 cm(-1). The two-phonon scattering is also observed in the range of 600-1100 cm(-1) The experimental results indicate that the silicon crystallites in the films consist of nanocrystalline phase and amorphous phase; both can contribute to the Raman scattering. Besides the red-shift of the first order optical phonon modes with the decreasing size of silicon nanocrystallites, we have also found an enhancement effect on the second order Raman scattering, and the size effect on their Raman shift.

Linear and nonlinear intersubband optical properties in a step quantum well with an applied electric field

Within the framework of the effective-mass envelope-function theory, the field-dependent intersubband optical properties of a Al0.4Ga0.6As/Al0.2Ga0.8As/GaAs step quantum well are investigated theoretically based on the periodic boundary condition. A very large Stark shift occurs when the lowest subband electron remains confined to the small well while the higher subband electron confined to the big well. The optical nonlinearity in a step well due to resonant intersubband transition (ISBT) is analyzed using a density-matrix approach. The second-harmonic generation coefficient chi(2 omega)((2)) and nonlinear optical rectification chi(0)((2)) have also been investigated theoretically. The results show that the ISBT in a step well can generate very large second order optical nonlinearities, chi(0)((2)) and chi(2 omega)((2)) can be tuned by the electric field over a wide range.

Design of surface emitting distributed feedback quantum cascade laser with single-lobe far-field pattern and high outcoupling efficiency

A 7.8-mu m surface emitting second-order distributed feedback quantum cascade laser (DFB QCL) structure with metallized surface grating is studied. The modal property of this structure is described by utilizing coupled-mode theory where the coupling coefficients are derived from exact Floquet-Bloch solutions of infinite periodic structure. Based on this theory, the influence of waveguide structure and grating topography as well as device length on the laser performance is numerically investigated. The optimized surface emitting second-order DFB QCL structure design exhibits a high surface outcoupling efficiency of 22% and a low threshold gain of 10 cm(-1). Using a pi phase-shift in the centre of the grating, a high-quality single-lobe far-field radiation pattern is obtained.

On the acid-base stability of Keggin Al-13 and Al-30 polymers in polyaluminum coagulants

The acid-base stabilities of Al-13 and Al-30 in polyaluminum coagulants during aging and after dosing into water were studied systematically using batch and flow-through acid-base titration experiments. The acid decomposition rates of both Al-13 and Al-30 increase rapidly with the decrease in solution pH. The acid decompositions of Al-13 and Al-30 with respect to H+ concentration are composed of two parallel first-order and second-order reactions, and the reaction orders are 1.169 and 1.005, respectively. The acid decomposition rates of Al-13 and Al-30 increase slightly when the temperature increases from 20 to ca. 35 A degrees C, but decrease when the temperature increases further. Al-30 is more stable than Al-13 in acidic solution, and the stability difference increases as the pH decreases. Al-30 is more possible to become the dominant species in polyaluminum coagulants than Al-13. The acid catalyzed decomposition and followed by recrystallization to form bayerite is one of the main processes that are responsible for the decrease of Al-13 and Al-30 in polyaluminum coagulants during storage. The deprotonation and polymerization of Al-13 and Al-30 depend on solution pH. The hydrolysis products are positively charged, and consist mainly of repeated Al-13 and Al-30 units rather than amorphous Al(OH)(3) precipitates. Al-30 is less stable than Al-13 upon alkaline hydrolysis. Al-13 is stable at pH < 5.9, while Al-30 lose one proton at the pH 4.6-5.75. Al-13 and Al-30 lose respective 5 and 10 protons and form [Al-13] (n) and [Al-30] (n) clusters within the pH region of 5.9-6.25 and 5.75-6.65, respectively. This indicates that Al-30 is easier to aggregate than Al-13 at the acidic side, but [Al-13] (n) is much easier to convert to Alsol-gel than [Al-30] (n) . Al-30 possesses better characteristics than Al-13 when used as coagulant because the hydrolysis products of Al-30 possess higher charges than that of Al-13, and [Al-30] (n) clusters exist within a wider pH range.

Investigation of spectral bandwidth of optical parametric amplification

The spectral bandwidth of three-wave-mixing optical parametric amplification has been investigated. A general mathematical model for evaluating the spectral bandwidth of optical parametric amplification is developed with parametric bandwidth and gain bandwidth via three-wave noncollinear interactions. The spectral bandwidth is determined by expanding the wave-vector mismatch in a Taylor series and retaining terms through second order. The model takes into account the effects of crystal length, noncollinear angle, group velocity, group-velocity dispersion and gain coefficient. The relation between parametric bandwidth and gain bandwidth is clearly defined. The model is applied to a BBO OPA, a LBO OPA and a CLBO OPA.

Ultrafast sum-frequency polarization beats in twin Markovian stochastic correlation

An analytic closed form for the second- order or fourth- order Markovian stochastic correlation of attosecond sum- frequency polarization beat ( ASPB) can be obtained in the extremely Doppler- broadened limit. The homodyne detected ASPB signal is shown to be particularly sensitive to the statistical properties of the Markovian stochastic light. fields with arbitrary bandwidth. The physical explanation for this is that the Gaussian- amplitude. field undergoes stronger intensity. fluctuations than a chaotic. field. On the other hand, the intensity ( amplitude). fluctuations of the Gaussian- amplitude. field or the chaotic. field are always much larger than the pure phase. fluctuations of the phase-diffusion field. The field correlation has weakly influence on the ASPB signal when the laser has narrow bandwidth. In contrast, when the laser has broadband linewidth, the ASPB signal shows resonant- nonresonant cross correlation, and the sensitivities of ASPB signal to three Markovian stochastic models increase as time delay is increased. A Doppler- free precision in the measurement of the energy- level sum can be achieved with an arbitrary bandwidth. The advantage of ASPB is that the ultrafast modulation period 900as can still be improved, because the energy- level interval between ground state and excited state can be widely separated.

Twin Markovian field correlation on four-level attosecond polarization beats

Based on the phase-conjugate polarization interference between two two-photon processes, we obtained an analytic closed form for the second-order or fourth-order Markovian stochastic correlation of the four-level attosecond sum-frequency polarization beat (FASPB) in the extremely Doppler-broadened limit. The homodyne-detected FASPB signal is shown to be particularly sensitive to the statistical properties of the Markovian stochastic light fields with arbitrary bandwidth. The different roles of the amplitude fluctuations and the phase fluctuations can be understood physically in the time-domain picture. The field correlation has a weak influence on the FASPB signal when the laser has narrow bandwidth. In contrast, when the laser has broadband linewidth, the FASPB signal shows resonant-nonresonant cross-correlation, and drastic difference for three Markovian stochastic fields. The maxima of the two two-photon signals are shifted from zero time delay to the opposite direction, and the signal exhibits damping oscillation when the laser frequency is off-resonant from the two-photon transition. A Doppler-free precision in the measurement of the energy-level sum can be achieved with an arbitrary bandwidth. As an attosecond ultrafast modulation process, it can be extended intrinsically to any sum frequency of energy levels.

Coherent laser control in attosecond sum-frequency polarization beats using twin noisy driving fields

Based on the phase-conjugate polarization interference between two-pathway excitations, we obtained an analytic closed form for the second-order or fourth-order Markovian stochastic correlation of the V three-level sum-frequency polarization beat (SFPB) in attosecond scale. Novel interferometric oscillatory behavior is exposed in terms of radiation-radiation, radiation-matter, and matter-matter polarization beats. The phase-coherent control of the light beams in the SFPB is subtle. When the laser has broadband linewidth, the homodyne detected SFPB signal shows resonant-nonresonant cross correlation, a drastic difference for three Markovian stochastic fields, and the autocorrelation of the SFPB exhibits hybrid radiation-matter detuning terahertz damping oscillation. As an attosecond ultrafast modulation process, it can be extended intrinsically to any sum frequency of energy levels. It has been also found that the asymmetric behaviors of the polarization beat signals due to the unbalanced controllable dispersion effects between the two arms of interferometer do not affect the overall accuracy in case using the SFPB to measure the Doppler-free energy-level sum of two excited states.

NEAR-RESONANT RAMAN-SCATTERING FROM GAAS/ALAS SUPERLATTICES

This article presents the results of near-resonant Raman scattering measurements on GaAs/AlAs superlattices at room temperature. A strong enhancement of GaAs LO phonon-even modes resulted owing to a dipole-allowed Frohlich interaction in superlattices. Similar to the previous results, the LO phonon-even modes in a polarized configuration are observed. In contrast to previous work, however, what we observed in depolarized configurations is the LO phonon-odd modes instead of even modes. It is confirmed that the selection rules for near-resonant Raman scattering from LO phonons in this kind of superlattices are the same as those for off-resonant scattering. From the second-order Raman scattering, it is confirmed that polarized second-order Raman scattering spectra consist of overtones and combinations of two even modes, and depolarized second-order Raman scattering spectra consist of combinations of an even mode and an odd mode. Our experimental results coincide with the predictions using the recently developed Huang-Zhu model. A brief discussion on interface modes and their combination with confined modes is also presented.