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.

Two bifurcation processes for onset of oscillatory thermocapillary convection in a floating half zone

An overview on the onset of thermocapillary oscillatory convection in a floating half zone is provided, and it is a typical subject in the microgravity sciences related to the space materials science, especially the floating zone processing, and also to the microgravity fluid physics. The main interests are focused around the process for onset of oscillatory thermocapillary convection, which is known also as the bifurcation transition from quasi-steady convection to oscillatory convection. The onset of oscillation depends on a set of critical parameters, such as the Marangoni number, Prandtl number, geometrical parameters, and heat transfer parameters. Recent studies show that, there exists the bifurcation transition from steady and axial symmetric convection to the steady and axial non-symmetric convection before the onset of oscillation in cases of small Prandtl number fluids and in cases of larger Prandtl number fluids of fat liquid bridge with small aspect ratio. The transition process is a strong non-linear process because the velocity deviation has the same order of magnitude as that of an average flow after the onset of oscillation, and unsteady 3-D numerical simulation is suitable to do in depth analysis on strong non-linear process, and leads generally to a better comparison with the experimental results.

Reduced deep-tissue image degradation in three-dimensional multiphoton microscopy with concentric two-color two-photon fluorescence excitation

We theoretically demonstrate that enhanced penetration depth in three-dimensional multiphoton microscopy can be achieved using concentric two-color two-photon (C2C2P) fluorescence excitation in which the two excitation beams are separated in space before reaching their common focal spot. Monte Carlo simulation shows that, in comparison with the one-color two-photon excitation scheme, the C2C2P fluorescence microscopy provides a significantly greater penetration depth for imaging into a highly scattering medium. (C) 2008 Optical Society of America.

Two-color two-photon excitation of indole using a femtosecond laser regenerative amplifier

The fluorescence emission from indole resulting from two-color two-photon (2C2P) excitation with 400 and 800 nm wavelengths is observed, using the second harmonic and fundamental wavelength of a 800 nm 40 fs pulsed Ti:Sapphire femtosecond (fs) regenerative amplifier operating at a repetition rate of 1 kHz. By delaying one fs laser pulse relative to the other, the cross correlation of fluorescence is observed, which indicates the generation of 2C2P fluorescence signal in the experiment. The strongest 2C2P fluorescence emission characterized by the peak of cross correlation curve suggests optimal temporal overlap of the two fs laser pulses. The 2C2P fluorescence signal is linearly dependent on the total excitation intensity. The fluorescence signals with 400 nm and 800 nm irradiation alone are also demonstrated and discussed in this paper. (C) 2008 Elsevier B.V. All rights reserved.

Universal Greenberger-Horne-Zeilinger-state analyzer based on two-photon polarization parity detection

We present a universal analyzer for the three-particle Greenberger-Horne-Zeilinger (GHZ) states with quantum nondemolition parity detectors and linear-optics elements. In our scheme, all of the three-photon GHZ states can be discriminated with nearly unity probability in the regime of weak nonlinearity feasible at the present state of the art experimentally. We also show that our scheme can be easily extended to the analysis of the multi-particle GHZ states.

Measurement of two-photon excitation cross-section of a new symmetric-type fluorene derivative

A new dye, 2,7-bis(4-methoxystyryl)-9,9-bis(2-ethylhexyl)-9H-fluorene, has been synthesized, which is a D-pi-D symmetrical-type fluorene derivative. The two-photon absorption (TPA) of this new dye has been experimentally studied by comparable two-photon-induced fluorescence method. This new dye has a TPA cross-section of 84 x 10(-50) cm(4) s/photon at 790 nm/13 fs. (c) 2004 Elsevier GmbH. All rights reserved.

Optimal feedback control of two-photon fluorescence based on genetic algorithm

An optimal feedback control of two-photon fluorescence in the ethanol solution of 4-dicyanomethylene-2-methyl-6-p-dimethyl-amiiiostryryl-4H-pyran (DCM) using pulse-shaping technique based on genetic algorithm is demonstrated experimentally. The two-photon fluorescence of the DCM ethanol solution is enhanced in intensity of about 23%. The second harmonic generation frequency-resolved optical gating (SHG-FROG) trace indicates that the effective population transfer arises from the positively chirped pulse. The experimental results appear the potential applications of coherent control to the complicated molecular system.

Optimal feedback control of two-photon fluorescence in Coumarin 515 based on genetic algorithm

An optimal feedback control of two-photon fluorescence in the Coumarin 515 ethanol solution excited by shaping femtosecond laser pulses based on genetic algorithm is demonstrated experimentally. The two-photon fluorescence intensity can be enhanced by similar to 20%. Second harmonic generation frequency-resolved optical gating traces indicate that the optimal laser pulses are positive chirp, which are in favor of the effective population transfer of two-photon transitions. The dependence of the two-photon fluorescence signal on the laser pulse chirp is investigated to validate the theoretical model for the effective population transfer of two-photon transitions. The experimental results appear the potential applications in nonlinear spectroscopy and molecular physics. (c) 2005 Elsevier B.V. All rights reserved.

A new strategy of enhancing two-photon absorption in benzothiazole-containing fluorene molecules: Introduction of auxiliary donor-acceptor effects

A series of benzothiazole-containing fluorene molecules have been designed and their one- and two-photon absorption properties have been investigated theoretically by using the ZINDO method. The effects of electron-excessive/deficient heterocyclic bridges as auxiliary donors (auxD)/acceptors (auxA) on TPA cross-sections were studied. The results show that the molecules with D-pi-auxA-A, D-aux D-pi-A, or D-auxD-pi-auxA-A structure types have large TPA cross-section, which can be a valuable strategy in the design of two-photon absorption materials. Also, a linear relationship between the first hyperpolarizability and the TPA cross-section is observed. (c) 2006 Elsevier B.V. All rights reserved.

Theoretical investigation on the one- and two-photon absorption properties for a series of symmetrical charge transfer fluorene-phenylene and fluorene-thiophene derivatives

One- and two-photon absorption properties of a series of fluorene derivatives with symmetrical charge transfer D-IT-D and A-IT-A structural motifs have been theoretically investigated with ZINDO/S method. The optimized structures and the characterization of frontier molecular orbitals were obtained by using AMI calculations. Two-photon absorption properties of molecules have been studied using three-state model. The calculation results have shown that fluorene-thiophene derivatives exhibit larger two-photon absorption cross-section as compared with other studied molecules. To illustrate the results, the crucial effects of thiophene ring on fluorenethiophene derivatives and the net charge changes on the pi-conjugated bridges are analyzed theoretically. (c) 2006 Elsevier B.V. All rights reserved.