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Guang S He

Publications and source records attributed to Guang S He.

11 recordsLinked to original sources
PubMed2006

Experimental and quantum chemical studies of cooperative enhancement of three-photon absorption, optical limiting, and stabilization behaviors in multibranched and dendritic structures.

This paper reports on cooperative enhancement of three-photon absorption (3PA) cross section, studied by nonlinear transmission method, in going from a one-branched to a three-branched and then to a dendritic structure. Experimentally, we observe a 72% enhanced 3PA cross-section value in going from the one-branched chromophore to the dendritic chromophore, and a 49% enhanced 3PA cross-section value in going from the one-branched chromophore to the three-branched chromophore, when the 3PA cross-section values are normalized per structure unit. Quantum chemical calculation for the one- and three-branched structures, using the cubic response (CR) theory applied to a single determinant self-consistent field (SCF) reference state, also predicts such an enhancement. Two-dimensional pi-delocalization, resulting in extended charge-transfer network in the case of the multibranched structures, is the main cause of the cooperative enhancement. Owing to the increased 3PA cross-section value for the dendritic chromophore, improved optical limiting performance at an optical communication wavelength of 1310 nm was observed, compared with the one-branched (or three-branched) chromophore, using comparable structure-unit-based concentrations. Optical stabilization capability of the dendritic chromophore was also observed at this wavelength.

Absorption↗
PubMed2006

Infrared two-photon-excited visible lasing from a DNA-surfactant-chromophore complex.

Infrared two-photon-pumped and cavity-enhanced frequency upconversion lasing has been achieved in a novel DNA-surfactant-chromophore complex (DSCC) gel system, which is a new step toward producing a biological laser. Once the focused intensity of the 150 fs and approximately 775 nm pump laser beam is higher than a certain threshold level, highly directional stimulated emission at approximately 582 nm wavelength can be observed from a 1 cm long DSCC complex gel cell. With cavity feedback provided by the two optical windows, the pump threshold can be further reduced, the highly directional output lasing can be greatly enhanced, and the output spectral linewidth can be reduced to less than 1/5 of the spontaneous fluorescence spectral bandwidth.

DNA↗
PubMed2005

Ultrafast dynamics in multibranched structures with enhanced two-photon absorption.

The understanding of the mechanism of the enhanced two-photon absorption (TPA) in multibranched chromophore systems is of importance to the design of materials with the large TPA cross-sections and for future applications. In this communication, the mechanism of enhanced TPA properties is investigated. For a dendritic model system, the excited-state dynamics for both population (T1-process) and phase relaxation (T2-process) processes involved are investigated by a combination of time-resolved spectroscopic techniques. The results of time-resolved fluorescence anisotropy are compared with previous results obtained from other branched chromophore systems. It is found that the PRL-701 trimer system, which possesses the large enhancement of two-photon absorption cross-section, gives a faster anisotropy decay (fluorescence upconversion and transient absorption), a longer population relaxation time (fluorescence lifetime), and a weaker coupling to the solvent (a larger photon echo peak shift initial value). New strategies for rational design of large TPA materials can be achieved based on a better understanding of the mechanism of the enhancement.

Journal Article↗
PubMed2005

Nonlinear optical stabilization of 1064-nm laser pulses with a two-photon absorbing liquid-dye salt system.

Highly effective optical power-limiting and optical-stabilization performances have been achieved in a new type of two-photon absorbing medium. That is a liquid-dye salt system, trans-4-[p-(N,N-dimethoxyethylamino)styryl]-N-3,6,9-trioxadecylpyridinium tetrafluoroborate (abbreviated as ASDPT), which features an unusually high molar concentration (-1 M) of two-photon absorbing chromophores and the capability of withstanding a higher pulsed laser power and energy. The nonlinear transmission property and output-input characteristics were studied based on a 1-cm-long liquid-dye salt sample by use of nanosecond 1064-nm laser pulses with a repetition rate variable from 1 to 10 Hz. A superior optical-stabilization behavior of the studied material was demonstrated; the relative fluctuation of the nanosecond laser pulses can be reduced by more than two times simply by passing them through this highly concentrated nonlinear absorbing medium.

Journal Article↗
PubMed2005

Direct four-photon excitation of amplified spontaneous emission in a nonlinear organic chromophore.

We report four-photon pumped amplified spontaneous emission in an organic chromophore. The phenomenon is observed when intense infrared laser radiation illuminates a nonlinear chromophore solution. As a result of this illumination, a strong and highly directional radiation in the visible wavelength range is generated in both the forward and the backward directions, with an angular divergence similar to that of the pump beam.

Fluorescent Dyes↗
PubMed2004

Degenerate two-photon-absorption spectral studies of highly two-photon active organic chromophores.

Degenerate two-photon absorption (TPA) spectral properties of five AFX chromophore solutions have been studied using a single and spectrally dispersed sub-picosecond white-light continuum beam. In a specially designed optical configuration, optical pathways inside the sample solution for different spectral components of the focused continuum beam were spatially separated from each other. Thus, the nondegenerate TPA processes coming from different spectral components can be eliminated, and the direct nonlinear absorption spectrum attributed to degenerate TPA processes can be readily obtained. Using this new technique, the complete TPA spectra for these five highly two-photon-active compounds (AF-380, AF-350, AF-295, AF-270, and AF-50) were obtained in the spectral range from 600 to 950 nm on an absolute scale of TPA cross section. The relationship between the molecular structures and their TPA spectral behaviors are discussed. In general the measured TPA spectra are not identical with the linear absorption spectra on the scale of absorbed photon(s) energy. Moreover, for some sample (such as AF-380), the TPA spectrum is totally different from the linear spectrum, which implies the difference of molecular transition pathways and selection rules for one- and two-photon excitation processes. At high excitation intensity levels (>or=15 GW/cm(2)), the saturation behavior of TPA transition can be observed obviously in AF-350 and AF-380 solutions that exhibit much higher nonlinear absorptivity than the other chromophores investigated.

Journal Article↗
PubMed2003

Two-photon excited intramolecular energy transfer and light-harvesting effect in novel dendritic systems.

Two-photon absorption excited intramolecular energy transfer and light-harvesting effects are demonstrated in three novel dendritic systems. These systems contain both an antenna structure that can effectively absorb two-photon energy at approximately 800 nm and emit fluorescence at approximately 515 nm and a core moiety that can absorb one-photon energy at approximately 520 nm and emit at approximately 590 nm. Covalently combining the core and antenna functionalities intrinsically changes the optical behavior of the component pieces. The two-photon energy absorbed by the antenna structure is resonantly transferred to the core, where the core's emission intensity is enhanced by 8, 20, and 34 times for the three dendritic systems.

Journal Article↗
PubMed2003

Ultrashort 1.5-microm laser excited upconverted stimulated emission based on simultaneous three-photon absorption.

Simultaneous three-photon excited stimulated emission at (cavityless lasing) approximately 610 nm has been achieved in an organic chromophore solution pumped by approximately 1.5-microm ultrashort coherent radiation. The stimulated emission can be observed only in the forward and backward directions and is characterized by its high directionality and spectral narrowing. The divergence angle for the backward stimulated emission is considerably smaller than that for the forward stimulated emission, which resembles optical phase conjugation.

Lasers↗
PubMed2003

Fluorescence resonance energy transfer in a novel two-photon absorbing system.

A novel fluorescence resonance energy transfer (FRET) system containing a two-photon absorbing dye and a nile red chromophore has been synthesized. Upon two-photon excitation by laser at 815 nm this molecule displays efficient energy transfer from the two-photon absorbing dye to the nile red moiety, with an 8-fold increase in emission compared to the model compound. Similarly, single-photon excitation of the two-photon absorbing moiety at 405 nm results in >99% energy-transfer efficiency, along with a 3.4-fold increase in nile red emission compared to direct excitation of the nile red chromophore at 540 nm. This system provides an effective way to use IR radiation to excite molecules that, by themselves, have little or no two-photon absorption.

Journal Article↗
PubMed2002

Observation of stimulated emission by direct three-photon excitation.

Multiphoton processes, predicted theoretically in 1931, were for a long time considered to be mainly of academic interest. This view changed when it was shown that a two-photon absorption process could, because of a quadratic dependence of excitation on intensity, produce a spatially confined excitation useful for three-dimensional data storage and imaging. Two-photon absorption has received considerable attention recently because of the development of highly efficient two-photon-sensitive materials, leading to numerous technological applications. These successes have created interest in exploring applications based on three-photon excitations. For a three-photon process, a longer excitation wavelength such as those common in optical communications can be used. Also, the cubic dependence of the three-photon process on the input light intensity provides a stronger spatial confinement, so that a higher contrast in imaging can be obtained. Here we report the observation of a highly directional and up-converted stimulated emission as an amplified spontaneous emission, produced in an organic chromophore solution by a strong simultaneous three-photon absorption at 1.3 microm. This achievement suggests opportunities for a three-photon process in frequency-upconversion lasing, short-pulse optical communications, and the emerging field of biophotonics.

Coloring Agents↗