Push-pull charge-transfer organic molecules exhibit large second-order nonlinear optical nonlinearity , and have been used to manufacture efficient photonic devices .We study a series of CT molecules by using the two-photon scattering method with a tunable femto-second pulsed-laser to obtain the value of the molecular first hyperpolarizability (£]) .We discuss the relationship between the£]value and chemical structure , and compare the£]values with the two-level model prediction for several incident laser excitation wavelength.

Thesis (Ph.D)--Chemistry and Biochemistry, Georgia Institute of Technology, 2009. / Committee Chair: Brédas, Jean-Luc; Committee Member: Janata, Jiri; Committee Member: Kippelen, Bernard; Committee Member: Marder, Seth; Committee Member: Sherrill, David. Part of the SMARTech Electronic Thesis and Dissertation Collection.

Thesis (Ph. D.)--University of Washington, 2003. / Vita. Includes bibliographical references (leaves 143-146).

DNA photocleaving reagents are a unique class of molecules that display the ability to cleave DNA, causing strand breaks, upon exposure to an irradiation source. In terms of biological applications, achieving excitation through a two-photon absorption event provides for unique benefits that can be useful in such applications as photodynamic therapy and cell viability studies. Thus, this thesis pertains to the study of a class of photocleaving reagents that have been shown to become excited through a twophoton process during irradiation with a pulsed femtosecond laser at 775 nm. N-(Alkoxy)pyridinethiones were selected as possible oxygen-based radical generators upon irradiation at two-photon wavelengths. Experiments were carried out with pBR 322 plasmid DNA to determine if these N-(alkoxy)pyridinethiones could cause strand cleavage and if so how efficient they are in doing so. Several compounds were found to be effective DNA strand cleavers when irradiated at two-photon wavelengths, displaying the utility of two-photon excitation in biological studies. Rationale is suggested for the observed variation in cleaving efficiency based on inherent properties of the generated radicals. A second study was done to measure the two-photon cross section of the compound N-(anthracenoyloxy)pyridinethione. The two-photon cross section was found by measuring the fraction of substrate remaining after specific periods of femtosecond laser irradiation at 775 nm, and the two-photon cross section was found to be 0.051 GM.

The purpose of this thesis is to investigate the nonlinear phenomena known as doubly-stimulated, non-degenerate two-photon emission (ND-2PE) in Gallium Arsenide (GaAs). 2PE refers to the simultaneous emission of two-photons as electrons move from the conduction band in a direct gap semiconductor to the valence band. Following the same path for describing one-photon emission (1PE) we describe 2PE as a product of the irradiance, and the negative of the loss which in this case is two-photon absorption, , the negative coming from the population inversion. We attempt to observe 2PE by using a frequency non-degenerate pump-probe experiment in which a third beam optically excites a 4 µm thick GaAs sample. We use nondegenerate beams in hopes of utilizing the 3-orders of magnitude enhancement seen in twophoton absorption (2PA) by going to extreme nondegeneracy (END) to enhance 2PE. GaAs is chosen due to the availability of the appropriate wavelengths, the maturity of the GaAs technology, its use in optoelectronic devices and its ability to be electrically pumped. During the experimental development we learn how to effectively etch and manipulate thin GaAs samples and model the transmission spectrum of these samples using thin film transmission matrices. We are able to match the measured transmission spectrum with the theoretical transmission spectrum. Here we etch the bulk GaAs left on the sample leaving only the 4 µm thickness of molecular beam epitaxial grown GaAs plus additional layers of aluminum gallium arsenide (AlGaAs). These samples were grown for us by Professor Gregory Salamo of the University of Arkansas. iv Using the pump-probe experiment on the 4 µm GaAs sample, we measure the change of the 2PA due to the presence of optically excited carriers. The goal is to reduce the 2PA signal to zero and then invert the 2PA signal indicating an increase in transmission indicative of 2PE when the population is inverted. Our results show that we achieve a 45% reduction in the 2PA signal in a 4 μm thick GaAs sample due to the excited carriers. Unfortunately, we currently cannot experimentally determine whether the reduction is strictly due to free-carrier absorption (FCA) of our pump or possibly due to a change in the two-photon absorption coefficient. We measure the transmission of various wavelengths around the bang gap of GaAs as a function of excitation wavelength and achieve a transmittance of ~80% which we attribute to possibly be one photon gain (1PG) at 880 nm. We also go to cryogenic temperatures to concentrate the carriers near the bottom of the conduction band and improve the theoretical gain coefficient for 2PE. Unfortunately, we do not observe a measurable change in 2PA with the addition of optically excited carriers. Along with FCA of our infrared pump we suspect that the difficulties in this first set of experiments are also a result or radiative recombination due to amplified spontaneous emission reducing our free carrier density along with the fact that 4 m is too thick for uniform excitation. We now have 1 m samples from Professor Gregory Salamo which we hope will give better and more definitive results

No description available.

Astrocytes, the major type of non-neuronal cells in the brain, play an important functional role in the brains extracellular potassium (K+) and pH homeostasis. Pathological brain states have been shown to cause astrocyte swelling. However, these volume changes have never before been verified to occur in response to physiological activity. In the present thesis, two-photon laser scanning microscopy was used to visualize real-time astrocyte volume changes in the stratum radiatum of the CA1 region of the hippocampus. Astrocyte somas and primary processes were observed to swell by 19.0±0.9% in response to a physiological (3 mM) increase in the concentration of extracellular K+. Astrocyte swelling was partially mediated by K+ influx through inwardly rectifying K+ channels (Kir), as their inhibition resulted in a significant decrease of the increased K+ induced astrocyte swelling (13.9±0.9%). In addition, the bicarbonate ion (HCO3-) was found to play a significant role in the increased K+ induced astrocyte swelling. The astrocyte swelling was significantly decreased when the influx of HCO3- was decreased in 1) a HCO3- free extracellular solution (5.4±0.7%), 2) in the presence of an extracellular carbonic anhydrase inhibitor (11.4±0.6% ), and 3) when the activity of the sodium-bicarbonate cotransporter (NBC) was blocked (8.3±0.7%) . Conversely, astrocytes were found to shrink by 7.7±0.5% in response to ã-Amino-butyric Acid (GABA) receptor activation. GABAA receptor mediated astrocyte shrinkage was significantly decreased to 5.0±0.6% when HCO3- efflux was reduced. Furthermore, in this thesis it was shown for the first time that astrocytes swell in response to neuronal stimulation (4.0±0.4%). This activity induced astrocyte swelling was significantly decreased to 1.5±0.2% in a HCO3- free extracellular solution. These astrocyte volume changes may have important implications for the regulation of brain activity under both physiological and pathological brain states.

Astrocytes, the major type of non-neuronal cells in the brain, play an important functional role in the brains extracellular potassium (K+) and pH homeostasis. Pathological brain states have been shown to cause astrocyte swelling. However, these volume changes have never before been verified to occur in response to physiological activity. In the present thesis, two-photon laser scanning microscopy was used to visualize real-time astrocyte volume changes in the stratum radiatum of the CA1 region of the hippocampus. Astrocyte somas and primary processes were observed to swell by 19.0±0.9% in response to a physiological (3 mM) increase in the concentration of extracellular K+. Astrocyte swelling was partially mediated by K+ influx through inwardly rectifying K+ channels (Kir), as their inhibition resulted in a significant decrease of the increased K+ induced astrocyte swelling (13.9±0.9%). In addition, the bicarbonate ion (HCO3-) was found to play a significant role in the increased K+ induced astrocyte swelling. The astrocyte swelling was significantly decreased when the influx of HCO3- was decreased in 1) a HCO3- free extracellular solution (5.4±0.7%), 2) in the presence of an extracellular carbonic anhydrase inhibitor (11.4±0.6% ), and 3) when the activity of the sodium-bicarbonate cotransporter (NBC) was blocked (8.3±0.7%) . Conversely, astrocytes were found to shrink by 7.7±0.5% in response to ã-Amino-butyric Acid (GABA) receptor activation. GABAA receptor mediated astrocyte shrinkage was significantly decreased to 5.0±0.6% when HCO3- efflux was reduced. Furthermore, in this thesis it was shown for the first time that astrocytes swell in response to neuronal stimulation (4.0±0.4%). This activity induced astrocyte swelling was significantly decreased to 1.5±0.2% in a HCO3- free extracellular solution. These astrocyte volume changes may have important implications for the regulation of brain activity under both physiological and pathological brain states.

Coherent control of laser induced processes is based on the quantum interference among multiple excitation pathways. Progress in the field has been fueled by advances in pulse shaping techniques, allowing modulation of phase and amplitude across the bandwidth of ultra short pulses. This dissertation makes use of coherent control technique for the optimization of two-photon fluorescence (TPF) and its applications in selective excitation for biomedical imaging. Different physical processes, e.g. TPF, second harmonic generation (SHG) and their ratios (e.g. TPF/SHG) were optimized by using feedback control pulse shaping technique with an evolutionary algorithm. Various nonlinear effects, e.g. filamentation, intensity clamping and white light generation were studied using two-photon fluorescence and Z-scan technique with different dyes and biomarkers. Simultaneous measurements of different nonlinear effects were performed. Novel methods were proposed and implemented to obtain two-photon excitation characteristics in intensity-resolved manner. Understanding of these nonlinear effects can give new solution to the issues of spatial resolution and molecular contrast for cellular and tissue imaging.

The techniques of optical beam induced current (OBIC) have found wide-spread applications in characterizing many semiconductor and optoelectronic devices. A two-photon confocal microscope is adapted for investigating the dynamics of light emitting devices through the contrast mechanisms of two-photon DC and radio frequency (RF) optical beam induced current (OBIC). For comparison, the 2p-OBIC technique detects the photocurrent signal by exciting the semiconductor sample with a pulsed laser that has a wavelength below the bandgap of the semiconductor. It has high accuracy and spatial resolution. We demonstrate that the bias on the devices (forward and reverse) strongly modifies the DC and RF OBIC signals. Finally we will discuss how to explain this result, and we will provide a program to show the phase distribution of GaP LED.