Abstract The first hyperpolarizability(£]) of five charge-transfer molecules are determined using the hyper-Rayleigh scattering (HRS) technique at two excitation wavelengths : 1064nm and 1907nm. The 1064nm excitation wavelength is derived from a Nd: YAG pulsed laser, and the 1907nm excitation wavelength is obtained by shifting the 1064nm laser light by stimulated Raman scattering of pressurized H2 gas. Four of the five samples contains thiophene and thiazole are synthetized by Prof. Shu Ching-Fong at the National Chiao Tung University (NCTU) and the other sample is synthetized by Prof. Hong, Jin-Long at the National Sun Yat-sen University (NSYSU). The measured £] values are used to calculate the intrinsic molecular hyperpolarizabilities using the two-level model previously developed by Oudar and Chemla. The results are related to molecular structure.

The technique of hyper-Rayleigh scattering is employed to measure the first molecular hyperpolarizabilities£]of nonlinear optical chromophores provided by Industrial Technology Research Institute. £]0. In the thesis, the effect of the molecular structure and the solvent on the hyperpolarizabilities will be discussed further.

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Thesis (Ph. D.)--Ohio University, November, 1995. / Title from PDF t.p.

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Filtered Rayleigh scattering (FRS) is a non-intrusive, optical measurement technique that can currently provide time-averaged, simultaneous planar measurements of three-component velocity, static temperature, and static density of aerodynamic flows. Development of the FRS technique has typically employed 532 nm Nd:YAG lasers coupled with the use of iodine vapor cells as the molecular filter. One method to improve the effective signal-to-noise ratio (SNR), and therefore the performance of an FRS system, is to use shorter wavelengths. This takes advantage of the dependence of the Rayleigh scattering signal on the inverse of the wavelength of the incident laser light to the fourth power: even small shifts to shorter wavelengths can offer significant gains in SNR as a result. This study explores the implementation of an ultraviolet (UV) FRS system nominally at 387 nm with the use cesium vapor as the molecular filter. The cesium absorption lineshapes (corresponding to the 62S1/2 → 82P3/2 atomic transitions around 387 nm) are considered along with camera specifications to simulate an ultraviolet filtered Rayleigh scattering (UV FRS) measurement of aerodynamic flows. A signal model is developed using numerical functions for the cesium vapor cell transmission, camera specifications, signal-dependent shot noise, and signal-independent electronic detector read noise. Using this noise-inclusive model (over a 2.4 GHz scan bandwidth with a 7.5 cm long cesium vapor cell corresponding to current Virginia Tech FRS capabilities) velocity, static temperature, and static density measurement sensitivities for this proposed configuration are analyzed by evaluating and deriving the Cramér-Rao lower bound (CRLB) for each quantity. The effects of different flow conditions, Mie and geometric scattering levels, cesium vapor cell temperature, and spectral resolution are demonstrated. It is found that the best possible theoretical measurement results are obtained for high-speed wind tunnel flow conditions with high spectral resolution, and that the CRLB for velocity, static temperature, and static density for a 387 nm system approaches or exceeds that of a 532 nm system for a given signal-to-noise ratio (SNR). / Master of Science / One type of non-intrusive measurement technique that can be applied to aerodynamic flows is filtered Rayleigh scattering (FRS). Unlike other non-intrusive techniques such as particle image velocimetry (PIV) and Doppler global velocimetry (DGV), FRS does not require that the flow be seeded with particles and can provide simultaneous measurements of three-component velocity, static temperature, and static density. Current FRS measurement systems commonly use 532 nm green-light lasers and iodine cells for filtering. However, a stronger Rayleigh scattering signal (and therefore better measurement) can be attained by using shorter laser wavelengths as the strength of the Rayleigh scattering is related to the inverse of the incident wavelength to the fourth power. This study takes advantage of this fact to propose an FRS measurement system using ultraviolet laser light at nominally 387 nm. The implementation of a commercially available 387 nm laser system with the use of cesium cells for filtering is investigated. In order to simulate the performance of the system, a signal model is developed that includes both signal-dependent shot noise, and signal-independent electronic detector read noise. The signal model is combined with the transmission profile of cesium vapor, commercially available camera specifications, and typical FRS measurement parameters to simulate a 387 nm FRS system measurement. The measurement sensitives and performance of the proposed UV FRS system at 387 nm are investigated by deriving and evaluating the Cramér-Rao lower bound (CRLB) for velocity, static temperature, and static density. The effects of different flow conditions, Mie and geometric scattering levels, cesium vapor cell temperature, and scan resolution are demonstrated. The best performance is attained at high-speed conditions with high spectral resolution, and this approaches or exceeds the simulated performance of a 532 nm system with an iodine vapor cell over the same range of conditions.

Plasmonic nanoparticles, specifically gold and silver nanoparticles, exhibit unique optical, physical, and chemical properties that are exploited in many biomedical applications. Due to their nanometer size, facile surface functionalization and enhanced optical performance, gold and silver nanoparticles can be used to investigate cellular biology. The work herein highlights a new methodology that has exploited these remarkable properties in order to probe various aspect of cancer cell biology, such as cell cycle progression, drug delivery, and cell death. Cell death mechanisms due to localized gold and silver nanoparticle exposure were also elucidated in this work. Chapter 1 introduces the reader to the synthesis and functionalization of gold and silver nanoparticles as well as reviews their implementation in biodiagnostic and therapeutic applications to provide a foundation for Chapters 3 and 4, where their use in spectroscopic and cytotoxic studies are presented. Chapter 2 provides the reader with detailed explanations of experimental protocols for nanoparticle synthesis and functionalization, in vitro cellular biology experiments, and live-cell Raman spectroscopy experiments that were utilized throughout Chapters 3 and 4. Chapter 3 presents the use of nuclear-targeted gold nanoparticles in conjunction with a Raman microscope modified to contain a live-cell imaging chamber to probe cancer cell cycle progression (Chapter 3.1), examine drug efficacy (Chapter 3.2), monitor drug delivery (Chapter 3.3), and detect apoptotic molecular events in real-time (Chapter 3.4). In Chapter 4, the intracellular effects of gold and silver nanoparticles are explored through live-cell Rayleigh imaging, cell cycle analysis and DNA damage (Chapter 4.1), as well as through the elucidation of cytotoxic cell death mechanisms after nanoparticle exposure (Chapter 4.2) and live cell imaging of silver nanoparticle treated cancer cell communities (Chapter 4.3).

Neste trabalho, estudamos as propriedade ópticas da tetrapiridilporfirina (TPyP), usando clorofórmio como sol vente. Para a caracterização óptica linear foram medidos os espectros de fluorescência e absorbância, tendo este último nos permitido determinar a seção de choque para o estado fundamental com radiação incidente em 532 nm. Usamos a técnica de varredura Z com trem de pulsos (VZTP) para medirmos a absorção não linear da TPyP, em 532 nm, e determinamos, através de um modelo fenomenológico de cinco níveis, vários parâmetros espectroscópicos tais como seções de choques e tempos de vida dos estados. Além disso, com a utilização da técnica de espalhamento hiperRayleigh (HRS) medimos a primeira hiperpolarizabilidade da TPyP, dissolvida em clorofórmio em 1064 nm usando, como material de referência, a p-nitroanilina (PN A), diluída em metanol. / This work reports on the optical properties of the tetrakis(pyridil)porphyrin (TPyP). In order to perform the linear optical characterization, fluorescence and absorbance spectra were obtained, where the latter allowed the determination of the cross-section for the ground state with incident radiation at À = 532 nm. We used the Zscan tecnique with pulse trains (ZSPT) to measure the nonlinear absorption of TPyP, at 532 nm, and we managed to determine, through a phenomenological five levels model, several spectroscopic parameters such as cross-sections and lifetime of the states. Moreover, we measured the first hyperpolarizability of TPyP dissolved in chloroform, at À = 1064 nm, using the Hyper-Rayleigh scattering (HRS) technique. The reference material used for HRS measurements was p-nitroaniline (PNA) dissolved in methanol.