Thesis (Ph.D.)--University of Nebraska-Lincoln, 2008. / Title from title screen (site viewed Sept. 16, 2008). PDF text: xvi, 196 p. : ill. (some col.) ; 9 Mb. UMI publication number: AAT 3297758. Includes bibliographical references. Also available in microfilm and microfiche formats.

Doctor of Philosophy / Department of Physics / Carlos A. Trallero / Ultra-fast spectroscopy has become a common tool for understanding the structure and dynamics of atoms and molecules, as evidenced by the award of the 1999 Nobel Prize in Chemistry to Ahmed H. Zewail for his pioneering work in femtochemistry. The use of shorter and more energetic laser pulses have given rise to high intensity table-top light sources in the visible and infrared which have pushed spectroscopic measurements of atomic and molecular systems into the strong-field limit. Within this limit, there are unique phenomena that are still not well understood. Many of such phenomena involve a photoionization step. For three decades, there has been a steady investigation of the single ionization of atomic systems in the strong-field regime both experimentally and theoretically. The investigation of the ionization of more complex molecular systems is of great interest presently and will help with the understanding of ultra-fast spectroscopy as a whole. In this thesis, we explore the single ionization of molecules in the presence of a strong electric field. In particular, we study molecular isomer pairs, molecules that are the same elementally, but different structurally. The main goal of this work is to compare the ionization yields of these similar molecular pairs as a function of intensity and gain some insight into what differences caused by their structure contribute to how they ionize in the strong-field limit. Through our studies we explore a wavelength dependence of the photoionization yield in order to move from the multi-photon regime of ionization to the tunneling regime with increasing wavelength. Also, in contrast to our strong-field studies, we investigate isomeric molecules in the weak-field limit through single photon absorption by measuring the total ionization yield as a function of photon energy. Our findings shed light on the complexities of photoionization in both the strong- and weak-field limits and will serve as examples for the continued understanding of single ionization both experimentally and theoretically.

Doctor of Philosophy / Department of Physics / Vinod Kumarappan / In general, molecules in the gas phase are free to rotate, and measurements made on such samples are averaged over a randomly oriented distribution of molecules. Any orientation dependent information is lost in such measurements. The goal of the work presented here is to a) mitigate or completely do away with orientational averaging, and b) make fully resolved orientation dependent measurements. In pursuance of similar goals, over the past 50 years chemists and physicists have developed techniques to align molecules, or to measure their orientation and tag other quantities of interest with the orientation. We focus on laser induced alignment of asymmetric top molecules. The first major contribution of our work is the development of an effective method to align all molecular axes under field-free conditions. The method employs a sequence of nonresonant, impulsive laser pulses with varied ellipticities. The efficacy of the method is first demonstrated by solution of the time dependent Schr\"{o}dinger equation for iodobenzene, and then experimentally implemented to three dimensionally align 3,5 difluoroiodobenzene. Measurement from molecules aligned in this manner greatly reduces orientational averaging. The technique was developed via a thorough understanding and extensive computations of the dynamics of rotationally excited asymmetric top molecules. The second, and perhaps more important, contribution of our work is the development of a new measurement technique to extract the complete orientation dependence of a variety of molecular processes initiated by ultrashort laser pulses. The technique involves pump-probe measurements of the process of interest from a rotational wavepacket generated by impulsive excitation of asymmetric top molecules. We apply it to make the first measurement of the single ionization probability of an asymmetric top molecule in a strong field as a function of all relevant alignment angles. The measurement and associated calculations help identify the orbital from which the electron is ionized. We expect that this technique will be widely applicable to ultrafast-laser driven processes in molecules and provide unique insight into molecular physics and chemistry.

No description available.

Master of Science / Physics / Vinod Kumarappan / This report includes the experimental details and results of two experiments. The first experiment addresses carrier envelope phase (CEP) effects in higher order harmonic generation (HHG), and the second experiment is a pump-probe experiment on CO₂ molecules using ultrashort laser pulses. Ultrashort laser pulses that are only a few optical cycles long are of interest for studying different atomic and molecular processes. The CEP of such a pulse is an important parameter that can affect the experimental results. Because the laser pulses we used in the HHG experiment have random CEP, we tagged a given harmonic spectrum with the CEP of the fundamental laser pulse that generated it by measuring both shot-by-shot. The first chapter of this report is about the experimental details and the results we got from our CEP-tagged HHG experiment that enabled us to observe the interference of different quantum pathways. In the second experiment, discussed in the second chapter of this report, we tried to study the structure of the CO₂⁺ ion created by strong field ionization in a pump-probe experiment. For this experiment, we used an ultrashort laser pulse to ionize CO₂ molecules, and after various time delays we probed the ionic wave packet by ionizing CO₂⁺ with another ultrashort laser pulse. By performing Fourier analysis on the delay-dependent CO₂⁺⁺ yield, we were able to identify the populated states of CO₂⁺.

Thesis (Ph. D.)--Florida State University, 2004. / Advisor: Dr. Alan Marshall, Florida State University, College of Arts and Sciences, Dept. of Chemistry and Biochemistry. Title and description from dissertation home page (viewed June 1, 2005). Document formatted into pages; contains xix, 146 pages. Includes bibliographical references.

Thesis (M.S.)--University of Texas at Dallas, 2008. / Includes vita. Includes bibliographical references (leaves 85-91)

We develop an efficient back gate for silicon-on-insulator (SOI) devices operating at cryogenic temperatures and measure the quadratic hyperfine Stark shift parameter of arsenic donors in isotopically purified 28Si-SOI layers using such structures. The back gate is implemented using MeV ion implantation through the SOI layer forming a metallic electrode in the handle wafer, enabling large and uniform electric fields up to 2V/lm to be applied across the SOI layer. Utilizing this structure, we measure the Stark shift parameters of arsenic donors embedded in the 28Si-SOI layer and find a contact hyperfine Stark parameter of na=-1.9+/-0.7x10-3 lm2/V2. We also demonstrate electric-field driven dopant ionization in the SOI device layer, measured by electron spin resonance.

This dissertation investigates the electronic spectroscopy of a series of alkyl phenyl ketone radical cations and the dynamics of selective launch states in the strong field regime with tunable near infrared ultrashort laser pulses from 790 nm - 1550 nm coupled to mass spectrometric detection. Our method relies on tunable strong field laser pulses in the range from 1150 nm - 1550 nm to adiabatically ioinized gas phase molecules and prepare ions in the ground ionic state that serve as a launch state for future excitation and control. Adiabatic ionization is capable of transferring little energy to the molecule and producing a majority of a parent molecular ion in comparison to nonadiabatic ionization wherein multiple ionic states can be populated with an accompanying high degree of molecular fragmentation. We measure a dynamic resonance in the low lying electronic states of the acetopheone radical cation via preparation of a launch state with adiabatic ionization followed by a one photon transition within a single pulse duration which facilitates bond dissociation to produce the benzoyl ion. Experiments on acetophenone homologues and derivatives elucidate the structural dependence of the electronic resonance and supporting ab initio calculations identify the dynamic resonance along the molecular torsional coordinate between the ground ionic state, D0, and second excited state, D2. Post ionization excitation within the pulse duration transfers the ground state wavepacket to the D2 surface where the wavepacket encounters a three state conical intersection that facilitates the preferred bond dissociation. Time resolved photodissociation experiments measure the dynamics of the launch state, large amplitude oscillations and extended coherence times support the notion that adiabatic ionization populates a majority of the ground ionic surface. Control of the dissociation products is initiated from the launch state by varying the pump wavelength and probe intensity. Elimination of the D0 wavepacket with a 1370 nm reveals additional secondary dynamics that are attributed to wavepacket motion on the D2 surface. Finally, the effect of para substitution on the acetophenone radical cation is explored as a strategy to control the launch state wavepacket dynamics. Suppresion of the wavepacket dynamics are observed with the addition of alkoxy groups whereas extended coherence of the launch state dynamics approaching ~5 ps is observed upon trifluoromethyl substitution. A possible mechanism for the extended coherenece based on coupled torsional rotors is proposed. / Chemistry

The present thesis is focused on study of dust grain charging. The experimental part covers interaction between dust grains and high-energy electrons and self-discharging of grains by both field electron emission and field ionization. The second part of the thesis describes construction and evaluation of a linear electrodynamic trap of the novel design. We have observed charging of small dust grains towards high positive electric potentials when bombarded by the high-energy electron beam. We have described an increase of the secondary electron- electron emission yield from negatively charged grains due to the surface field. Further, self-discharging characteristics for both positively and negatively charged grains were measured. The relationship between discharging rate and the rate of the flow of atoms leaving the grain surface due to diffusion was observed for positively charged grains. This suggests significantly lower surface field necessary for ionizing such atoms compared to the ionization of atoms of surrounding gas and compared to the typically published field ionization thresholds. Based on the design published in the master thesis, a linear quadrupole trap of novel design was constructed. Testing measurements confirmed functionality and expected characteristics of the trap. In addition, effects of...