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- All Subjects: Fluorescence spectroscopy
- Creators: Nye, Joshua
- Creators: Richert, Ranko
Description
Transient molecules are of great importance having proposed applications in quantum science and technology and tests of fundamental physics. In the present dissertation, the transient molecules studied are SrOH, ThF, ThCl, YbF and YbOH; each having been selected because of their proposed application. Specifically, SrOH is a candidate of constructing a molecular magneto-optical trap (MOT). The simple actinide molecules, ThF and ThCl, were selected as ligand bonding model systems to gain insight into chemical processing of Spent Nuclear Fuel. The lanthanides YbF and YbOH are venues for the determination of electron electric dipole moment (eEDM) and the studies in this dissertation provide the requisite properties for those experiments.
Intense supersonic molecular beams of these transient molecules were generated via laser ablation and spectroscopically characterized using a novel medium-resolution two-dimensional (2D) spectroscopic approach, as well as high-resolution laser induced fluorescence (LIF). The 2D medium resolution approach, which was used in the studies SrOH, ThF, ThCl and YbOH, uses a multiplexing method that simultaneously records dispersed fluorescence and excitation spectra. A significant advantage of 2D-LIF imaging is that all the electronics states can be targeted to determine the electronics states and associated vibrational spacing individually. Consequently, in the 2D spectra of ThF, ThCl and YbOH, several previously unobserved band systems have been detected in one single scan. For the DF spectra of SrOH and YbOH, the determined branching ratios show that the transitions of these molecules are diagonal (i.e. Δv=0), which is essential for the proposed potential for laser cooling. In the high-resolution of YbF, ThF, ThCl and SrOH optical spectra were recorded to an accuracy of ±30 MHz, which represents an unprecedented precision of 1:10+8.
In addition to field free spectra, optical Stark and Zeeman studies were performed to determine the most fundamental magneto-and electro-static properties. Effective Hamiltonian operators were employed to analyze the recorded spectra and determine the spectroscopic parameters. This data set also establishes a contribution toward developing new computational methodologies for treating relativistic effects and electron correlation.
Intense supersonic molecular beams of these transient molecules were generated via laser ablation and spectroscopically characterized using a novel medium-resolution two-dimensional (2D) spectroscopic approach, as well as high-resolution laser induced fluorescence (LIF). The 2D medium resolution approach, which was used in the studies SrOH, ThF, ThCl and YbOH, uses a multiplexing method that simultaneously records dispersed fluorescence and excitation spectra. A significant advantage of 2D-LIF imaging is that all the electronics states can be targeted to determine the electronics states and associated vibrational spacing individually. Consequently, in the 2D spectra of ThF, ThCl and YbOH, several previously unobserved band systems have been detected in one single scan. For the DF spectra of SrOH and YbOH, the determined branching ratios show that the transitions of these molecules are diagonal (i.e. Δv=0), which is essential for the proposed potential for laser cooling. In the high-resolution of YbF, ThF, ThCl and SrOH optical spectra were recorded to an accuracy of ±30 MHz, which represents an unprecedented precision of 1:10+8.
In addition to field free spectra, optical Stark and Zeeman studies were performed to determine the most fundamental magneto-and electro-static properties. Effective Hamiltonian operators were employed to analyze the recorded spectra and determine the spectroscopic parameters. This data set also establishes a contribution toward developing new computational methodologies for treating relativistic effects and electron correlation.
ContributorsNguyen, Duc Trung (Author) / Steimle, Timothy C (Thesis advisor) / Richert, Ranko (Committee member) / Chizmeshya, Andrew V.G. (Committee member) / Arizona State University (Publisher)
Created2019
Description
I present for the first time a broad-scale assessment of dissolved organic matter in the continental hot springs of Yellowstone National Park. The concentration of dissolved organic carbon in hot springs is highly variable, but demonstrates distinct trends with the geochemical composition of springs. The dissolved organic carbon concentrations are lowest in the hottest, most deeply sourced hot springs. Mixing of hydrothermal fluids with surface waters or reaction with buried sedimentary organic matter is typically indicated by increased dissolved organic carbon concentrations. I assessed the bulk composition of organic matter through fluorescence analysis that demonstrated different fluorescent components associated with terrestrial organic matter, microbial organic matter, and several novel fluorescent signatures unique to hot springs. One novel fluorescence signature is observed exclusively in acidic hot springs, and it is likely an end product of thermally-altered sedimentary organic matter. This acid-spring component precipitates out of solution under neutral or alkaline conditions and characterization of the precipitate revealed evidence for a highly condensed aromatic structure. This acid-spring component serves as a reliable tracer of acidic, hot water that has cycled through the subsurface. Overall, dissolved organic carbon concentrations and fluorescent features correlate with the inorganic indicators traditionally used to infer spring fluid mixing in the subsurface. Further, the fluorescence information reveals subtle differences in mixing between fluid phases that are not distinguishable through classic inorganic indicator species. My work assessing dissolved organic carbon in the Yellowstone National Park hot springs reveals that the organic matter in hydrothermal systems is different from that found in surface waters, and that the concentration and composition of hot spring dissolved organic matter reflects the subsurface geochemical and hydrological environment.
ContributorsNye, Joshua (Author) / Hartnett, Hilairy E (Thesis advisor) / Shock, Everett L (Committee member) / Jones, Anne K (Committee member) / Arizona State University (Publisher)
Created2020