Thesis
Theoretical investigations of surface-science phenomena and analysis of low-lying vibrational mode anharmonicity
Washington State University
Master of Science (MS), Washington State University
05/2020
DOI:
https://doi.org/10.7273/000004237
Handle:
https://hdl.handle.net/2376/125192
Abstract
In this day and age, computers, among all the other tasks they help us perform, can serve as invaluable tools in helping us understand chemistry and scientists across the globe are taking advantage of it. In recent years (and partially thanks to the advent of supercomputing), "first-principles" (or ab initio) calculations have allowed us to predict the properties of collections of atoms with no empirical input thus allowing for independent theoretical studies of chemical phenomena at this detailed scale. These calculations, although expensive, are extremely powerful and versatile as evidenced by their uses in a variety of fields from surface science to data science. This thesis is closely in line with the former field and uses these calculations to explore and rationalize phenomena observed in experimental surface-science-based studies to gain a comprehensive understanding of the chemistry observed in such studies from an atomistic point of view. In particular, we explore the interactions of two small probe molecules on a copper surface (propylene and propylene oxide), examining the electronic nature of their interactions with the surface and each other. Further, the information gleaned from these studies is applied in statistical mechanical calculations to understand how these molecules behave when including the effects of temperature and surface coverage. We also use theoretical calculations to gain insights into the reduction chemistry at metal-oxide interfaces of oxidized platinum-copper single-atom alloy surfaces. These calculations helped explain the atomic-scale underpinnings of the reduction kinetics observed on these oxidized substrates prepared through different synthesis protocols. Finally, the last chapter examines at applying previously-unused methods to the computation of anharmonic corrections in ab initio thermodynamical calculations. These are applied to computation of the Gibbs energy change of water trimer formation (from first principles) and the effects of these anharmonic corrections are discussed.
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Details
- Title
- Theoretical investigations of surface-science phenomena and analysis of low-lying vibrational mode anharmonicity
- Creators
- Kyle Groden
- Contributors
- Jean-Sabin McEwen (Advisor) - Washington State University, Chemical Engineering and Bioengineering, School of
- Awarding Institution
- Washington State University
- Academic Unit
- Chemical Engineering and Bioengineering, School of
- Theses and Dissertations
- Master of Science (MS), Washington State University
- Publisher
- Washington State University
- Identifiers
- 99900896421201842
- Language
- English
- Resource Type
- Thesis