In this dissertation, we address some of the needs faced in the development of modern ab initio quantum chemical methods to compute
high-accuracy ground and excited electronic states. Chapters 1 and 2 should be seen as introductory Chapters, where the mathematical
foundations of modern electronic structure theory necessary to understand this work are laid down. Chapters 3 and 4 covers the development of
methods and algorithms relevant to ground state computations. We propose a semi-definite-based algorithm to compute ground-state Hartree-Fock
energies and wave functions, that can be easily extended to Kohn-Sham density functional theory. We also propose a parametrized coupled-pair
functional to compute accurate non-covalent molecular interaction energies. Chapters 3 through 7 cover methods relevant to excited state
computations. We propose an explicitly time-dependent coupled-cluster framework rooted on the equation-of-motion formalism to compute linear
absorption spectra of molecular systems. The method is further expanded by recasting a linear absorption line shape function in terms of Pad
́e approximants. The expanded method is shown to be an efficient tool for the simulation of near-edge X-ray absorption fine structure.
Finally, we propose a time-dependent Hartree-Fock method within the framework of cavity quantum-electrodynamics that allows us to simulate
the interaction of molecular systems with quantized radiation fields, such as those found on plasmonic nanoparticles and nano
cavities. / A Dissertation submitted to the Department of Chemistry and Biochemistry in partial fulfillment of the
requirements for the degree of Doctor of Philosophy. / Fall Semester 2017. / November 15, 2017. / Includes bibliographical references. / Albert Eugene DePrince, III, Professor Directing Dissertation; Sachin Shanbhag, University
Representative; Naresh Dalal, Committee Member; Oliver Steinbock, Committee Member.
| Identifer | oai:union.ndltd.org:fsu.edu/oai:fsu.digital.flvc.org:fsu_604997 |
| Contributors | Nascimento, Daniel R. (Daniel Ricardo) (author), DePrince, A. Eugene (Albert Eugene) (professor directing dissertation), Shanbhag, Sachin (university representative), Dalal, Naresh S. (committee member), Steinbock, Oliver (committee member), Florida State University (degree granting institution), College of Arts and Sciences (degree granting college), Department of Chemistry and Biochemistry (degree granting departmentdgg) |
| Publisher | Florida State University |
| Source Sets | Florida State University |
| Language | English, English |
| Detected Language | English |
| Type | Text, text, doctoral thesis |
| Format | 1 online resource (168 pages), computer, application/pdf |
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