Computational Investigation of the Oxygen Evolving Complex of Photosystem II and Related Models via Density Functional Theory
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Terrett, Richard Norman Leslie
Description
The first step of photosynthetic metabolism effects the facile oxidation of water to dioxygen and hydrogen cations. This is achieved through an incompletely-understood process of light-driven four-electron oxidation at the Mn4CaO5 cofactor of the Oxygen Evolving Complex (OEC) of the Photosystem II (PSII) holoenzymatic complex in photosynthetic autotrophs. Biomimesis of this reaction—artificial photosynthesis—may offer energy-efficient routes to industrial...[Show more]
dc.contributor.author | Terrett, Richard Norman Leslie | |
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dc.date.accessioned | 2017-11-13T01:40:04Z | |
dc.date.available | 2017-11-13T01:40:04Z | |
dc.identifier.other | b48528973 | |
dc.identifier.uri | http://hdl.handle.net/1885/133592 | |
dc.description.abstract | The first step of photosynthetic metabolism effects the facile oxidation of water to dioxygen and hydrogen cations. This is achieved through an incompletely-understood process of light-driven four-electron oxidation at the Mn4CaO5 cofactor of the Oxygen Evolving Complex (OEC) of the Photosystem II (PSII) holoenzymatic complex in photosynthetic autotrophs. Biomimesis of this reaction—artificial photosynthesis—may offer energy-efficient routes to industrial hydrogen generation and value-added derivatives, with implications for solar energy fixation. This thesis consists of a compilation of four publications relating to Density Functional Theory (DFT) studies of structural and spectroscopic aspects of the OEC of PSII. These publications consist of research resolving the basis of structural anomalies in metal-substituted PSII, combinatoric simulation of difference spectra corresponding to proton-coupled oxido-reduction scenarios of PSII models, simulation of the hyperfine and superexchange magnetic interactions in PSII models, and the development of a methodology for obtaining vibrational intensities in the Mobiel Block Hessian (MBH) approximation, with applications to accelerated modeling of the vibrational structure of complex models of PSII, as well as other large molecules. These publications are presented alongside explanatory introductions and preceded by a general survey of the state of the art of photosynthesis research, context for the relevance of this research, and methodological discussion. Concluding remarks are also presented. | |
dc.language.iso | en | |
dc.subject | Photosynthesis | |
dc.subject | Photosystem II | |
dc.subject | Density Functional Theory | |
dc.subject | Computational Chemistry | |
dc.subject | Quantum Chemistry | |
dc.subject | Theoretical Chemistry | |
dc.subject | Electronic Structure | |
dc.subject | Molecular Structure | |
dc.subject | Biomimesis | |
dc.subject | Bioinorganic Chemistry | |
dc.subject | Vibrational Structure | |
dc.subject | Mobile Block Hessian | |
dc.subject | Infrared Difference Spectroscopy | |
dc.subject | Hyperfine Interaction | |
dc.subject | Magnetic Structure | |
dc.subject | Superexchange Interaction | |
dc.subject | Protein | |
dc.subject | Metalloprotein | |
dc.subject | Enzyme | |
dc.subject | Joliot-Kok Cycle | |
dc.subject | Artificial Photosynthesis | |
dc.subject | Water Oxidation | |
dc.subject | Water Splitting | |
dc.subject | Renewable Energy | |
dc.subject | Green Energy | |
dc.subject | Proton-Coupled Electron Transfer | |
dc.subject | Oxygen Evolving Complex | |
dc.subject | Water Oxidising Complex | |
dc.subject | Water Oxidizing Complex | |
dc.subject | Chloroplast | |
dc.subject | Thylakoid Membrane | |
dc.subject | Forster Resonance | |
dc.title | Computational Investigation of the Oxygen Evolving Complex of Photosystem II and Related Models via Density Functional Theory | |
dc.type | Thesis (PhD) | |
local.contributor.supervisor | Stranger, Robert | |
local.contributor.supervisorcontact | rob.stranger@anu.edu.au | |
dcterms.valid | 2017 | |
local.description.notes | the author deposited 13/11/17 | |
local.type.degree | Doctor of Philosophy (PhD) | |
dc.date.issued | 2017 | |
local.contributor.affiliation | Research School of Chemistry, The Australian National University | |
local.identifier.doi | 10.25911/5d70f1171441f | |
local.mintdoi | mint | |
Collections | Open Access Theses |
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