Abstract

The molecular design and photophysical characteristics of synthetic strongly coupled tetrapyrrole arrays are discussed. In these arrays, tetrapyrroles and auxillary chromophores such as perylenes are covalently connected by organic conjugated alkyne linkers, ensuring the strong electronic coupling among these chromophores. The intense electronic communication among these chromophores alter the nature of electronic structures in these chromophores, so the photophysical properties such as optical absorption/emission spectra and excited-state decay pathways are significantly changed from those of individual chromophores. The chemical structural factors such as linker position on each tetrapyrrole, linker identity, and the tetrapyrrole nature determine the electronic coupling nature. The first part describes how the electronic coupling between two identical hydroporphyrins (chlorin, bacteriochlorin) affects their electronic structures. The second part describes how the electronic coupling among different chromophores (porphyrin and perylenes) affects their electronic structures. The panchromatic absorption arisen from this type of electronic coupling is discussed, leading into the detailed study of the integrated molecular array of panchromatic absorption and charge separation. All these studies address the design strategy of synthetic strongly coupled tetrapyrrole arrays for solar-energy conversion and photomedicine.

Committee Chair

Dewey Holten

Committee Members

Robert Blankenship, Richard Mabbs, Liviu Mirica, Elijah Thimsen

Comments

Permanent URL: https://doi.org/10.7936/K7QN655W

Degree

Doctor of Philosophy (PhD)

Author's Department

Chemistry

Author's School

Graduate School of Arts and Sciences

Document Type

Dissertation

Date of Award

Winter 12-15-2016

Language

English (en)

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Available for download on Tuesday, December 15, 2116

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Chemistry Commons

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