Photoinduced heterogeneous electron transfer : ǂb spectroscopic investigation on perylene chromophores on TiO2 colloids

Author(s)Yan, Han
Date Accessioned2024-01-24T15:10:33Z
Date Available2024-01-24T15:10:33Z
Publication Date2023
SWORD Update2024-01-22T20:14:01Z
AbstractPhotoinduced heterogeneous electron transfer (HET) is fundamentally important in many physical, chemical, and biological processes, with a wide range of applications such as photocatalysis, sensors, dye-sensitized solar cells, photolithography, and artificial photosynthesis. In photoinduced HET, a photoexcited electron is transferred from a molecular donor state to multiple acceptor states in a semiconductor. These reactions can occur on time scales as short as a couple of femtoseconds. ☐ In this dissertation, HET is studied with ultrafast spectroscopy on HET systems comprised of perylene derivatives that are covalently bound to colloidal TiO2 surfaces. Perylene chromophores have been chosen for their electronic and optical properties, making them ideal model systems. The specific focus of this work involves the manipulation of the conformation and chemical structure of the linker group that attaches the perylene chromophore to the TiO2 surface. Ultrafast spectroscopy was employed to gain insights into dynamics, electronic coupling, vibrational states, and various effects such as vibronic, structural, and binding effects. ☐ Transient absorption and pump-degenerate four-wave mixing were the primary ultrafast spectroscopies used to study HET and the vibrational response of the system. The experimental results were compared with theoretical simulations from collaborators and revealed the importance of electronic-vibrational coupling on HET. Perylene chromophores with systematic changes in the substitution position and number of linker groups were compared, yielding unexpected results that were explained by vibronic effects, binding effects, as well as conformational effects.
AdvisorGundlach, Lars
DegreePh.D.
DepartmentUniversity of Delaware, Department of Chemistry and Biochemistry
DOIhttps://doi.org/10.58088/cjs2-bq38
Unique Identifier1428166503
URLhttps://udspace.udel.edu/handle/19716/33902
Languageen
PublisherUniversity of Delaware
URIhttps://www.proquest.com/pqdtlocal1006271/dissertations-theses/photoinduced-heterogeneous-electron-transfer/docview/2921858804/sem-2?accountid=10457
KeywordsPhotolithography
KeywordsMolecular donor state
KeywordsHeterogeneous electron transfer
KeywordsUltrafast spectroscopy
KeywordsPerylene chromophores
TitlePhotoinduced heterogeneous electron transfer : ǂb spectroscopic investigation on perylene chromophores on TiO2 colloids
TypeThesis
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