Utilizing Ultrafast Spectroscopy to Study Charge Separation for Solar Energy Conversion

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  • March 22, 2019
Creator
  • Gish, Melissa
    • Affiliation: College of Arts and Sciences, Department of Chemistry
Abstract
  • The ever-increasing demand for useable energy coupled with the depletion of fossil fuels require a shift to renewable energy resources. The dye-sensitized photoelectrosynthesis cell (DSPEC) takes inspiration from photosynthesis. The DSPEC is a tandem cell where a series of photon absorption and electron transfer events lead to water oxidation at a photoanode and CO2 reduction at a photocathode to store energy in chemical bonds (solar fuels). While overall efficiencies can be determined through electrochemistry, these methods fail to reveal information about underlying charge separation dynamics that may inhibit performance. To develop a fully realized picture of these dynamics, we need to utilize time-resolved transient absorption spectroscopy. This dissertation presents several systematic studies of charge separation dynamics on surfaces and in solution. We explored the thickness dependent interfacial dynamics of dye-sensitized core/shell films and how those dynamics change upon annealing these films. Next, we investigated the effects of immobilizing the dye on the surface with thin layers of a conductive metal oxide. Finally, we examined the length-dependent dynamics of a donor-acceptor system incorporating a thiophene oligomer donor and naphthalene diimide acceptors in solution. This work was made possible through extensive collaborations with the groups of Dr. Thomas J. Meyer and Dr. Kirk Schanze.
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Advisor
  • Dempsey, Jillian
  • Atkin, Joanna
  • Papanikolas, John
  • Waters, Marcey
  • Kanai, Yosuke
Degree
  • Doctor of Philosophy
Degree granting institution
  • University of North Carolina at Chapel Hill Graduate School
Graduation year
  • 2018
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