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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. Spring 2018 2018 Physical chemistry Charge Separation, Oligothiophene, Ruthenium, Solar Energy, Spectroscopy, Ultrafast eng Doctor of Philosophy Dissertation University of North Carolina at Chapel Hill Graduate School Degree granting institution Chemistry John Papanikolas Thesis advisor Yosuke Kanai Thesis advisor Jillian Dempsey Thesis advisor Joanna Atkin Thesis advisor Marcey Waters Thesis advisor text Melissa Gish Author Department of Chemistry College of Arts and Sciences Utilizing Ultrafast Spectroscopy to Study Charge Separation for Solar Energy Conversion 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. Spring 2018 2018 Physical chemistry Charge Separation, Oligothiophene, Ruthenium, Solar Energy, Spectroscopy, Ultrafast eng Doctor of Philosophy Dissertation University of North Carolina at Chapel Hill Graduate School Degree granting institution Chemistry John Papanikolas Thesis advisor Yosuke Kanai Thesis advisor Jillian Dempsey Thesis advisor Joanna Atkin Thesis advisor Marcey Waters Thesis advisor text Melissa Gish Author Department of Chemistry College of Arts and Sciences Utilizing Ultrafast Spectroscopy to Study Charge Separation for Solar Energy Conversion 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. Spring 2018 2018 Physical chemistry Charge Separation, Oligothiophene, Ruthenium, Solar Energy, Spectroscopy, Ultrafast eng Doctor of Philosophy Dissertation University of North Carolina at Chapel Hill Graduate School Degree granting institution Chemistry John Papanikolas Thesis advisor Yosuke Kanai Thesis advisor Jillian Dempsey Thesis advisor Joanna Atkin Thesis advisor Marcey Waters Thesis advisor text Melissa Gish Author Department of Chemistry College of Arts and Sciences Utilizing Ultrafast Spectroscopy to Study Charge Separation for Solar Energy Conversion 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. Spring 2018 2018 Physical chemistry Charge Separation, Oligothiophene, Ruthenium, Solar Energy, Spectroscopy, Ultrafast eng Doctor of Philosophy Dissertation Chemistry John Papanikolas Thesis advisor Yosuke Kanai Thesis advisor Jillian Dempsey Thesis advisor Joanna Atkin Thesis advisor Marcey Waters Thesis advisor text University of North Carolina at Chapel Hill Degree granting institution Melissa Gish Creator Department of Chemistry College of Arts and Sciences Utilizing Ultrafast Spectroscopy to Study Charge Separation for Solar Energy Conversion 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. Physical chemistry Charge Separation; Oligothiophene; Ruthenium; Solar Energy; Spectroscopy; Ultrafast eng Doctor of Philosophy Dissertation Chemistry John Papanikolas Thesis advisor Yosuke Kanai Thesis advisor Jillian Dempsey Thesis advisor Joanna Atkin Thesis advisor Marcey Waters Thesis advisor text University of North Carolina at Chapel Hill Degree granting institution 2018 2018-05 Melissa Gish Author Department of Chemistry College of Arts and Sciences Utilizing Ultrafast Spectroscopy to Study Charge Separation for Solar Energy Conversion 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. Spring 2018 2018 Physical chemistry Charge Separation, Oligothiophene, Ruthenium, Solar Energy, Spectroscopy, Ultrafast eng Doctor of Philosophy Dissertation University of North Carolina at Chapel Hill Graduate School Degree granting institution Chemistry John Papanikolas Thesis advisor Yosuke Kanai Thesis advisor Jillian Dempsey Thesis advisor Joanna Atkin Thesis advisor Marcey Waters Thesis advisor text Melissa Gish Creator Department of Chemistry College of Arts and Sciences 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. 2018-05 2018 Physical chemistry Charge Separation; Oligothiophene; Ruthenium; Solar Energy; Spectroscopy; Ultrafast eng Doctor of Philosophy Dissertation University of North Carolina at Chapel Hill Graduate School Degree granting institution John Papanikolas Thesis advisor Yosuke Kanai Thesis advisor Jillian Dempsey Thesis advisor Joanna Atkin Thesis advisor Marcey Waters Thesis advisor text Gish_unc_0153D_17610.pdf uuid:b4319cca-4831-4b49-98cd-cb81e901c816 2020-06-13T00:00:00 2018-04-09T21:53:56Z proquest application/pdf 4965698