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There are two different approaches to alleviating the demand on Earth’s natural resources: increase energy efficiency or utilize renewable resources. Vanadium dioxide (VO2) thermochromic windows passively modulate infrared (IR) transparency, aiding in reducing undesirable heat exchange from outside to indoors. This occurs through a semiconductor to metal transition upon heating which is coupled with an optical change from IR transparent to IR absorbing, respectively. The metallic phase exhibits a plasmon resonance and we can control the local environment by embedding the VO2 nanoparticles in a high refractive index material (i.e. a polymer) where the plasmon absorption intensity increases as does the overall device performance. Alternatively, to increase the production of renewable energy, p-type dye sensitized solar cells (DSSCs) are studied as a precursor to tandem devices for solar fuel production. A novel p-type semiconductor (photocathode), lead titanate was identified through a material informatics approach and utilized in fundamental studies of the semiconductor-electrolyte interaction. By tuning the electrolyte composition to increase the concentration of an efficient electron scavenger, I2, the photocurrent and fill factor approximately doubled resulting in a four-fold increase in power conversion efficiency. Simply changing the concentration of I2, and electron scavenger, in the electrolyte allows for more efficient charge separation at the semiconductor-chromophore-electrolyte interface, which improves two of the most problematic device performance metrics in p-type DSSCs, low photocurrent and low fill factor. Winter 2017 2017 Chemistry eng Doctor of Philosophy Dissertation University of North Carolina at Chapel Hill Graduate School Degree granting institution Chemistry James Cahoon Thesis advisor Thomas Meyer Thesis advisor Gerald Meyer Thesis advisor Yosuke Kanai Thesis advisor Scott Warren Thesis advisor text Taylor Moot Creator Department of Chemistry College of Arts and Sciences Probing the Metal Oxide Local Environment for Thermochromic and Photovoltaic Applications Energy demand is predicted to increase by 28% between 2015 and 2040, placing strain on the current reserves of petroleum, coal and natural gas. There are two different approaches to alleviating the demand on Earth’s natural resources: increase energy efficiency or utilize renewable resources. Vanadium dioxide (VO2) thermochromic windows passively modulate infrared (IR) transparency, aiding in reducing undesirable heat exchange from outside to indoors. This occurs through a semiconductor to metal transition upon heating which is coupled with an optical change from IR transparent to IR absorbing, respectively. The metallic phase exhibits a plasmon resonance and we can control the local environment by embedding the VO2 nanoparticles in a high refractive index material (i.e. a polymer) where the plasmon absorption intensity increases as does the overall device performance. Alternatively, to increase the production of renewable energy, p-type dye sensitized solar cells (DSSCs) are studied as a precursor to tandem devices for solar fuel production. A novel p-type semiconductor (photocathode), lead titanate was identified through a material informatics approach and utilized in fundamental studies of the semiconductor-electrolyte interaction. By tuning the electrolyte composition to increase the concentration of an efficient electron scavenger, I2, the photocurrent and fill factor approximately doubled resulting in a four-fold increase in power conversion efficiency. Simply changing the concentration of I2, and electron scavenger, in the electrolyte allows for more efficient charge separation at the semiconductor-chromophore-electrolyte interface, which improves two of the most problematic device performance metrics in p-type DSSCs, low photocurrent and low fill factor. 2017-12 2017 Chemistry eng Doctor of Philosophy Dissertation University of North Carolina at Chapel Hill Graduate School Degree granting institution Chemistry James Cahoon Thesis advisor Thomas Meyer Thesis advisor Gerald Meyer Thesis advisor Yosuke Kanai Thesis advisor Scott Warren Thesis advisor text Taylor Moot Creator Department of Chemistry College of Arts and Sciences Probing the Metal Oxide Local Environment for Thermochromic and Photovoltaic Applications Energy demand is predicted to increase by 28% between 2015 and 2040, placing strain on the current reserves of petroleum, coal and natural gas. There are two different approaches to alleviating the demand on Earth’s natural resources: increase energy efficiency or utilize renewable resources. Vanadium dioxide (VO2) thermochromic windows passively modulate infrared (IR) transparency, aiding in reducing undesirable heat exchange from outside to indoors. This occurs through a semiconductor to metal transition upon heating which is coupled with an optical change from IR transparent to IR absorbing, respectively. The metallic phase exhibits a plasmon resonance and we can control the local environment by embedding the VO2 nanoparticles in a high refractive index material (i.e. a polymer) where the plasmon absorption intensity increases as does the overall device performance. Alternatively, to increase the production of renewable energy, p-type dye sensitized solar cells (DSSCs) are studied as a precursor to tandem devices for solar fuel production. A novel p-type semiconductor (photocathode), lead titanate was identified through a material informatics approach and utilized in fundamental studies of the semiconductor-electrolyte interaction. By tuning the electrolyte composition to increase the concentration of an efficient electron scavenger, I2, the photocurrent and fill factor approximately doubled resulting in a four-fold increase in power conversion efficiency. Simply changing the concentration of I2, and electron scavenger, in the electrolyte allows for more efficient charge separation at the semiconductor-chromophore-electrolyte interface, which improves two of the most problematic device performance metrics in p-type DSSCs, low photocurrent and low fill factor. 2017-12 2017 Chemistry eng Doctor of Philosophy Dissertation University of North Carolina at Chapel Hill Graduate School Degree granting institution Chemistry James Cahoon Thesis advisor Thomas Meyer Thesis advisor Gerald Meyer Thesis advisor Yosuke Kanai Thesis advisor Scott Warren Thesis advisor text Taylor Moot Creator Department of Chemistry College of Arts and Sciences Probing the Metal Oxide Local Environment for Thermochromic and Photovoltaic Applications Energy demand is predicted to increase by 28% between 2015 and 2040, placing strain on the current reserves of petroleum, coal and natural gas. There are two different approaches to alleviating the demand on Earth’s natural resources: increase energy efficiency or utilize renewable resources. Vanadium dioxide (VO2) thermochromic windows passively modulate infrared (IR) transparency, aiding in reducing undesirable heat exchange from outside to indoors. This occurs through a semiconductor to metal transition upon heating which is coupled with an optical change from IR transparent to IR absorbing, respectively. The metallic phase exhibits a plasmon resonance and we can control the local environment by embedding the VO2 nanoparticles in a high refractive index material (i.e. a polymer) where the plasmon absorption intensity increases as does the overall device performance. Alternatively, to increase the production of renewable energy, p-type dye sensitized solar cells (DSSCs) are studied as a precursor to tandem devices for solar fuel production. A novel p-type semiconductor (photocathode), lead titanate was identified through a material informatics approach and utilized in fundamental studies of the semiconductor-electrolyte interaction. By tuning the electrolyte composition to increase the concentration of an efficient electron scavenger, I2, the photocurrent and fill factor approximately doubled resulting in a four-fold increase in power conversion efficiency. Simply changing the concentration of I2, and electron scavenger, in the electrolyte allows for more efficient charge separation at the semiconductor-chromophore-electrolyte interface, which improves two of the most problematic device performance metrics in p-type DSSCs, low photocurrent and low fill factor. 2017-12 2017 Chemistry eng Doctor of Philosophy Dissertation University of North Carolina at Chapel Hill Graduate School Degree granting institution Chemistry James Cahoon Thesis advisor Thomas Meyer Thesis advisor Gerald Meyer Thesis advisor Yosuke Kanai Thesis advisor Scott Warren Thesis advisor text Taylor Moot Creator Department of Chemistry College of Arts and Sciences Probing the Metal Oxide Local Environment for Thermochromic and Photovoltaic Applications Energy demand is predicted to increase by 28% between 2015 and 2040, placing strain on the current reserves of petroleum, coal and natural gas. There are two different approaches to alleviating the demand on Earth’s natural resources: increase energy efficiency or utilize renewable resources. Vanadium dioxide (VO2) thermochromic windows passively modulate infrared (IR) transparency, aiding in reducing undesirable heat exchange from outside to indoors. This occurs through a semiconductor to metal transition upon heating which is coupled with an optical change from IR transparent to IR absorbing, respectively. The metallic phase exhibits a plasmon resonance and we can control the local environment by embedding the VO2 nanoparticles in a high refractive index material (i.e. a polymer) where the plasmon absorption intensity increases as does the overall device performance. Alternatively, to increase the production of renewable energy, p-type dye sensitized solar cells (DSSCs) are studied as a precursor to tandem devices for solar fuel production. A novel p-type semiconductor (photocathode), lead titanate was identified through a material informatics approach and utilized in fundamental studies of the semiconductor-electrolyte interaction. By tuning the electrolyte composition to increase the concentration of an efficient electron scavenger, I2, the photocurrent and fill factor approximately doubled resulting in a four-fold increase in power conversion efficiency. Simply changing the concentration of I2, and electron scavenger, in the electrolyte allows for more efficient charge separation at the semiconductor-chromophore-electrolyte interface, which improves two of the most problematic device performance metrics in p-type DSSCs, low photocurrent and low fill factor. 2017-12 2017 Chemistry eng Doctor of Philosophy Dissertation Chemistry James Cahoon Thesis advisor Thomas Meyer Thesis advisor Gerald Meyer Thesis advisor Yosuke Kanai Thesis advisor Scott Warren Thesis advisor text University of North Carolina at Chapel Hill Degree granting institution Taylor Moot Creator Department of Chemistry College of Arts and Sciences Probing the Metal Oxide Local Environment for Thermochromic and Photovoltaic Applications Energy demand is predicted to increase by 28% between 2015 and 2040, placing strain on the current reserves of petroleum, coal and natural gas. There are two different approaches to alleviating the demand on Earth’s natural resources: increase energy efficiency or utilize renewable resources. Vanadium dioxide (VO2) thermochromic windows passively modulate infrared (IR) transparency, aiding in reducing undesirable heat exchange from outside to indoors. This occurs through a semiconductor to metal transition upon heating which is coupled with an optical change from IR transparent to IR absorbing, respectively. The metallic phase exhibits a plasmon resonance and we can control the local environment by embedding the VO2 nanoparticles in a high refractive index material (i.e. a polymer) where the plasmon absorption intensity increases as does the overall device performance. Alternatively, to increase the production of renewable energy, p-type dye sensitized solar cells (DSSCs) are studied as a precursor to tandem devices for solar fuel production. A novel p-type semiconductor (photocathode), lead titanate was identified through a material informatics approach and utilized in fundamental studies of the semiconductor-electrolyte interaction. By tuning the electrolyte composition to increase the concentration of an efficient electron scavenger, I2, the photocurrent and fill factor approximately doubled resulting in a four-fold increase in power conversion efficiency. Simply changing the concentration of I2, and electron scavenger, in the electrolyte allows for more efficient charge separation at the semiconductor-chromophore-electrolyte interface, which improves two of the most problematic device performance metrics in p-type DSSCs, low photocurrent and low fill factor. 2017-12 2017 Chemistry eng Doctor of Philosophy Dissertation Chemistry James Cahoon Thesis advisor Thomas Meyer Thesis advisor Gerald Meyer Thesis advisor Yosuke Kanai Thesis advisor Scott Warren Thesis advisor text University of North Carolina at Chapel Hill Degree granting institution Taylor Moot Creator Department of Chemistry College of Arts and Sciences Probing the Metal Oxide Local Environment for Thermochromic and Photovoltaic Applications Energy demand is predicted to increase by 28% between 2015 and 2040, placing strain on the current reserves of petroleum, coal and natural gas. There are two different approaches to alleviating the demand on Earth’s natural resources: increase energy efficiency or utilize renewable resources. Vanadium dioxide (VO2) thermochromic windows passively modulate infrared (IR) transparency, aiding in reducing undesirable heat exchange from outside to indoors. This occurs through a semiconductor to metal transition upon heating which is coupled with an optical change from IR transparent to IR absorbing, respectively. The metallic phase exhibits a plasmon resonance and we can control the local environment by embedding the VO2 nanoparticles in a high refractive index material (i.e. a polymer) where the plasmon absorption intensity increases as does the overall device performance. Alternatively, to increase the production of renewable energy, p-type dye sensitized solar cells (DSSCs) are studied as a precursor to tandem devices for solar fuel production. A novel p-type semiconductor (photocathode), lead titanate was identified through a material informatics approach and utilized in fundamental studies of the semiconductor-electrolyte interaction. By tuning the electrolyte composition to increase the concentration of an efficient electron scavenger, I2, the photocurrent and fill factor approximately doubled resulting in a four-fold increase in power conversion efficiency. Simply changing the concentration of I2, and electron scavenger, in the electrolyte allows for more efficient charge separation at the semiconductor-chromophore-electrolyte interface, which improves two of the most problematic device performance metrics in p-type DSSCs, low photocurrent and low fill factor. 2017-12 2017 Chemistry eng Doctor of Philosophy Dissertation Chemistry James Cahoon Thesis advisor Thomas Meyer Thesis advisor Gerald Meyer Thesis advisor Yosuke Kanai Thesis advisor Scott Warren Thesis advisor text University of North Carolina at Chapel Hill Degree granting institution Taylor Moot Creator Department of Chemistry College of Arts and Sciences Probing the Metal Oxide Local Environment for Thermochromic and Photovoltaic Applications Energy demand is predicted to increase by 28% between 2015 and 2040, placing strain on the current reserves of petroleum, coal and natural gas. There are two different approaches to alleviating the demand on Earth’s natural resources: increase energy efficiency or utilize renewable resources. Vanadium dioxide (VO2) thermochromic windows passively modulate infrared (IR) transparency, aiding in reducing undesirable heat exchange from outside to indoors. This occurs through a semiconductor to metal transition upon heating which is coupled with an optical change from IR transparent to IR absorbing, respectively. The metallic phase exhibits a plasmon resonance and we can control the local environment by embedding the VO2 nanoparticles in a high refractive index material (i.e. a polymer) where the plasmon absorption intensity increases as does the overall device performance. Alternatively, to increase the production of renewable energy, p-type dye sensitized solar cells (DSSCs) are studied as a precursor to tandem devices for solar fuel production. A novel p-type semiconductor (photocathode), lead titanate was identified through a material informatics approach and utilized in fundamental studies of the semiconductor-electrolyte interaction. By tuning the electrolyte composition to increase the concentration of an efficient electron scavenger, I2, the photocurrent and fill factor approximately doubled resulting in a four-fold increase in power conversion efficiency. Simply changing the concentration of I2, and electron scavenger, in the electrolyte allows for more efficient charge separation at the semiconductor-chromophore-electrolyte interface, which improves two of the most problematic device performance metrics in p-type DSSCs, low photocurrent and low fill factor. 2017-12 2017 Chemistry eng Doctor of Philosophy Dissertation University of North Carolina at Chapel Hill Graduate School Degree granting institution Chemistry James Cahoon Thesis advisor Thomas Meyer Thesis advisor Gerald Meyer Thesis advisor Yosuke Kanai Thesis advisor Scott Warren Thesis advisor text Taylor Moot Creator Department of Chemistry College of Arts and Sciences Probing the Metal Oxide Local Environment for Thermochromic and Photovoltaic Applications Energy demand is predicted to increase by 28% between 2015 and 2040, placing strain on the current reserves of petroleum, coal and natural gas. There are two different approaches to alleviating the demand on Earth’s natural resources: increase energy efficiency or utilize renewable resources. Vanadium dioxide (VO2) thermochromic windows passively modulate infrared (IR) transparency, aiding in reducing undesirable heat exchange from outside to indoors. This occurs through a semiconductor to metal transition upon heating which is coupled with an optical change from IR transparent to IR absorbing, respectively. The metallic phase exhibits a plasmon resonance and we can control the local environment by embedding the VO2 nanoparticles in a high refractive index material (i.e. a polymer) where the plasmon absorption intensity increases as does the overall device performance. Alternatively, to increase the production of renewable energy, p-type dye sensitized solar cells (DSSCs) are studied as a precursor to tandem devices for solar fuel production. A novel p-type semiconductor (photocathode), lead titanate was identified through a material informatics approach and utilized in fundamental studies of the semiconductor-electrolyte interaction. By tuning the electrolyte composition to increase the concentration of an efficient electron scavenger, I2, the photocurrent and fill factor approximately doubled resulting in a four-fold increase in power conversion efficiency. Simply changing the concentration of I2, and electron scavenger, in the electrolyte allows for more efficient charge separation at the semiconductor-chromophore-electrolyte interface, which improves two of the most problematic device performance metrics in p-type DSSCs, low photocurrent and low fill factor. 2017-12 2017 Chemistry eng Doctor of Philosophy Dissertation Chemistry James Cahoon Thesis advisor Thomas Meyer Thesis advisor Gerald Meyer Thesis advisor Yosuke Kanai Thesis advisor Scott Warren Thesis advisor text University of North Carolina at Chapel Hill Degree granting institution Taylor Moot Creator Department of Chemistry College of Arts and Sciences Probing the Metal Oxide Local Environment for Thermochromic and Photovoltaic Applications Energy demand is predicted to increase by 28% between 2015 and 2040, placing strain on the current reserves of petroleum, coal and natural gas. There are two different approaches to alleviating the demand on Earth’s natural resources: increase energy efficiency or utilize renewable resources. Vanadium dioxide (VO2) thermochromic windows passively modulate infrared (IR) transparency, aiding in reducing undesirable heat exchange from outside to indoors. This occurs through a semiconductor to metal transition upon heating which is coupled with an optical change from IR transparent to IR absorbing, respectively. The metallic phase exhibits a plasmon resonance and we can control the local environment by embedding the VO2 nanoparticles in a high refractive index material (i.e. a polymer) where the plasmon absorption intensity increases as does the overall device performance. Alternatively, to increase the production of renewable energy, p-type dye sensitized solar cells (DSSCs) are studied as a precursor to tandem devices for solar fuel production. A novel p-type semiconductor (photocathode), lead titanate was identified through a material informatics approach and utilized in fundamental studies of the semiconductor-electrolyte interaction. By tuning the electrolyte composition to increase the concentration of an efficient electron scavenger, I2, the photocurrent and fill factor approximately doubled resulting in a four-fold increase in power conversion efficiency. Simply changing the concentration of I2, and electron scavenger, in the electrolyte allows for more efficient charge separation at the semiconductor-chromophore-electrolyte interface, which improves two of the most problematic device performance metrics in p-type DSSCs, low photocurrent and low fill factor. 2017-12 2017 Chemistry eng Doctor of Philosophy Dissertation James Cahoon Thesis advisor Thomas Meyer Thesis advisor Gerald Meyer Thesis advisor Yosuke Kanai Thesis advisor Scott Warren Thesis advisor text University of North Carolina at Chapel Hill Degree granting institution Moot_unc_0153D_17433.pdf uuid:24d84d1d-4a55-4815-b581-8063921bcae0 2019-12-31T00:00:00 2017-12-03T20:24:20Z proquest application/pdf 6424979