{"id":{"repo_id":"houston","oai_identifier":"oai:uh-ir.tdl.org:10657/3958"},"canonical_url":"https://search.dev.ndltd.org/etd/houston/oai:uh-ir.tdl.org:10657/3958","repository":{"repo_id":"houston","name":"University of Houston","base_url":"https://uh-ir.tdl.org/server/oai/request"},"display":{"title":"The Role of Disorder in the Charge Dissociation and Recombination Processes of Organic Photovoltaic Materials","abstract":"Organic Photovoltaic devices (OPVs) are becoming adequately cost and energy efficient to be considered a good investment and it is, therefore, especially important to have a concrete understanding of their operation. In this work, we use a fully quantum mechanical model of the electronic states of a bulk-heterojunction interface to investigate how presence of disorder in OPVs affects the recombination of triplet charge-transfer states and influences the free energy of an electron as it separates away from the interface into the free carrier phase. Our model simplifies complicated molecular structures to a lattice system, while taking into account electron and hole Coulombic and exchange interactions, lattice vibrations, and electron-phonon couplings. In addition, we examine the role of band-width and interfacial driving forces in determining the dissociation free energy of an electron/hole pair. With proper statistical treatment of the CT energies we recover experimentally observed ''hot'' and "cold'' exciton dissociation pathways. We also recover experimental values for the open-circuit voltage for the systems with 50-100 meV of energy disorder. Our model combines quantum and statistical treatments of a system with the large number of parameters and all possible electron-hole configurations to give results that provide a unifying picture linking various proposed mechanisms for charge separation. With many different theoretical tools and protocols available, our model stands out as combines scalability of molecular dynamics simulations with quantum mechanical treatment of electronics states.","abstract_html":"Organic Photovoltaic devices (OPVs) are becoming adequately cost and energy efficient to be considered a good investment and it is, therefore, especially important to have a concrete understanding of their operation. In this work, we use a fully quantum mechanical model of the electronic states of a bulk-heterojunction interface to investigate how presence of disorder in OPVs affects the recombination of triplet charge-transfer states and influences the free energy of an electron as it separates away from the interface into the free carrier phase. Our model simplifies complicated molecular structures to a lattice system, while taking into account electron and hole Coulombic and exchange interactions, lattice vibrations, and electron-phonon couplings. In addition, we examine the role of band-width and interfacial driving forces in determining the dissociation free energy of an electron/hole pair. With proper statistical treatment of the CT energies we recover experimentally observed ''hot'' and "cold'' exciton dissociation pathways. We also recover experimental values for the open-circuit voltage for the systems with 50-100 meV of energy disorder. Our model combines quantum and statistical treatments of a system with the large number of parameters and all possible electron-hole configurations to give results that provide a unifying picture linking various proposed mechanisms for charge separation. With many different theoretical tools and protocols available, our model stands out as combines scalability of molecular dynamics simulations with quantum mechanical treatment of electronics states.","abstract_has_math":false,"creators":["Lankevich, Vladimir 1991-"],"institution":"University of Houston","degree_name":"Doctor of Philosophy","degree_level":"Doctoral","degree_discipline":"Chemistry","degree_department":null,"school":null,"contributors":[],"advisors":["Bittner, Eric R."],"committee_chairs":[],"committee_members":["Lubchenko, Vassiliy","Su, Wu-Pei","Smith, Mark","Brgoch, Jakoah"],"year":2018,"date_issued":"2018-08","date_published":"2018-08","updated_at":"2026-07-24T02:32:47Z","subjects":["Organic photovoltaics","Exciton","Disorder","Lattice Model","Entropy"],"languages":["eng"],"rights":["The author of this work is the copyright owner. UH Libraries and the Texas Digital Library have their permission to store and provide access to this work. 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In this work, we use a fully quantum mechanical model of the electronic states of a bulk-heterojunction interface to investigate how presence of disorder in OPVs affects the recombination of triplet charge-transfer states and influences the free energy of an electron as it separates away from the interface into the free carrier phase. Our model simplifies complicated molecular structures to a lattice system, while taking into account electron and hole Coulombic and exchange interactions, lattice vibrations, and electron-phonon couplings. In addition, we examine the role of band-width and interfacial driving forces in determining the dissociation free energy of an electron/hole pair. With proper statistical treatment of the CT energies we recover experimentally observed ''hot'' and "cold'' exciton dissociation pathways. We also recover experimental values for the open-circuit voltage for the systems with 50-100 meV of energy disorder. Our model combines quantum and statistical treatments of a system with the large number of parameters and all possible electron-hole configurations to give results that provide a unifying picture linking various proposed mechanisms for charge separation. With many different theoretical tools and protocols available, our model stands out as combines scalability of molecular dynamics simulations with quantum mechanical treatment of electronics states."]},{"key":"dc:format.mimetype","label":"Dc Format Mimetype","values":["application/pdf"]},{"key":"dc:title","label":"Title","values":["The Role of Disorder in the Charge Dissociation and Recombination Processes of Organic Photovoltaic Materials"]}]}],"canonical_facts":{"dc:contributor.advisor":["Bittner, Eric R."],"dc:contributor.committeemember":["Lubchenko, Vassiliy","Su, Wu-Pei","Smith, Mark","Brgoch, Jakoah"],"dc:creator":["Lankevich, Vladimir 1991-"],"dc:date.accessioned":["2019-05-23T13:12:47Z"],"dc:date.issued":["2018-08"],"dc:description.abstract":["Organic Photovoltaic devices (OPVs) are becoming adequately cost and energy efficient to be considered a good investment and it is, therefore, especially important to have a concrete understanding of their operation. In this work, we use a fully quantum mechanical model of the electronic states of a bulk-heterojunction interface to investigate how presence of disorder in OPVs affects the recombination of triplet charge-transfer states and influences the free energy of an electron as it separates away from the interface into the free carrier phase. Our model simplifies complicated molecular structures to a lattice system, while taking into account electron and hole Coulombic and exchange interactions, lattice vibrations, and electron-phonon couplings. In addition, we examine the role of band-width and interfacial driving forces in determining the dissociation free energy of an electron/hole pair. With proper statistical treatment of the CT energies we recover experimentally observed ''hot'' and "cold'' exciton dissociation pathways. We also recover experimental values for the open-circuit voltage for the systems with 50-100 meV of energy disorder. Our model combines quantum and statistical treatments of a system with the large number of parameters and all possible electron-hole configurations to give results that provide a unifying picture linking various proposed mechanisms for charge separation. With many different theoretical tools and protocols available, our model stands out as combines scalability of molecular dynamics simulations with quantum mechanical treatment of electronics states."],"dc:format.mimetype":["application/pdf"],"dc:identifier.uri":["https://hdl.handle.net/10657/3958"],"dc:language.iso":["eng"],"dc:rights":["The author of this work is the copyright owner. UH Libraries and the Texas Digital Library have their permission to store and provide access to this work. Further transmission, reproduction, or presentation of this work is prohibited except with permission of the author(s)."],"dc:subject":["Organic photovoltaics","Exciton","Disorder","Lattice Model","Entropy"],"dc:title":["The Role of Disorder in the Charge Dissociation and Recombination Processes of Organic Photovoltaic Materials"],"thesis:degree_discipline":["Chemistry"],"thesis:degree_level":["Doctoral"],"thesis:degree_name":["Doctor of Philosophy"],"thesis:institution_name":["University of Houston"]},"updated_at":"2026-07-24T02:32:47Z"}