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dc.contributor.advisorTroy Van Voorhis.en_US
dc.contributor.authorKowalczyk, Timothy Danielen_US
dc.contributor.otherMassachusetts Institute of Technology. Dept. of Chemistry.en_US
dc.date.accessioned2012-09-27T18:11:28Z
dc.date.available2012-09-27T18:11:28Z
dc.date.copyright2012en_US
dc.date.issued2012en_US
dc.identifier.urihttp://hdl.handle.net/1721.1/73432
dc.descriptionThesis (Ph. D.)--Massachusetts Institute of Technology, Dept. of Chemistry, 2012.en_US
dc.descriptionCataloged from student-submitted PDF version of thesis.en_US
dc.descriptionIncludes bibliographical references (p. 161-185).en_US
dc.description.abstractOur understanding of organic materials for solar energy conversion stands to benefit greatly from accurate, computationally tractable electronic structure methods for excited states. Here we apply two approaches based on density functional theory (DFT) to predict excitation energies and electron transfer parameters in organic chromophores and semiconductors in solution. First, we apply constrained DFT to characterize charge recombination in a photoexcited donor-acceptor dyad and to understand the photophysical behavior of a fluorescent sensor for aqueous zinc. Second, we discover that the delta-self-consistent-field ([Delta]SCF) approach to excited states in DFT offers accuracy comparable to that of the better-established but more indirect linear-response time-dependent DFT approach, and we offer some justification for the similarity. Finally, we investigate a spin-restricted analog of [Delta]SCF known as restricted open-shell Kohn-Sham (ROKS) theory. We resolve a known ambiguity in the formal solution of the ROKS equations for the singlet excited state by presenting a self-consistent implementation of ROKS with respect to the mixing angle between the two open shells. The excited state methods developed and applied in this work contribute to the expanding toolkit of electronic structure theory for challenging problems in the characterization and design of organic materials.en_US
dc.description.statementofresponsibilityby Timothy Daniel Kowalczyk.en_US
dc.format.extent185 p.en_US
dc.language.isoengen_US
dc.publisherMassachusetts Institute of Technologyen_US
dc.rightsM.I.T. theses are protected by copyright. They may be viewed from this source for any purpose, but reproduction or distribution in any format is prohibited without written permission. See provided URL for inquiries about permission.en_US
dc.rights.urihttp://dspace.mit.edu/handle/1721.1/7582en_US
dc.subjectChemistry.en_US
dc.titleExcited states and electron transfer in solution : models based on density functional theoryen_US
dc.typeThesisen_US
dc.description.degreePh.D.en_US
dc.contributor.departmentMassachusetts Institute of Technology. Dept. of Chemistry.en_US
dc.identifier.oclc809562721en_US


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