Excited-State Studies with the Constricted Variational Density Functional Theory (CV-DF) Method

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atmire.migration.oldid4226
dc.contributor.advisorRauk, Arvi
dc.contributor.advisorZiegler, Tom (deceased)
dc.contributor.authorSeidu, Issaka
dc.contributor.committeememberSalahub, Dennis
dc.contributor.committeememberMacCallum, Justin
dc.contributor.committeememberNooijen, Marcel
dc.contributor.committeememberSanders, Barry
dc.date.accessioned2016-04-08T18:40:43Z
dc.date.available2016-04-08T18:40:43Z
dc.date.issued2016
dc.date.submitted2016en
dc.description.abstractTheoretical calculations have played a vital role in understanding electronic properties of chemically and electronically relevant systems. Some of the roles played by theoretical approaches include the assignment and interpretation of spectra of chemical species such as the transition metal (TM) complexes. However, before these theoretical methods can be used as predictive tools in the chemical analysis of compounds for which experimental results are unavailable, the performance and scope of applicability of these methods must be well understood and improvements made wherever necessary. In this work, the Constricted Variational Density Functional Theory (CV-DFT) method is used in detailed analyses of excited-state properties of TM and other chemical species. Studies are carried out with the CV-DFT method in areas where the adiabatic Time-Dependent Density Functional Theory (ATD-DFT) method have been found insufficient, such as charge transfer (CT) and Rydberg excitations, as well as areas where ATD-DFT performed well. This was done to ensure that, the CV-DFT method not only show good performance for excitations poorly described by ATD-DFT but those that are sufficiently described as well. For a better understanding of the strengths and weaknesses of the CV-DFT methods, our calculated results are compared to experimental and/or high level ab initio results whenever available. Finally, an extension is made to CV-DFT for double excitation. These double excitations are known to be important for excited-state studies in conjugated systems such as the polyenes. Future work will be carried to examine the performance of this method. We find, in general, that CV-DFT shows accurate performance for excitations that are poorly described by the ATD-DFT method, and comparable performance for excitations in which ATD-DFT performs adequately.en_US
dc.identifier.citationSeidu, I. (2016). Excited-State Studies with the Constricted Variational Density Functional Theory (CV-DF) Method (Doctoral thesis, University of Calgary, Calgary, Canada). Retrieved from https://prism.ucalgary.ca. doi:10.11575/PRISM/26035en_US
dc.identifier.doihttp://dx.doi.org/10.11575/PRISM/26035
dc.identifier.urihttp://hdl.handle.net/11023/2882
dc.language.isoeng
dc.publisher.facultyGraduate Studies
dc.publisher.institutionUniversity of Calgaryen
dc.publisher.placeCalgaryen
dc.rightsUniversity of Calgary graduate students retain copyright ownership and moral rights for their thesis. You may use this material in any way that is permitted by the Copyright Act or through licensing that has been assigned to the document. For uses that are not allowable under copyright legislation or licensing, you are required to seek permission.
dc.subjectChemistry--Inorganic
dc.subjectChemistry--Physical
dc.subjectMathematics
dc.subjectPhysics--Molecular
dc.subject.classificationDensity Functional Theory (DFT)en_US
dc.subject.classificationExcitationen_US
dc.subject.classificationExcited-state studiesen_US
dc.subject.classificationTransition metalen_US
dc.subject.classificationCV-DFTen_US
dc.subject.classificationSpin-flipen_US
dc.subject.classificationETS-NOCVen_US
dc.subject.classificationDouble elctron excitationen_US
dc.subject.classificationRydbergen_US
dc.subject.classificationCharge-transferen_US
dc.subject.classificationDensityen_US
dc.titleExcited-State Studies with the Constricted Variational Density Functional Theory (CV-DF) Method
dc.typedoctoral thesis
thesis.degree.disciplineChemistry
thesis.degree.grantorUniversity of Calgary
thesis.degree.nameDoctor of Philosophy (PhD)
ucalgary.item.requestcopytrue
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