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dc.contributor.advisorChairperson, Graduate Committee: Erik Grumstrupen
dc.contributor.authorHickey, Casey Lynnen
dc.contributor.otherAndrew H. Hill, Eric S. Massaro and Erik M. Grumstrup were co-authors of the article, 'Ultrafast excited-state transport and decay dynamics in cesium lead mixed halide perovskites' in the journal 'ACS energy letters' which is contained within this dissertation.en
dc.contributor.otherAndrew H. Hill and Erik M. Grumstrup were co-authors of the article, 'Screening links transport and recombination mechanisms in lead halide perovskites' in the journal 'The journal of physical chemistry C' which is contained within this dissertation.en
dc.contributor.otherErik M. Grumstrup was a co-author of the article, 'Direct correlation of charge carrier transport to local crystal quality in lead halide perovskites' submitted to the journal 'Nano letters' which is contained within this dissertation.en
dc.contributor.otherErik M. Grumstrup was a co-author of the article, 'A reduced artifact approach for determining diffusion coefficients in time-resolved microscopy' submitted to the journal 'The journal of physical chemistry C' which is contained within this dissertation.en
dc.date.accessioned2021-02-04T16:25:37Z
dc.date.available2021-02-04T16:25:37Z
dc.date.issued2020en
dc.identifier.urihttps://scholarworks.montana.edu/xmlui/handle/1/15880en
dc.description.abstractUnderstanding fundamental processes which drive the behavior of photoexcited charge carriers is essential to the development of novel semiconducting materials. The studies presented in this work combine ultrafast microscopy with a novel data analysis technique to provide an in-depth characterization of the excited state transport and recombination dynamics which occur in a series of lead halide perovskites. An investigation of the impact halide composition has on recombination dynamics in CsPbI 2Br revealed that trap-mediated recombination dominates at low fluences, with Auger recombination becoming increasingly important as the excitation density increases. Additionally, the average diffusivity measured for CsPbI 2Br (DA = 0.27 cm2/s) is nearly 10x lower than that observed in MAPbI 3. Further, it was determined that the dielectric constants relevant to photoexcited charge carriers in CsPbBr3 and MAPbBr3 perovskites (11.5 and 13, respectively) are intermediate between the high and low frequency limits, and that halide chemistry plays an integral role in determining the screening ability of lead halide perovskites. By correlating charge carrier diffusivities to locally measured crystal quality, it was found that solution processing methods can cause subtle lattice defects which act to impede transport and risk going undetected by bulk measurement techniques. Finally, to improve upon the traditional method for extracting diffusivities from transport measurements, which relies on perfectly Gaussian point spread functions, a new method was developed which instead relies on a numerical convolution of the actual point spread function with the diffusion equation. Compared to the traditional Gaussian method, the numerical convolution method proved to more accurately determine the diffusion coefficient, especially in the case of an anomalous point spread function.en
dc.language.isoenen
dc.publisherMontana State University - Bozeman, College of Letters & Scienceen
dc.subject.lcshCharge exchangeen
dc.subject.lcshEnergy levels (Quantum mechanics)en
dc.subject.lcshElectron microscopyen
dc.subject.lcshMetal halidesen
dc.subject.lcshPerovskiteen
dc.titleCharacterizing excited state transport and charge carrier dynamics in lead halide perovskitesen
dc.typeDissertationen
dc.rights.holderCopyright 2020 by Casey Lynn Hickeyen
thesis.degree.committeemembersMembers, Graduate Committee: Robert Walker; Mary J. Cloninger; Aleksander Rebane; Rufus L. Cone.en
thesis.degree.departmentChemistry & Biochemistry.en
thesis.degree.genreDissertationen
thesis.degree.namePhDen
thesis.format.extentfirstpage1en
thesis.format.extentlastpage134en
mus.data.thumbpage34en


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