Development of guidelines towards an understanding of the structure of the cation - structure of the hybrid haloplumbate material relationship
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Tremblay, Marie-Helene
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Abstract
Organic-inorganic hybrid haloplumbate materials have attracted ever-increasing interest in the last ten years, initially due to their incorporation in high efficiency solar cells, but increasingly due to their utility in a variety of technological applications (e.g. light emitting diodes, transistors, laser, catalysis). By mixing PbI2 with an organic cation, one can synthesize 3D, 2D, 1D and 0D perovskite or perovskitoid compounds depending on the cation used. This thesis is concerned with identifying structural factors of the organic cation that influence the observed structures of low- dimensional organic lead-iodide perovskites and perovskitoids. This understanding is necessary to develop design strategies that enable one to predict the structure of the perovskite and perovskitoid based on the organic cation used. As previously suggested, it was found that both the interaction between adjacent cations or between the inorganic layer and the organic cation have structure directing roles in perovskites and perovskitoids. In each class of cations examined, the cation- cation and cation-inorganic layer interactions that determine the structures are discussed. An understanding of how the structure of the cation determines the structure of the hybrid material helps modify materials properties such as stability and optical properties.
The first chapter surveys the structural types adopted by organic iodoplumbates reported in the literature. Following, several studies are described in which 34 crystal structures are determined for families of compounds including 2D perovskites with substituted phenylethylammonium and benzylammonium cations, a corrugated 2D structure using the 4-nitrophenylethylammonium cation, and 1D perovskitoids. The final chapter summarizes the findings of the thesis, and puts them in a broader perspective, comparing them to related structural relationships among previously reported structures, recapitulates how this thesis has improved our understanding of the cation structure – iodoplumbate structure relationships, and suggests future directions.
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2020-07-21
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Dissertation