Reactive Organometallic Complexes and Ligand Design for Catalysis, Actinide Complexation, and Thin Film Deposition

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The Emslie research program is focused on the design and synthesis of unique metal-containing molecules (typically highly reactive molecules) which can provide new understanding of chemical bonding and reactivity, and can advance specific applications. These applications include catalytic reactions to manufacture new organic molecules and materials including polymers, methods to deposit currently inaccessible ultra-thin films during microprocessor and memory device fabrication, and chemical techniques to separate actinide metals from other metals. In research area 1, we will synthesize uncommonly rigid metal-binding molecules (ligands) which have been designed to tightly control the metal binding environment for a specific purpose. These ligands will be used to prepare and study the structures of extremely uncommon rare earth, actinide and group 4 alkyl dications which are both highly reactive and thermally robust, thereby enabling the study of their structures and reactivity, and the development of applications in catalysis (e.g. alkene polymerization and hydroelementation). Furthermore, they will be used to prepare actinide complexes featuring unprecedented actinide-ligand interactions. Study of these molecules will provide a better understanding of the bonding in actinide complexes, and may point the way towards improved methods for actinide separation in environmental radiochemistry and actinide recycling. Research area 2 is focused on the synthesis and applications of highly reactive molecules (those containing metal-carbon linkages) for thin film deposition using Atomic Layer Deposition (ALD). ALD is arguably the only technique capable of depositing the ultra-thin and highly conformal (i.e. surface hugging) films which will be required in future microprocessors and memory devices, especially when deposition is required on surfaces with nano-scale features such as deep trenches. However, film growth in ALD relies upon surface-based reactions between molecules, and in many cases, suitable molecules and reactions have yet to be conceived. Thermal ALD of pure metals is particularly challenging, and has not been achieved for most early and mid transition metals. In this research, we will develop unique molecules and reactions to enable ALD of currently inaccessible early and mid transition metal thin films; those required to manufacture future technological devices. In research area 3, we will work towards the development of broadly-applicable new routes to metal-containing molecules which feature ligands with multiple bonds to elements such as silicon. This work builds upon several recent Emslie group publications in the chemistry of manganese, and targets rare or unprecedented metal-ligand interactions of fundamental interest. The structures, bonding, and reactivity of the resulting metal-containing molecules will be investigated, and their potential involvement in catalytic reactions, such as alkene hydrosilylation, will be explored.