The research discussed in this dissertation spans both synthetic inorganic and nanomaterials chemistry. Aluminum hydride complexes have been synthesized and characterized which are highly volatile and thermally stable and their potential as reducing agents for ALD of electropositive metal and metal-containing films was evaluated. A major discovery has been the deposition of aluminum metal films by thermal ALD using an aluminum dihydride complex supported by a simple amido-amine ligand (Chapters 2). Aluminum is the most electropositive element deposited by purely thermal ALD to date and represents a significant breakthrough for this field. This process may have important industrial applications and the aluminum hydride reducing agents should enable a variety of novel ALD processes for metals and elements. The deposition of titanium metal films by ALD was attempted using the aluminum hydride reducing agents (Chapter 3). Rather than pure titanium films, highly thermodynamically stable titanium carbonitride (TiCxNy) films were deposited instead. Chapter 4 explored the ubiquitous ALD precursor trimethylaluminum (AlMe3) as a potential reducing agent and high quality tungsten carbide films were deposited using AlMe3 and WCl6. Tungsten-rich tungsten carbide films were deposited using WCl¬6 and an aluminum hydride reducing agent instead of AlMe3 (Chapter 5). While exploring the chemistry and properties of N-heterocyclic carbene aluminum hydride complexes, a structurally unusual dialane complex was synthesized which displayed good volatility and thermal stability and it was used to deposit aluminum metal by a thermal ALD process (Chapter 6)
