Molecular Quantum Cellular Automata: Synthesis and Characterization

Molecular quantum cellular automata (QCA) is a computing paradigm that solves many of the problems plaguing current microprocessors. Molecules suitable for QCA are generally mixed-valent and organometallic in nature. The aim of this thesis is to describe the synthesis and characterization of a variety of molecules. The majority of the molecules were targeted with the aim of studying their utility for molecular QCA. This thesis is a portion of a larger collaborative work that includes work from the labs of Lent, Snider, Kandel, and Corcelli at the University of Notre Dame.

The introduction builds context for the majority of the work done in this dissertation. This includes a brief introduction to QCA and electron transfer in molecular systems.

Chapter 2 focuses on the synthesis and characterization of a variety of substituted 1,2-diferrocenylacetylenes. The synthesis of substituted 1,2-diferrocenylacetylenes supports two goals: to study substituent effects on electron transfer and redox chemistry in the 1,2-diferrocenylacetylene system, and to synthesize precursors for the preparation of more complex molecules found in later chapters.

Chapter 3 focuses on the synthetic extension of substituted 1,2-diferrocenylacetylene compounds from Chapter 2 to square planar tetraferrocenyl compounds. This supports two goals: incorporating functionality that allows for the exploration of supramolecular interactions on surfaces with our scanning tunneling microscopy (STM) collaborators, and incorporating functionality to prevent thermal motion during STM imaging.

Chapter 4 focuses on the synthesis, oxidation, and characterization of a series of ferrocene substituted carboranes. Emphasis is placed on the characterization of electron transfer within 7-Fc-8-Fc⁺-7,8-nido-[C₂B₉H₁₀­_­­]^- (4.3), which is found to be bridge mediated.

Chapter 5 focuses on the synthesis and structural characterization of 1,2-Fc-1,2-closo-C₂B₁₀H₁₀ (5.1). The compound is also explored computationally. Possible synthetic routes are discussed in the future work section with the intent of creating alternate metal analogues of this interesting compound.

Chapter 6 is from an earlier, unrelated project. The focus of Chapter 6 is the synthesis of imidazolium-containing metal organic frameworks with the end goal of utilizing these materials for gas separation, specifically, CO₂ from N₂. The work outlined in this chapter is incomplete due to a change in project focus.