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Utilizing Spin-Orbit Coupling to Manipulate the Properties of Inorganic Compounds

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Spin-orbit coupling (SOC) underlies myriad phenomena in chemistry and physics. Arbitrary manipulation of spin-orbit coupling would enable precise control over such parameters as magnetic anisotropy, the sensitivity of quantum sensors, and even the selectivity of certain catalytic processes. Herein, I describe my efforts directed towards utilizing SOC as a handle to tune the properties of both molecular magnets as well as both molecular and solid-state defect-based quantum bits. Chapter one provides a discussion of how SOC might be manipulated and a summary of our approach towards tuning it. Chapter two discusses an early success in enhancing magnetic anisotropy in a heterobimetallic molecular complex. Chapter three and four describe some insights that we gained throughout our study of transition metal-main group heterobimetallics featuring direct bonds between transition metals and main group metals. Chapters five and six describe my efforts to understand the role of spin-orbit coupling both in molecular and solid-state quantum bits. Chapter five details my early exploration of the coherence properties of two octacyanometallate ions with successively higher spin-orbit coupling constants. Chapter six describes my work in examining the relationship between specific phonon modes and the coherence properties of oxygen-deficient double perovskites.

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