Synthetic Elucidation of Design Principles for Molecular QubitsPublic Deposited
Quantum information processing (QIP) is an emerging computational paradigm with the potential to enable a vast increase in computational power, fundamentally transforming fields from structural biology to finance. QIP employs qubits, or quantum bits, as its fundamental units of information, which can exist in not just the classical states of 0 or 1, but in a superposition of the two. In order to successfully perform QIP, this superposition state must be sufficiently long-lived. One promising paradigm for the implementation of QIP involves employing unpaired electrons in coordination complexes as qubits. This architecture is highly tunable and scalable, however coordination complexes frequently suffer from short superposition lifetimes, or T2. In order to capitalize on the promise of molecular qubits, it is necessary to develop a set of design principles that allow the rational synthesis of complexes with sufficiently long values of T2. n this dissertation, I report efforts to use the synthesis of series of complexes to elucidate design principles for molecular qubits. Chapter 1 details previous work by our group and others in the field. Chapter 2 details the first efforts of our group to determine the impact of varying spin and spin-orbit coupling on T2. Chapter 3 examines the effect of removing nuclear spins on coherence time, and reports a series of vanadyl bis(dithiolene) complexes which exhibit extremely long coherence lifetimes, in excess of the 100 μs threshold for qubit viability. Chapters 4 and 5 form two complimentary halves of a study to determine the exact relationship between electronic spin–nuclear spin distance and the effect of the nuclear spins on T2. Finally, chapter 6 suggests next directions for the field as a whole, including the potential for work in this field to impact the development of other technologies as diverse as quantum sensors and magnetic resonance imaging contrast agents.