The emerging paradigm of quantum information science (QIS) vows to transform a wide range of fields, such as computation, communication, and sensing. The fundamental unit at the core of any QIS system is a quantum bit, or qubit. Rather than be restricted to one of two classical states (0 or 1), a qubit can be manipulated into any superposition of its two quantum states. The realization of a QIS system is predicated on the design of viable qubits, necessitating long superposition lifetimes, scalability, initialization, and readout at the single qubit level. Electronic spins in paramagnetic coordination compounds are an attractive platform to realize viable qubit candidates given the inherent tunability of their electronic structure using ligand field theory and synthetic chemistry. Notably, coordination compounds enable access to S > ½ spins states, permitting us to exploit their tunable electronic structures to tailor their quantum properties, design multi-qubit species, and imbue them with electronic structures that facilitate spin polarization and optical readout to satisfy the exhaustive criteria for a viable qubit. In this dissertation, I explore the relaxation dynamics of coordination compounds and examine the suitability of their electronic structure to QIS applications. Chapter one provides a brief review of recent results from our group aimed at accessing long superposition lifetimes and scalability of qubits into arrays. Chapter two examines the impact of metal-ligand covalency on spin-lattice and spin-spin relaxation in vanadium(IV) and copper(II) complexes. Chapter 3 dissects the dichotomy of design principles for qubits versus single-molecule magnets (SMM). Chapter 4 explores how subtle changes in the local coordination environment of a SMM can have drastic effects on its electronic structure, transforming a coordination compound from a molecular magnet to a qubit candidate. Chapter 5 reports the use of the previously learned design principles to access a single molecule housing two qubits within its ground state electronic structure. Chapter six discusses our future goals and strategies towards enabling optical addressability of molecular qubits by imbuing them with an optically induced spin polarization mechanism to enable optically detected magnetic resonance at the single molecule level.

Creator

• Fataftah, Majed

DOI

• https://doi.org/10.21985/n2-k60r-rx33

Subject

• Inorganic chemistry
• Molecular chemistry

Language

• en

Alternate Identifier

• http://dissertations.umi.com/northwestern:14734
• etdadmin_upload_674052

Date created

• 2019-01-01

Resource type

• Dissertation

Rights statement

• In Copyright