Coherent Control of Hyperfine-coupled Electron and Nuclear Spins for Quantum Information Processing

Coupled electron-nuclear spins are promising physical systems for quantum in-formation processing: By combining the long coherence times of the nuclear spins with the ability to initialize, control, and measure the electron spin state, the favor-able properties of each spin species are utilized. This thesis discusses a procedure to initialize these nuclear spin qubits, and presents a vision of how these systems could be used as the fundamental processing unit of a quantum computer. The fo-cus of this thesis is on control of a system in which a single electron spin is coupled to N nuclear spins via resolvable anisotropic hyperfine (AHF) interactions. High-fidelity universal control of this le-Nn system is possible using only excitations on a single electron spin transition. This electron spin actuator control is implemented by using optimal control theory to find the modulation sequences that generate the desired unitary operations. Decoherence and the challenge of making useful qubits from these systems are also discussed. Experimental evidence of control using an electron spin actuator was acquired with a custom-built pulsed electron spin resonance spectrometer. Complex mod