Understanding and Controlling Spin-Systems Using Electron Spin Resonance Techniques

Single molecule magnets (SMMs) posses multi-level energy structures with properties that make them attractive candidates for implementation into quantum information technologies. However there are some major hurdles that need to be overcome if these systems are to be used as the fundamental components of an eventual quantum computer. One such hurdle is the relatively short coherence times these systems display which severely limits the amount of time quantum information can remain encoded within them. In this dissertation, recent experiments conducted with the intent of bringing this technology closer to realization are presented. The detailed knowledge of the spin Hamiltonian and mechanisms of decoherence in SMMs are absolutely essential if these systems are to be used in technologies. To that effect, experiments were done on a particularly promising SMM, the complex K₆[V[superscript IV over subscript 15As[superscript III over subscript 6]O₄₂(H₂O)] ⋅ 8H₂O, known as V₁₅. High-field electron spin resonance (ESR) measurements were performed on this system at the National High Magnetic Field Laboratory. The resulting spectra allowed for detailed analysis of the V₁₅ spin Hamiltonian which will be presented as well as the most precise values yet reported for the g-factors of this system. Additionally, the line widths of the ESR spectra are studied in depth and found to reveal that fluctuations within the spin-orbit interaction are a mechanism for decoherence in V₁₅. A new model for decoherence is presented that describes very well both the temperature and field orientation dependences of the measured ESR line widths. Also essential is the ability to control spin-states of SMMs. Presented in this dissertation as well is the demonstration of the coherent manipulation of the multi-state spin system Mn[subperscript 2+] diluted in MgO by means of a two-tone pulse drive. Through the detuning between the excitation and readout radio frequency pulses it is possible to select the number of photons involved in a Rabi oscillation as well as increase the frequency of this nutation. Experimental findings fit well the analytical model developed. This process could lead to the use of multi-level spin systems as tunable solid state qubits. Finally, if quantum computing technologies are to be commercially realized, an on-chip method to address qubits must be developed. One way to incorporate SMMs to an on-chip device is by way of a coplanar waveguide (CPW) resonator. Efforts to create a resonator of this type to be used to perform low-temperature ESR on-chip will be described. Our work is focused on implementing such on-chip techniques in high magnetic fields, which is desirable for ESR-type of experiments in (quasi-)isotropic spin systems. Considerable attention is given to the coupling of these devices and a geometry is presented for a superconducting CPW resonator that is critically coupled. The effect of the magnetic field on the resonance position and its quality factor is addressed as well. Our devices show robust performance in field upwards of 1 Tesla and their use in performing on-chip ESR measurements seem promising.