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Defect center-based spin qubits in solid-state materials show great promise as quantum sensors and nodes in quantum networks. The success of these applications relies on precise control and understanding of the qubit host material and noise environment, which ultimately dictate qubit coherence. The nitrogen vacancy (NV) center in diamond is a particular defect qubit with a robust spin-photon interface and long spin relaxation times, enabling a range of advances in quantum information science. However, open questions remain regarding the surrounding host material. In particular, while it is possible to routinely grow single crystal diamond with nitrogen doping, to synthesize NV centers, a reliable method for characterizing this doping under growth parameters relevant for many NV applications is lacking. Furthermore, unconverted nitrogen spins (P1 centers) constitute a major source of decoherence in the diamond lattice. While P1 center spin properties have been studied in bulk, there are few experiments that probe single P1 centers. Characterizing single P1 spins will advance understanding of P1-induced decoherence as well as aid in the implementation of P1 centers as auxiliary qubits in applications of the NV center. In this thesis, I will describe our recent studies of interactions between the NV center and nearby P1 electron spins. After an introduction into quantum science and engineering in Ch. 1, I describe the two defect centers in Ch. 2. I then lay the groundwork for the studies in this thesis from two very different perspectives: In Ch. 3 I review a theoretical treatment of noise and spin baths; in Ch. 4 I discuss the details of plasma …