Developing and applying quantum sensors based on optically addressable spin defects

Quantum sensing aims to further our understanding of the natural world and support an upcoming technological revolution by exploiting quantum properties or systems to exceed the performance of classical sensing. Owing to their convenient modes of operation and strong room temperature quantum properties, optically active spin defects hosted within solid state materials have come to prominence as one of the foremost tools of choice in this landscape. Many applications now aim to leverage dense ensembles of such defects to boost measurement sensitivity or scale up, which places greater emphasis on the quality of the host material and sensor production methods since cherry-picking individual defects is no longer an option. The prototypical example of such a defect is the nitrogen-vacancy (NV) centre in diamond, which exhibits remarkable room temperature spin coherence, bestowed upon it by diamond's material properties. In this thesis, we first look at optimising the production of NV ensembles for quantum sensing, aiming to efficiently and cost-effectively produce sensors capable of performing high sensitivity measurements in two key regimes that will be central to the experimental applications explored later. The topics examined are hyperpolarisation of a nuclear spin ensemble on the diamond surface through coupling to an ultra-near-surface NV layer, and investigating the properties of a van der Waals antiferromagnet through widefield NV microscopy. The demands placed on the NV layer for these applications are diverse from one another, with charge stability and quantum coherence properties being vital for the former, and the ability to scalably and reproducibly create layers of known thickness crucial to the latter. In light of these studies, we finally consider whether a different spin system housed within an entirely separate materials system, the boron-vacancy defect in hexagonal boron nitride, may be a suitable alternative to the well-established NV diamond system.