Guiding Diamond Spin Qubit Growth with Computational Methods*

The nitrogen vacancy (NV) center in diamond, a well-studied, optically active spin defect, is the prototypical system in many state-of-the-art quantum sensing and communication applications. In addition to the enticing properties intrinsic to the NV center, its diamond host's nuclear and electronic spin baths can be leveraged as resources for quantum information, rather than considered solely as sources of decoherence. However, current synthesis approaches result in stochastic defect spin positions, reducing the potential for deterministic control and yield of NV-spin bath systems, as well as scalability and integration with other technologies. Here, we demonstrate the use of theoretical calculations of electronic central spin decoherence as an integral part of an NV-spin bath synthesis workflow, providing a path forward for the quantitative design of spin qubit systems. We use computationally generated coherence data to characterize the properties of single NV center qubits across relevant growth parameters, develop an in-situ growth characterization tool, and explore the impact of dimensionality on strongly coupled spin systems. These methods are general and applicable to other qubit platforms.