Zero-field identification and control of hydrogen-related electron-nuclear spin registers in diamond

Spin defects in diamond serve as powerful building blocks for quantum technologies, especially for applications in quantum sensing and quantum networks. Electron-nuclear defects formed in the environment of optically active spins, such as the nitrogen-vacancy (NV) center, can be harnessed as qubits to construct larger hybrid quantum registers. However, many of these defects have yet to be characterized, limiting their integration into scalable devices. Here, we introduce an approach to identify the hyperfine components and nuclear spin species of spin defects through measurements on a nearby NV center. This approach combines double electron-electron resonance performed at zero field (ZF-DEER) with nuclear-electron-electron triple resonance (NEETR), which we use to characterize two unknown defects at the single-spin level, yielding self-consistent results. These results provide a guide to resolving the defect structures using ab initio calculations, leading to the identification of a new hydrogen defect structure and an accurate match to a previously identified nitrogen defect. Building on the NEETR protocol, we then demonstrate initialization, unitary control, and long-lived coherence of the nuclear spin qubit of the hydrogen defect with T₂ = 1.0(3) ms. Our characterization and control tools establish a framework to expand the accessible defect landscape for hybrid electron-nuclear registers and enable applications in quantum sensing, networks, and atomic-scale magnetic resonance imaging at room temperature.