Readout and Control of a Single Nuclear Spin with a Metastable Electron Spin Ancilla

Electron and nuclear spins associated with point defects in insulators are promising systems for solid-state quantum technology1, 2, 3. The electron spin is usually used for readout and addressing, and nuclear spins are used as exquisite quantum bits4, 5 and memory systems3, 6. With these systems, single-shot readout of single nuclear spins5, 7 as well as entanglement4, 8, 9, aided by the electron spin, have been shown. Although the electron spin in this example is essential for readout, it usually limits the nuclear spin coherence10, leading to a quest for defects with spin-free ground states9, 11. Here, we isolate a hitherto unidentified defect in diamond and use it at room temperature to demonstrate optical spin polarization and readout with exceptionally high contrast (up to 45%), coherent manipulation of an individual excited triplet state spin, and coherent nuclear spin manipulation using the triplet electron spin as a metastable ancilla. We demonstrate nuclear magnetic resonance and Rabi oscillations of the uncoupled nuclear spin in the spin-free electronic ground state. Our study demonstrates that nuclei coupled to single metastable electron spins are useful quantum systems with long memory times, in spite of electronic relaxation processes.