Electron and nuclear spins associated with point defects in insulators are promising systems for solid state quantum technology. While the electron spin usually is used for readout and addressing, nuclear spins are exquisite quantum bits and memory systems. With these systems single-shot readout of nearby nuclear spins as well as entanglement aided by the electron spin has been shown. While the electron spin in this example is essential for readout it usually limits nuclear spin coherence. This has set of the quest for defects with spin-free ground states. 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 meta-stable ancilla. By this 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 despite electronic relaxation processes.
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