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Solid-state nuclear spins surrounding individual, optically addressablequbits provide a crucial resource for quantum networks, computation andsimulation. While hosts with sparse nuclear spin baths are typically chosen tomitigate qubit decoherence, developing coherent quantum systems in nuclearspin-rich hosts enables exploration of a much broader range of materials forquantum information applications. The collective modes of these dense nuclearspin ensembles provide a natural basis for quantum storage, however, utilizingthem as a resource for single spin qubits has thus far remained elusive. Here,by using a highly coherent, optically addressed 171Yb3+ qubit doped into anuclear spin-rich yttrium orthovanadate crystal, we develop a robust quantumcontrol protocol to manipulate the multi-level nuclear spin states ofneighbouring 51V5+ lattice ions. Via a dynamically-engineered spin exchangeinteraction, we polarise this nuclear spin ensemble, generate collective spinexcitations, and subsequently use them to implement a long-lived quantummemory. We additionally demonstrate preparation and measurement of maximallyentangled 171Yb--51V Bell states. Unlike conventional, disordered nuclear spinbased quantum memories, our platform is deterministic and reproducible,ensuring identical quantum registers for all 171Yb qubits. Our approachprovides a framework for utilising the complex structure of dense nuclear spinbaths, paving the way for building large-scale quantum networks using singlerare-earth ion qubits.

Nuclear spin-wave quantum register for a solid state qubit