Cavity-enhanced optical readout and control of nuclear spin qubits.

Their exceptional coherence makes nuclear spins in solids a prime candidate for quantum memories in quantum networks and repeaters. Still, the direct all-optical initialization, coherent control, and readout of individual nuclear spin qubits have been an outstanding challenge. Here, this is achieved by embedding 167Er dopants in yttrium orthosilicate in a cryogenic Fabry-Perot cavity, whose linewidth of 65 MHz is much smaller than the 0.9 GHz separation of neighboring hyperfine levels. Frequency-selective emission enhancement thus enables a single-shot readout fidelity of 91(2) %. Furthermore, a large magnetic field freezes paramagnetic impurities, leading to coherence times exceeding 0.2 s. The combination of nuclear-spin qubits with frequency-multiplexed addressing and lifetime-limited photon emission in the minimal-loss telecommunications C-band establishes 167Er as a leading platform for long-range, fiber-based quantum networks.