Hyperfine Spectroscopy and Fast, All-Optical Arbitrary State Initialization and Readout of a Single, Ten-Level

A high-spin nucleus coupled to a color center can act as a long-lived memory qudit in a spin-photon interface. The germanium vacancy (GeV) in diamond has attracted recent attention due to its excellent spectral properties and provides access to the ten-dimensional Hilbert space of the I=9/2 ^{73}Ge nucleus. Here, we observe the ^{73}GeV hyperfine structure, perform nuclear spin readout, and optically initialize the ^{73}Ge spin into any eigenstate on a µs timescale and with a fidelity of up to ∼84%. Our results establish ^{73}GeV as an optically addressable high-spin quantum platform for a high-efficiency spin-photon interface as well as for foundational quantum physics and metrology.