Cavity-Enhanced Spectroscopy of Individual Nuclear Spins in a Dense Bath

Echo-based spectroscopy of the superhyperfine interaction of an electronic spin with nuclear spins in its surroundings enables detailed insights into the microscopic magnetic environment of spins in solids. Still, it is an outstanding challenge to resolve individual nuclear spins in a dense bath, in which many of them exhibit a comparable coupling strength. This simultaneously requires a high spectral resolution and a large signal-to-noise ratio. However, when probing spin ensembles, dipolar interactions between the dopants can lead to a concentration-dependent trade-off between resolution and signal. Here, we fully eliminate this limitation of previous optical-echo-envelope-modulation spectroscopy experiments by integrating the emitters into a high-finesse resonator, which allows for strong optical echoes even at very low concentrations. To demonstrate its potential, the technique is applied to erbium dopants in yttrium orthosilicate (Er:YSO). Achieving an unprecedented spectral resolution enables precise measurements of the superhyperfine interaction with four of the Y nuclear spins densely surrounding each emitter. The achieved boost of the signal, enabled by the resonator, allows for extending the approach to the lowest concentration possible - to the level of single dopants, thereby providing a tool for detecting and studying individual nuclear spins. Thus, our technique paves the way for an improved understanding of dense nuclear-spin baths in solids.