Readout and control of an endofullerene electronic spin

Atomic spins for quantum technologies need to be individually addressed and positioned with nanoscale precision. C(60) fullerene cages offer a robust packaging for atomic spins, while allowing in-situ physical positioning at the nanoscale. However, achieving single-spin level readout and control of endofullerenes has so far remained elusive. In this work, we demonstrate electron paramagnetic resonance on an encapsulated nitrogen spin ((14)N@C(60)) within a C(60) matrix using a single near-surface nitrogen vacancy (NV) center in diamond at 4.7 K. Exploiting the strong magnetic dipolar interaction between the NV and endofullerene electronic spins, we demonstrate radio-frequency pulse controlled Rabi oscillations and measure spin-echos on an encapsulated spin. Modeling the results using second-order perturbation theory reveals an enhanced hyperfine interaction and zero-field splitting, possibly caused by surface adsorption on diamond. These results demonstrate the first step towards controlling single endofullerenes, and possibly building large-scale endofullerene quantum machines, which can be scaled using standard positioning or self-assembly methods.