A single nitrogen-vacancy (NV) center is used to sense individual, as well as small ensembles of, electron spins placed outside the diamond lattice. Applying double electron–electron resonance techniques, we were able to observe Rabi nutations of these external spins as well as the coupling strength between the external spins and the NV sensor, via modulations and accelerated decay of the NV spin echo. Echo modulation frequencies as large as 600 kHz have been observed, being equivalent to a few nanometers distance between the NV and an unpaired electron spin. Upon surface modification, the coupling disappears, suggesting the spins to be localized at surface defects. The present study is important for understanding the properties of diamond surface spins so that their effects on NV sensors can eventually be mitigated. This would enable potential applications such as the imaging and tracking of single atoms and molecules in living cells or the use of NVs on scanning probe tips to entangle remote spins for scalable room temperature quantum computers.
