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Nitrogen-vacancy (NV) centers in diamond have emerged as valuable tools forsensing and polarizing spins. Motivated by potential applications in chemistry,biology, and medicine, we show that NV-based sensors are capable of detectingsingle spin targets even if they undergo diffusive motion in an ambient thermalenvironment. Focusing on experimentally relevant diffusion regimes, we derivean effective model for the NV-target interaction, where parameters entering themodel are obtained from numerical simulations of the target motion. Thepracticality of our approach is demonstrated by analyzing two realisticexperimental scenarios: (i) time-resolved sensing of a fluorine nuclear spinbound to an N-heterocyclic carbene-ruthenium (NHC-Ru) catalyst that isimmobilized on the diamond surface and (ii) detection of an electron spin labelby an NV center in a nanodiamond, both attached to a vibrating chemokinereceptor in thermal motion. We find in particular that the detachment of afluorine target from the NHC-Ru carrier molecule can be monitored with a timeresolution of a few seconds.

Sensing of single nuclear spins in random thermal motion with proximate nitrogen-vacancy centers