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Magnetic resonance detection is one of the most important tools used inlife-sciences today. However, as the technique detects the magnetization oflarge ensembles of spins it is fundamentally limited in spatial resolution tomesoscopic scales. Here we detect the natural fluctuations of nanoscale spinensembles at ambient temperatures by measuring the decoherence rate of a singlequantum spin in response to introduced extrinsic target spins. In ourexperiments 45 nm nanodiamonds with single nitrogen-vacancy (NV) spins wereimmersed in solution containing spin 5/2 Mn^2+ ions and the NV decoherence ratemeasured though optically detected magnetic resonance. The presence of bothfreely moving and accreted Mn spins in solution were detected via significantchanges in measured NV decoherence rates. Analysis of the data using a quantumcluster expansion treatment of the NV-target system found the measurements tobe consistent with the detection of ~2,500 motionally diffusing Mn spins overan effective volume of (16 nm)^3 in 4.2 s, representing a reduction in targetensemble size and acquisition time of several orders of magnitude overstate-of-the-art electron spin resonance detection. These measurements providethe basis for the detection of nanoscale magnetic field fluctuations withunprecedented sensitivity and resolution in ambient conditions.

Ambient Nanoscale Sensing with Single Spins Using Quantum Decoherence