The detection of small numbers of magnetic spins is a significant challenge in the life, physical and chemical sciences, especially when room temperature operation is required. Here we show that a proximal nitrogen-vacancy spin ensemble serves as a high precision sensing and imaging array. Monitoring its longitudinal relaxation enables sensing of freely diffusing, unperturbed magnetic ions and molecules in a microfluidic device without applying external magnetic fields. Multiplexed charge-coupled device acquisition and an optimized detection scheme permits direct spin noise imaging of magnetically labelled cellular structures under ambient conditions. Within 20 s we achieve spatial resolutions below 500 nm and experimental sensitivities down to 1,000 statistically polarized spins, of which only 32 ions contribute to a net magnetization. The results mark a major step towards versatile subcellular magnetic imaging and real-time spin sensing under physiological conditions providing a minimally invasive tool to monitor ion channels or haemoglobin trafficking inside live cells.

We present a solid state magnetic field imaging technique using a two-dimensional array of spins in diamond. The magnetic sensing spin array is made of nitrogen vacancy (NV) centers created at shallow depths. Their optical response is used for measuring external magnetic fields in close proximity. Optically detected magnetic resonance is read out from a 60×60 μm2 field of view in a multiplexed manner using a charge coupled device camera. We experimentally demonstrate full two-dimensional vector imaging of the magnetic field produced by a pair of current carrying microwires. The presented wide-field NV magnetometer offers, in addition to its high magnetic sensitivity and vector reconstruction, an unprecedented spatiotemporal resolution and functionality at room temperature.

Doping of carbon nanoparticles with impurity atoms is central to their application. However, doping has proven elusive for very small carbon nanoparticles because of their limited availability and a lack of fundamental understanding of impurity stability in such nanostructures. Here, we show that isolated diamond nanoparticles as small as 1.6 nm, comprising only ∼400 carbon atoms, are capable of housing stable photoluminescent colour centres, namely the silicon vacancy (SiV). Surprisingly, fluorescence from SiVs is stable over time, and few or only single colour centres are found per nanocrystal. We also observe size-dependent SiV emission supported by quantum-chemical simulation of SiV energy levels in small nanodiamonds. Our work opens the way to investigating the physics and chemistry of molecular-sized cubic carbon clusters and promises the application of ultrasmall non-perturbative fluorescent nanoparticles as markers in microscopy and sensing.

Magnetic field fluctuations arising from fundamental spins are ubiquitous in nanoscale biology, and are a rich source of information about the processes that generate them. However, the ability to detect the few spins involved without averaging over large ensembles has remained elusive. Here, we demonstrate the detection of gadolinium spin labels in an artificial cell membrane under ambient conditions using a single-spin nanodiamond sensor. Changes in the spin relaxation time of the sensor located in the lipid bilayer were optically detected and found to be sensitive to nearindividual (4 ± 2) proximal gadolinium atomic labels. The detection of such small numbers of spins in a model biological setting, with projected detection times of 1 s [corresponding to a sensitivity of ∼5 Gd spins per Hz 1/2 ], opens a pathway for in situ nanoscale detection of dynamical processes in biology.nitrogen-vacancy center | biophysics | nanomagnetometry T he development of sensitive and highly localized probes has driven advances in our understanding of the basic processes of life at increasingly smaller scales (1). In the last decade there has been a strong drive to expand the range of probes that can be used for studying biological systems (2-6), with emphasis on the detection of atoms and molecules in nanometer-sized volumes to gain access to information that may be hidden in ensemble averaging. However, at present there are no nanoprobes suitable for directly sensing the weak magnetic fields arising from small numbers of fundamental spins in nanoscale biology, occurring naturally (e.g., free radicals) or introduced (e.g., spin labels). These can be a rich source of information about processes at the atomic and molecular level. Magnetic resonance techniques such as electron spin resonance (ESR) have played an important role in the development of our understanding of membranes, proteins, and free radicals (7); however, ESR sensitivity and resolution are fundamentally limited to mesoscopic ensembles of at least 10 7 spins with a sensitivity of ∼2 × 10 9 spins per Hz 1/2 (8). In a typical ESR application, small electron spin label moieties are attached to the system of interest and their environment is investigated through spin measurements on the labels. Because of the large ensemble required, nanoscopic detail at the few-spin level can be lost in the averaging process. Recently, magnetic resonance force microscopy techniques have demonstrated single-spin detection (9-11), but these require cryogenic temperatures and vacuum. Here, we demonstrate a nanoparticle probe--a nitrogen-vacancy spin in a nanodiamond--which is situated in the target structure itself and acts as a nanoscopic magnetic field detector under ambient conditions with noncontact optical readout. We use this probe to detect near-individual spin labels in an artificial cell membrane at a projected sensitivity of ∼5 Gd spins per Hz 1/2 , effectively bridging the gap between traditional ESR ensemble-based techniques and the ultimate goal of few-spin nanoscale detection...

Sensing and imaging paramagnetic species under physiological conditions is a key technology in chemical and biochemical analytics, cell biology, and medical sciences. At submicrometer length scales, nitrogen-vacancy (NV) centers in diamond offer atom-sized probes for magnetic fields. We show that spin relaxation of an ensemble NV sensor allows sensing of adsorbed and freely diffusing manganese(II) ions and adsorbed ferritin. Sensitivities approach 175 Mn ions and 10 ferritin proteins per diffraction limited spot under ambient conditions.