Application of nuclear magnetic resonance (NMR) spectroscopy to nanoscale samples has remained an elusive goal, achieved only with great experimental effort at subkelvin temperatures. We demonstrated detection of NMR signals from a (5-nanometer)(3) voxel of various fluid and solid organic samples under ambient conditions. We used an atomic-size magnetic field sensor, a single nitrogen-vacancy defect center, embedded ~7 nanometers under the surface of a bulk diamond to record NMR spectra of various samples placed on the diamond surface. Its detection volume consisted of only 10(4) nuclear spins with a net magnetization of only 10(2) statistically polarized spins.

We demonstrate a protocol using individual nitrogen-vacancy centres in diamond to observe the time evolution of proton spins from organic molecules located a few nanometres from the diamond surface. The protocol records temporal correlations among the interacting protons, and thus is sensitive to the local dynamics via its impact on the nuclear spin relaxation and interaction with the nitrogen vacancy. We gather information on the nanoscale rotational and translational diffusion dynamics by analysing the time dependence of the nuclear magnetic resonance signal. Applying this technique to liquid and solid samples, we find evidence that liquid samples form a semi-solid layer of 1.5-nm thickness on the surface of diamond, where translational diffusion is suppressed while rotational diffusion remains present. Extensions of the present technique could be exploited to highlight the chemical composition of molecules tethered to the diamond surface or to investigate thermally or chemically activated dynamical processes such as molecular folding.

The controlled scaling of diamond defect center based quantum registers relies on the ability to position NVs with high spatial resolution. Using ion implantation, shallow (< 10 nm) NVs can be placed with accuracy below 20nm, but generally show reduced spin properties compared to bulk NVs. We demonstrate the augmentation of spin properties for shallow implanted NV centers using an overgrowth technique. An increase of the coherence times up to an order of magnitude (T 2 = 250s) was achieved. Dynamic decoupling of defects spins achieves ms decoherence times. The study marks a further step towards achieving strong coupling among defects positioned with nm precision.One of the key challenges in experimental quantum information science is the identification of isolated quantum mechanical systems which exhibit long coherence times and can be manipulated and coupled in a scalable fashion. Single defects in diamond and especially the negatively charged nitrogen vacancy (NV) center are a perfect platform for studying the quantum dynamics of spin systems. The NV consists of a substitutional nitrogen atom with an adjacent vacancy and an extra electron attached to its complex. It has a long-lived spin triplet in its electronic ground state with coherence times ranging up to 3 ms under ambient conditions [1]. The NV spin can be prepared and detected by optical means, and microwave excitation can be used to control its spin state [2,3,4]. Quantum registers based on the coupling of one NV center to an electron spin of another proximal NV center [5,6] as well as with nuclear spins of neighboring 13 C atoms [7,8,9,10,11] have already been demonstrated experimentally.Of special interest in the context of large scale spin arrays is the generation of multiple strongly coupled NV centers, since this allows the performance of advanced quantum protocols. Since the