  Understanding the dynamics of molecules adsorbed to surfaces or confined to
small volumes is a matter of increasing scientific and technological
importance. Here, we demonstrate a pulse protocol using individual paramagnetic
nitrogen vacancy (NV) centers in diamond to observe the time evolution of 1H
spins from organic molecules located a few nanometers from the diamond surface.
The protocol records temporal correlations among the interacting 1H spins, and
thus is sensitive to the local system dynamics via its impact on the nuclear
spin relaxation and interaction with the NV. We are able to gather information
on the nanoscale rotational and translational diffusion dynamics by carefully
analyzing the time dependence of the NMR signal. Applying this technique to
various 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 adapted 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.
