Nuclear magnetic resonance (NMR) and magnetic resonance imaging (MRI) are wellestablished techniques that provide valuable information in a diverse set of disciplines but are currently limited to macroscopic sample volumes. Here we demonstrate nanoscale NMR spectroscopy and imaging under ambient conditions of samples containing multiple nuclear species, using nitrogen-vacancy (NV) colour centres in diamond as sensors. With single, shallow NV centres in a diamond chip and samples placed on the diamond surface, we perform NMR spectroscopy and one-dimensional MRI on few-nanometre-sized samples containing 1 H and 19 F nuclei. Alternatively, we employ a high-density NV layer near the surface of a diamond chip to demonstrate wide-field optical NMR spectroscopy of nanoscale samples containing 1 H, 19 F, and 31 P nuclei, as well as multi-species two-dimensional optical MRI with sub-micron resolution. For all diamond samples exposed to air, we identify a ubiquitous 1 H NMR signal, consistent with a ∼ 1 nm layer of adsorbed hydrocarbons or water on the diamond surface and below any sample placed on the diamond. This work lays the foundation for nanoscale NMR and MRI applications such as studies of single proteins and functional biological imaging with subcellular resolution, as well as characterization of thin films with sub-nanometre resolution.

The spin chemical potential characterizes the tendency of spins to diffuse. Probing this quantity could provide insight into materials such as magnetic insulators and spin liquids and aid optimization of spintronic devices. Here we introduce single-spin magnetometry as a generic platform for nonperturbative, nanoscale characterization of spin chemical potentials. We experimentally realize this platform using diamond nitrogen-vacancy centers and use it to investigate magnons in a magnetic insulator, finding that the magnon chemical potential can be controlled by driving the system's ferromagnetic resonance. We introduce a symmetry-based two-fluid theory describing the underlying magnon processes, measure the local thermomagnonic torque, and illustrate the detection sensitivity using electrically controlled spin injection. Our results pave the way for nanoscale control and imaging of spin transport in mesoscopic systems.

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