Subnanometre resolution in three-dimensional magnetic resonance imaging of individual dark spins.

Magnetic resonance imaging (MRI) has revolutionized biomedical science by providing non-invasive, three-dimensional biological imaging. However, spatial resolution in conventional MRI systems is limited to tens of micrometres, which is insufficient for imaging on molecular scales. Here, we demonstrate an MRI technique that provides subnanometre spatial resolution in three dimensions, with single electron-spin sensitivity. Our imaging method works under ambient conditions and can measure ubiquitous 'dark' spins, which constitute nearly all spin targets of interest. In this technique, the magnetic quantum-projection noise of dark spins is measured using a single nitrogen-vacancy (NV) magnetometer located near the surface of a diamond chip. The distribution of spins surrounding the NV magnetometer is imaged with a scanning magnetic-field gradient. To evaluate the performance of the NV-MRI technique, we image the three-dimensional landscape of electronic spins at the diamond surface and achieve an unprecedented combination of resolution (0.8 nm laterally and 1.5 nm vertically) and single-spin sensitivity. Our measurements uncover electronic spins on the diamond surface that can potentially be used as resources for improved magnetic imaging. This NV-MRI technique is immediately applicable to diverse systems including imaging spin chains, readout of spin-based quantum bits, and determining the location of spin labels in biological systems.

A robust scanning diamond sensor for nanoscale imaging with single nitrogen-vacancy centres.

The nitrogen-vacancy defect centre in diamond has potential applications in nanoscale electric and magnetic-field sensing, single-photon microscopy, quantum information processing and bioimaging. These applications rely on the ability to position a single nitrogen-vacancy centre within a few nanometres of a sample, and then scan it across the sample surface, while preserving the centre's spin coherence and readout fidelity. However, existing scanning techniques, which use a single diamond nanocrystal grafted onto the tip of a scanning probe microscope, suffer from short spin coherence times due to poor crystal quality, and from inefficient far-field collection of the fluorescence from the nitrogen-vacancy centre. Here, we demonstrate a robust method for scanning a single nitrogen-vacancy centre within tens of nanometres from a sample surface that addresses both of these concerns. This is achieved by positioning a single nitrogen-vacancy centre at the end of a high-purity diamond nanopillar, which we use as the tip of an atomic force microscope. Our approach ensures long nitrogen-vacancy spin coherence times (∼75 µs), enhanced nitrogen-vacancy collection efficiencies due to waveguiding, and mechanical robustness of the device (several weeks of scanning time). We are able to image magnetic domains with widths of 25 nm, and demonstrate a magnetic field sensitivity of 56 nT Hz(-1/2) at a frequency of 33 kHz, which is unprecedented for scanning nitrogen-vacancy centres.