Abstract
Magnetic resonance imaging (MRI) has revolutionized biomedical science by providing non-invasive, three-dimensional biological imaging1. However, spatial resolution in conventional MRI systems is limited to tens of micrometres2, 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.
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Acknowledgements
The authors thank S. Kolkowitz, N. de Leon and C. Belthangady for technical discussions regarding optimizing NV-based sensors and M. Markham and Element Six for providing diamond samples. The authors acknowledge discussions on the detection of dark spins using DEER with M. D. Lukin, A. Sushkov, I. Lovchinsky, N. Chisholm, S. Bennett, and N. Yao. M.S.G. is supported through fellowships from the Department of Defense (NDSEG programme) and the National Science Foundation. M.W. is supported through a Marie Curie Fellowship and K.D.G. acknowledges support from the Harvard Quantum Optics Center as an HQOC postdoctoral fellow. This work was supported by the DARPA QuEST and QuASAR programmes and the MURI QuISM.
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M.S.G., M.W. and A.Y. conceived the basic principles of NV-MRI. M.S.G., S.H., P.M. and A.Y. built the combined atomic force and confocal microscope for NV experiments. M.S.G. and A.Y. performed the experiments and analysed the data with input from all authors. All authors contributed to writing the manuscript.
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Grinolds, M., Warner, M., De Greve, K. et al. Subnanometre resolution in three-dimensional magnetic resonance imaging of individual dark spins. Nature Nanotech 9, 279–284 (2014). https://doi.org/10.1038/nnano.2014.30
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DOI: https://doi.org/10.1038/nnano.2014.30
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