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Quantum diamond spectrometer for nanoscale NMR and ESR spectroscopy

Nature Protocols volume 14, pages 2707–2747 (2019)Cite this article

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Abstract

Nitrogen-vacancy (NV) quantum defects in diamond are sensitive detectors of magnetic fields. Owing to their atomic size and optical readout capability, they have been used for magnetic resonance spectroscopy of nanoscale samples on diamond surfaces. Here, we present a protocol for fabricating NV diamond chips and for constructing and operating a simple, low-cost ‘quantum diamond spectrometer’ for performing NMR and electron spin resonance (ESR) spectroscopy in nanoscale volumes. The instrument is based on a commercially available diamond chip, into which an NV ensemble is ion-implanted at a depth of ~10 nm below the diamond surface. The spectrometer operates at low magnetic fields (~300 G) and requires standard optical and microwave (MW) components for NV spin preparation, manipulation, and readout. We demonstrate the utility of this device for nanoscale proton and fluorine NMR spectroscopy, as well as for the detection of transition metals via relaxometry. We estimate that the full protocol requires 2–3 months to implement, depending on the availability of equipment, diamond substrates, and user experience.

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Fig. 1: NV center overview.
Fig. 2: Nuclear and electronic spin-sensing schemes with NV centers.
Fig. 3: Overview of the procedure.
Fig. 4: Schematic of optical components.
Fig. 5: Schematic of electronic components.
Fig. 6: Overview of the described pulse sequences.
Fig. 7
Fig. 8
Fig. 9
Fig. 10: Magnet mount with x, z rotation for B0 field alignment.
Fig. 11: Avalanche photodiode (APD) holder.
Fig. 12: Photo of the quantum diamond spectrometer.
Fig. 13: Microwave delivery loop.
Fig. 14: Magnetic field alignment.
Fig. 15: Setting timing between the readout pulses.
Fig. 16: Rabi contrast.
Fig. 17: Detection of an external AC signal from an RF loop at 1.25 MHz with an XY8-12 dynamic decoupling sequence.
Fig. 18: Nuclear spin sensing with a dynamic decoupling sequence at 311 G.
Fig. 19: Correlation spectroscopy for NV-NMR sensing at 311 G.
Fig. 20: Electronic spin detection with NV-T1 relaxometry.
Fig. 21: Fourier transform of the NV-NMR correlation signal at 311 G.

Data availability

The primary data of this study are available from the corresponding authors upon reasonable request.

Code availability

The qdSpectro package is available to download from https://gitlab.com/dplaudecraik/qdSpectro and is licensed under the MIT License. The most recent version at the time of writing is v.1.0.1, but the user is encouraged to download the latest version and refer to the readme file for any patches and updates. The package is registered at https://doi.org/10.5281/zenodo.1478113, which points to the latest version.

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Acknowledgements

This article is based on work supported by, or supported in part by, the US Army Research Laboratory and the US Army Research Office under contract/grant no. W911NF1510548. D.B.B. was partially supported by the German Research Foundation (BU 3257/1-1). D.P.L.A.C. was partially supported by the NSF STC ‘Center for Integrated Quantum Materials’ under cooperative agreement no. DMR-1231319.

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Authors and Affiliations

  1. Harvard-Smithsonian Center for Astrophysics, Cambridge, MA, USA

    Dominik B. Bucher, Mikael P. Backlund, Oren Ben Dor & Ronald L. Walsworth

  2. Department of Physics, Harvard University, Cambridge, MA, USA

    Dominik B. Bucher, Diana P. L. Aude Craik, Mikael P. Backlund, Matthew J. Turner, Oren Ben Dor, David R. Glenn & Ronald L. Walsworth

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  1. Dominik B. Bucher
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Contributions

D.B.B. led the development of the protocol, buildup of the quantum diamond spectrometer, and acquisition and analysis of data, informed by extensive past work in the Walsworth group and aided closely by D.P.L.A.C. and M.P.B. D.P.L.A.C. wrote the qdSpectro software package. M.J.T. prepared the NV-diamond chip and provided technical assistance in buildup of the quantum diamond spectrometer. O.B.D. performed a pilot run of the protocol and provided feedback to improve procedures. D.R.G. provided technical guidance to all aspects of the effort. R.L.W. supervised the project. All authors discussed the results and participated in writing the manuscript.

Corresponding authors

Correspondence to Dominik B. Bucher or Ronald L. Walsworth.

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Key references using this protocol

DeVience, S. J. et al. Nat. Nanotechnol. 10, 129–134 (2015): https://www.nature.com/articles/nnano.2014.313

Kehayias, P. et al. Nat. Commun. 8, 188 (2017): https://www.nature.com/articles/s41467-017-00266-4

Steinert, S. et al. Nat. Commun. 4, 1607 (2013): https://www.nature.com/articles/ncomms2588

Staudacher, T. et al. Science 339, 561–563 (2013): https://science.sciencemag.org/content/339/6119/561

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Bucher, D.B., Aude Craik, D.P.L., Backlund, M.P. et al. Quantum diamond spectrometer for nanoscale NMR and ESR spectroscopy. Nat Protoc 14, 2707–2747 (2019). https://doi.org/10.1038/s41596-019-0201-3

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