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Nuclear spin polarization and control in hexagonal boron nitride

Abstract

Electron spins in van der Waals materials are playing a crucial role in recent advances in condensed-matter physics and spintronics. However, nuclear spins in van der Waals materials remain an unexplored quantum resource. Here we report optical polarization and coherent control of nuclear spins in a van der Waals material at room temperature. We use negatively charged boron vacancy (\({V}_{\mathrm{B}}^{-}\)) spin defects in hexagonal boron nitride to polarize nearby nitrogen nuclear spins. We observe the Rabi frequency of nuclear spins at the excited-state level anti-crossing of \({V}_{\mathrm{B}}^{-}\) defects to be 350 times larger than that of an isolated nucleus, and demonstrate fast coherent control of nuclear spins. Further, we detect strong electron-mediated nuclear–nuclear spin coupling that is five orders of magnitude larger than the direct nuclear-spin dipolar coupling, enabling multi-qubit operations. Our work opens new avenues for the manipulation of nuclear spins in van der Waals materials for quantum information science and technology.

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Fig. 1: Optical polarization of nuclear spins in hBN with \({V}_{\mathrm{B}}^{-}\) spin defects.
Fig. 2: Polarization of the three nearest nitrogen nuclear spins.
Fig. 3: ODNMR spectroscopy of the three nearest nitrogen nuclear spins.
Fig. 4: Coherent control of nuclear spins in hBN.

Data availability

Source data are provided with this paper. All other data that support the plots within this paper and other findings of this study are available from the corresponding author upon reasonable request.

Code availability

The custom codes that support the findings of this study are available from the corresponding author upon reasonable request.

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Acknowledgements

T.L. thanks the Purdue Quantum Science and Engineering Institute (PQSEI) for support through the seed grant, the DARPA NLM program, the DARPA QUEST program and the National Science Foundation under grant no. PHY-2110591. Y.P. is supported by the National Science Foundation under grant no. DMR-1760260. A.E.L.A and Y.P.C. acknowledge support by the Quantum Science Center, a US Department of Energy, Office of Science, National Quantum Information Science Research Center. Y.P.C. also thanks the hospitality of NIMS and support of Tohoku AIMR and FriDUO program. B.J. and S.A.B. are supported by the Office of Naval Research (ONR) grant award no. N00014-20-1-2806. K.W. and T.T. acknowledge support from JSPS KAKENHI (grant nos. 19H05790, 20H00354 and 21H05233). The ab initio calculations used resources of the lux supercomputer at the University of California, Santa Cruz, funded by the National Science Foundation MRI grant no. AST 1828315; the Center for Functional Nanomaterials, which is a US Department of Energy, Office of Science, facility; and the Scientific Data and Computing center, a component of the Computational Science Initiative, at Brookhaven National Laboratory under contract no. DE-SC0012704.

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Contributions

T.L. and X.G. conceived and designed the project. X.G., Z.X., S.V., P.J. and K.S. built the setup. K.L., X.G. and S.V. performed the calculations. B.J. fabricated the MW waveguides. T.T. and K.W. grew the hBN crystals. X.G., S.V. and A.E.L.A. created the hBN nanosheets with spin defects. X.G. performed the measurements. X.G., T.L., S.V., K.L. and Y.P. analysed the results. T.L., Y.P., Y.P.C. and S.A.B supervised the project. All the authors contributed to the writing of the manuscript.

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Correspondence to Tongcang Li.

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Nature Materials thanks Weibo Gao, Fedor Jelezko and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Gao, X., Vaidya, S., Li, K. et al. Nuclear spin polarization and control in hexagonal boron nitride. Nat. Mater. 21, 1024–1028 (2022). https://doi.org/10.1038/s41563-022-01329-8

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