Single nuclear spin detection and control in a van der Waals material

Xingyu Gao; Sumukh Vaidya; Kejun Li; Zhun Ge; Saakshi Dikshit; Shimin Zhang; Peng Ju; Kunhong Shen; Yuanbin Jin; Yuan Ping; Tongcang Li

doi:10.1038/s41586-025-09258-7

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Single nuclear spin detection and control in a van der Waals material

Xingyu Gao et al.

2025Nature 643, 943-949CC BY 4.0LCP000077

Nature 643, 943-949 (2025) · DOI: 10.1038/s41586-025-09258-7

License: CC BY 4.0.

Abstract

Optically active spin defects in solids are leading candidates for quantum sensing and quantum networking. Recently, single spin defects were discovered in hexagonal boron nitride (hBN), a layered van der Waals (vdW) material. Owing to its two-dimensional structure, hBN allows spin defects to be positioned closer to target samples than in three-dimensional crystals, making it ideal for atomic-scale quantum sensing, including nuclear magnetic resonance (NMR) of single molecules. However, the chemical structures of these defects remain unknown and detecting a single nuclear spin with a hBN spin defect has been elusive. Here we report the creation of single spin defects in hBN using ¹³C ion implantation and the identification of three distinct defect types based on hyperfine interactions. We observed both S = 1/2 and S = 1 spin states within a single hBN spin defect. We demonstrated atomic-scale NMR and coherent control of individual nuclear spins in a vdW material, with a π-gate fidelity up to 99.75% at room temperature. By comparing experimental results with density functional theory (DFT) calculations, we propose chemical structures for these spin defects. Our work advances the understanding of single spin defects in hBN and provides a pathway to enhance quantum sensing using hBN spin defects with nuclear spins as quantum memories.

Figures

24 panels with data across 5 figures. Each panel page shows the plot, its columns and its files; each data.csv begins with a header naming the paper, the panel, the source, the license and the provenance route.

Fig. 1

panel (d): Optical (PL) spectrum of defect 1, group I: PL intensity (a.u.) against wavelength (nm). The $g^{(2)}(\tau)$ inset is panel d-inset. data.csv
panel (d-inset): Inset of panel (d): second-order photon correlation $g^{(2)}(\tau)$ against delay $\tau$ (ns), measured points (black) with the fit (red); grey dashed lines mark $g^{(2)} = 1$ and $0.5$. data.csv
panel (e): Optical (PL) spectrum of defect 2, group II: PL intensity (a.u.) against wavelength (nm). The $g^{(2)}(\tau)$ inset is panel e-inset. data.csv
panel (e-inset): Inset of panel (e): second-order photon correlation $g^{(2)}(\tau)$ against delay $\tau$ (ns), measured points (black) with the fit (red); grey dashed lines mark $g^{(2)} = 1$ and $0.5$. data.csv
panel (f): Optical (PL) spectrum of defect 3, group III: PL intensity (a.u.) against wavelength (nm). The $g^{(2)}(\tau)$ inset is panel f-inset. data.csv
panel (f-inset): Inset of panel (f): second-order photon correlation $g^{(2)}(\tau)$ against delay $\tau$ (ns), measured points (black) with the fit (red); grey dashed lines mark $g^{(2)} = 1$ and $0.5$. data.csv
panel (g): ODMR spectrum of defect 1 (group I) at 62.5 mT: contrast (%) against microwave frequency (GHz), measured points (orange) with the fit (red). The grey shading of the central branch and the resonance labels of the print are not drawn. data.csv
panel (h): ODMR spectrum of defect 2 (group II) at 62.5 mT: contrast (%) against microwave frequency (GHz), measured points (orange) with the fit (red). The grey shading of the central branch and the resonance labels of the print are not drawn. data.csv
panel (i): ODMR spectrum of defect 3 (group III) at 62.5 mT: contrast (%) against microwave frequency (GHz), measured points (orange) with the fit (red). The grey shading of the central branch and the resonance labels of the print are not drawn. data.csv
panel (k): Magnetic-field-dependent ODMR spectra of defect 2 (group II): ODMR signal (a.u.) as a colour map against out-of-plane field $B$ (mT) and microwave frequency (GHz). The print has no colour bar; the resonance labels are not drawn. data.csv
panel (l): Magnetic-field-dependent ODMR spectra of defect 3 (group III): ODMR signal (a.u.) as a colour map against out-of-plane field $B$ (mT) and microwave frequency (GHz). The print has no colour bar; the resonance labels are not drawn. data.csv

Fig. 2

panel (h): ODNMR spectrum of defect 2 (group II) with the microwave driving II-2: contrast (%) against RF frequency (MHz), measured points (light blue) with the fit (dark blue). The zoom inset is panel h-inset. data.csv
panel (h-inset): Inset of panel (h): the same ODNMR spectrum on 62 to 70 MHz, contrast (%) against RF frequency (MHz), measured points (light blue) with the fit (dark blue). data.csv
panel (i): ODNMR spectrum of defect 3 (group III) with the microwave driving III-4: contrast (%) against RF frequency (MHz), measured points (light blue) with the fit (dark blue). The zoom inset is panel i-inset. data.csv
panel (i-inset): Inset of panel (i): ODNMR spectrum of defect 3 on 140 to 160 MHz, contrast (%) against RF frequency (MHz), measured points (light blue) with the fit (dark blue). data.csv

Fig. 3

panel (b-1): Top plot of panel (b): ODMR contrast (%) against frequency (GHz) after nuclear spin initialization for polarization $P = 0.43$, over resonances III-2, III-3 and III-4; measured points (blue) with the fit (red). data.csv
panel (b-2): Bottom plot of panel (b): ODMR contrast (%) against frequency (GHz) after nuclear spin initialization for polarization $P = -0.33$, over resonances III-2, III-3 and III-4; measured points (blue) with the fit (red). data.csv
panel (d): Nuclear spin Rabi oscillation: normalized contrast against RF pulse duration $\tau$ ($\mu$s), measured points joined by a line (blue) with the fit (red). data.csv
panel (e): Nuclear spin Rabi frequency $f_{\mathrm{Rabi},n}$ (MHz) against the square root of the RF power $\sqrt{P}$ (W$^{1/2}$): measured points (blue) with a linear fit (red). data.csv
panel (f): Nuclear spin Rabi oscillations at RF powers of 30, 80 and 320 mW: normalized contrast against pulse duration $\tau$ ($\mu$s), measured points with fits in the same colour. As printed, the 80 mW and 30 mW traces are offset upward by 1.5 and 3. data.csv

Fig. 4

panel (b): Nuclear spin Ramsey fringe: contrast (%) against free evolution time $\tau$ ($\mu$s) with the RF slightly detuned ($f_{\mathrm{RF}} = 151.44$ MHz, blue dots) and on resonance ($f_{\mathrm{RF}} = 151.60$ MHz, red squares), each with its fit. data.csv
panel (d): Nuclear spin Hahn echo: contrast (%) against total free evolution time $\tau$ ($\mu$s), measured points (blue dots) with the decay fit (blue line). data.csv

Fig. 5

panel (b): ODMR spectrum of a group II defect, normalized contrast against frequency (GHz): experiment (blue, points joined by a line) compared with the spectrum simulated for the positively charged C$_{\mathrm{B}}$C$_{\mathrm{N}}$-DAP-2 defect from its calculated hyperfine parameters (red). data.csv
panel (d): ODMR spectrum of a group III defect, normalized contrast against frequency (GHz): experiment (blue, points joined by a line) compared with the spectrum simulated for the positively charged C$_{\mathrm{B}}$O$_{\mathrm{N}}$ defect from its calculated hyperfine parameters (red). data.csv

Ext. Data Fig. 1

Illustrative figure, no extractable data. Shown in the paper PDF.

Cite

Xingyu Gao et al. (11 authors). Single nuclear spin detection and control in a van der Waals material. Nature 643, 943-949 (2025). https://doi.org/10.1038/s41586-025-09258-7

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