Abstract
Detecting individual spins—including stable and metastable states—represents a fundamental challenge in quantum sensing, with broad applications across condensed matter physics1,2, quantum chemistry3 and single-molecule magnetic resonance imaging4,5. Although nitrogen–vacancy (NV) centres in diamond have emerged as powerful nanoscale sensors, their performance for single-spin detection remains constrained by substantial environmental noise and restricted sensing volume6,7. Here we propose and demonstrate an entanglement-enhanced sensing protocol that overcomes these limitations through the strategic use of entangled NV pairs. Our approach achieves a 3.4-fold enhancement in sensitivity and a 1.6-fold improvement in spatial resolution relative to single NV centres under ambient conditions. The protocol uses carefully engineered entangled states that amplify target spin signals through quantum interference while suppressing environmental noise. Crucially, we extend these capabilities to resolve metastable single-spin dynamics, directly observing stochastic transitions between different spin states by identifying state-dependent coupling strengths. This dual functionality enables simultaneous detection of static and dynamic spin species for studying complex quantum systems. The achieved performance establishes entanglement-enhanced sensing as a viable pathway towards atomic-scale characterization of quantum materials and interfaces.
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Data availability
Source data for the main figures are provided with this paper. Further data generated during the study are available from the corresponding authors on request.
Code availability
All code that supports the findings of this study is available from the corresponding authors on reasonable request.
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Acknowledgements
This work was supported by the National Natural Science Foundation of China (grant nos. T2325023, T2388102, 92265204, T2125011, 12474500, 12504570, 12504594 and 12261160569), the Quantum Science and Technology—National Science and Technology Major Project (grant no. 2021ZD0302200), the Fundamental Research Funds for the Central Universities, the Postdoctoral Fellowship Program and China Postdoctoral Science Foundation (grant no. BX20240347).
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Y.W. and J.D. conceived the idea. Y.W., M.W. and X.Z. designed the experiment. M.W. and X.Y. prepared the sample. X.Z., Y.G., H.S., S.H., Z.C. and W.J. performed the experiments and analysed the data. Y.W., X.Z., M.W., K.X., F.S. and J.D. wrote the manuscript. All authors discussed the results and commented on the manuscript. J.D. and Y.W. supervised the project.
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Extended data figures and tables
Extended Data Fig. 1 The electron spin position determined by magnetic dipole interaction results under different external magnetic fields.
a–c, Experimental measurements of NV–NV couplings. NVi+(−) denotes that the ith NV is prepared in the state ms = +1(−1). The angular parameters of the magnetic field θ and ϕ in spherical coordinates are defined through the coordinate transformation relationships from the Cartesian system (x, y, z), in which θ ∈ [0, π] denotes the polar angle and φ ∈ [0, 2π] specifies the azimuthal angle. d, The possible spatial positions of NV2 determined from the hyperfine coupling obtained in a according to ({r|[|A(r, B) − ANV1,NV2+| < ΔA] ∩ [|A(r, B) − ANV1,NV2−| < ΔA]}) with a coupling error of ΔA = 20 kHz used as illustration. e, Correlated determination of NV2 location according to hyperfine coupling of a (red band), b (blue band) and c (green band). The position of NV2 is listed in the upper-left corner. f, The spatial positioning schematic diagram of DS1 by the sensing of the entangled state (|ψ2⟩). Each band in the figure is determined by the effective coupling of the entangled states and DS1 under two magnetic fields (\(\{{\bf{r}}| [| A({\bf{r}},{{\bf{B}}}_{1})-{A}_{{\psi }_{2},{\rm{DS1}}}({{\bf{B}}}_{1})| < \Delta A]\cap [| A({\bf{r}},{{\bf{B}}}_{2})-{A}_{{\psi }_{2},{\rm{DS1}}}({{\bf{B}}}_{2})| < \Delta A]\}\)). For the red band, in the magnetic field (B0, θ, φ) = (100.6 G, 0.62π, 0.68π) and (B0, θ, φ) = (151.84 G, 0.696π, 0.5π), the effective couplings are 585 and 907 kHz, respectively. For the cyan band, in the magnetic field (B0, θ, φ) = (147.4 G, 0.7π, 1.58π) and (B0, θ, φ) = (66 G, 0.85π, 0.37π), the effective couplings are 702 and 359 kHz, respectively.
Extended Data Fig. 2 Dark spin resonance frequencies under different magnetic field directions.
Dark spin resonance frequencies measured by |ψ2⟩-DEER spectroscopy under external magnetic fields along the NV1 axis (a) and the NV2 axis (b).
Supplementary information
Supplementary Information (download PDF )
This Supplementary Information contains 6 Supplementary Figures, 1 Supplementary Table and Supplementary References and the following sections: 1. Fluorescence counts and ODMR of entangled NV pairs; 2. High-precision vector magnetic field measurement; 3. Entangled state preparation and sensing; 4. Decoherence analysis for entangled NV pairs; 5. Dark spin identification; 6. DS1 initialization and NV1–DS1 entangled state preparation; and 7. Sensitivity analysis.
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Zhou, X., Wang, M., Ye, X. et al. Entanglement-enhanced nanoscale single-spin sensing. Nature 647, 883–888 (2025). https://doi.org/10.1038/s41586-025-09790-6
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DOI: https://doi.org/10.1038/s41586-025-09790-6
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