- Open Access
High-sensitivity optical detection of electron-nuclear spin clusters in diamond
Phys. Rev. Research 8, 023337 – Published 25 June, 2026
DOI: https://doi.org/10.1103/g88t-fddb
Abstract
We perform sensitive nuclear magnetic resonance (NMR) with spin ensembles that are polarized by nitrogen-vacancy (NV) centers in diamond at room temperature. Using stabilized lasers, a balanced detection, and a highly uniform magnetic field, we resolve sharp NMR features arising from multiple spin clusters. In particular, we investigate the coupling between nuclear spins and NV centers in the neutral and negatively charged states. Further, we perform high-precision NMR and coherent control of families of nuclear spin ensembles in the level of the NV ground state. Applying an off-axis magnetic field reveals the various sites associated with the otherwise degenerate couplings of the sites around the NV electronic spin, providing access to all the hyperfine tensor components. Finally, we observe spectroscopic signatures of pairs of nuclear spins coupled to the same NV center. These results are relevant for ensemble measurements of dynamical polarization that currently rely on expensive nuclear magnetic resonance systems as well as for recently proposed nuclear spin gyroscopes.
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References (56)
- M. H. Appel, A. Ghorbal, N. Shofer, L. Zaporski, S. Manna, S. F. C. da Silva, U. Haeusler, C. Le Gall, A. Rastelli, D. A. Gangloff, and M. Atatüre, Many-body quantum register for a spin qubit, Nat. Phys. 21, 368 (2024).
- J. C. Marcks, B. Pingault, J. Zhang, C. Zeledon, F. J. Heremans, and D. D. Awschalom, Nuclear spin engineering for quantum information science, J. Mater. Res. 40, 1433 (2025).
- J. Kenny, F. Zhou, R. He, F. Jelezko, T. S. Koh, and W. Gao, Quantum sensing enhancement through a nuclear spin register in nitrogen-vacancy centers in diamond, Appl. Phys. Rev. 12, 021323 (2025).
- C. E. Bradley, J. Randall, M. H. Abobeih, R. C. Berrevoets, M. J. Degen, M. A. Bakker, M. Markham, D. J. Twitchen, and T. H. Taminiau, A ten-qubit solid-state spin register with quantum memory up to one minute, Phys. Rev. X 9, 031045 (2019).
- M. P. Ledbetter, K. Jensen, R. Fischer, A. Jarmola, and D. Budker, Gyroscopes based on nitrogen-vacancy centers in diamond, Phys. Rev. A 86, 052116 (2012).
- A. Ajoy and P. Cappellaro, Stable three-axis nuclear-spin gyroscope in diamond, Phys. Rev. A 86, 062104 (2012).
- A. Jarmola, S. Lourette, V. M. Acosta, A. G. Birdwell, P. Blümler, D. Budker, T. Ivanov, and V. S. Malinovsky, Demonstration of diamond nuclear spin gyroscope, Sci. Adv. 7, eabl3840 (2021).
- J. Smits, J. T. Damron, P. Kehayias, A. F. McDowell, N. Mosavian, I. Fescenko, N. Ristoff, A. Laraoui, A. Jarmola, and V. M. Acosta, Two-dimensional nuclear magnetic resonance spectroscopy with a microfluidic diamond quantum sensor, Sci. Adv. 5, eaaw7895 (2019).
- J.-P. Tetienne, L. T. Hall, A. J. Healey, G. A. L. White, M.-A. Sani, F. Separovic, and L. C. L. Hollenberg, Prospects for nuclear spin hyperpolarization of molecular samples using nitrogen-vacancy centers in diamond, Phys. Rev. B 103, 014434 (2021).
- R. Budakian et al., Roadmap on nanoscale magnetic resonance imaging, Nanotechnology 35, 412001 (2024).
- A. Ajoy et al., Room-temperature optical hyperpolarization in powdered diamond, Sci. Adv. 4, eaar5492 (2018).
- J. Scheuer, I. Schwartz, S. Müller, Q. Chen, I. Dhand, M. B. Plenio, B. Naydenov, and F. Jelezko, Robust techniques for polarization and detection of nuclear spin ensembles, Phys. Rev. B 96, 174436 (2017).
- J. Henshaw, D. Pagliero, P. R. Zangara, M. B. Franzoni, A. Ajoy, R. H. Acosta, J. A. Reimer, A. Pines, and C. A. Meriles, Carbon-13 dynamic nuclear polarization in diamond via a microwave-free integrated cross effect, Proc. Natl. Acad. Sci. USA 116, 18334 (2019).
- R. Blinder, Y. Mindarava, M. Korzeczek, A. Marshall, F. Glöckler, S. Nothelfer, A. Kienle, C. Laube, W. Knolle, C. Jentgens, M. B. Plenio, and F. Jelezko, hyperpolarization with nitrogen-vacancy centers in micro- and nanodiamonds for sensitive magnetic resonance applications, Sci. Adv. 11, eadq6836 (2025).
- B. Smeltzer, J. McIntyre, and L. Childress, Robust control of individual nuclear spins in diamond, Phys. Rev. A 80, 050302(R) (2009).
- M. Steiner, P. Neumann, J. Beck, F. Jelezko, and J. Wrachtrup, Universal enhancement of the optical readout fidelity of single electron spins at nitrogen-vacancy centers in diamond, Phys. Rev. B 81, 035205 (2010).
- A. Jarmola, I. Fescenko, V. M. Acosta, M. W. Doherty, F. K. Fatemi, T. Ivanov, D. Budker, and V. S. Malinovsky, Robust optical readout and characterization of nuclear spin transitions in nitrogen-vacancy ensembles in diamond, Phys. Rev. Res. 2, 023094 (2020).
- L. Childress, M. V. G. Dutt, J. M. Taylor, A. S. Zibrov, F. Jelezko, J. Wrachtrup, P. R. Hemmer, and M. D. Lukin, Coherent dynamics of coupled electron and nuclear spin qubits in diamond, Science 314, 281 (2006).
- A. Dréau, J.-R. Maze, M. Lesik, J.-F. Roch, and V. Jacques, High-resolution spectroscopy of single NV defects coupled with nearby nuclear spins in diamond, Phys. Rev. B 85, 134107 (2012).
- See Supplemental Material at http://link.aps.org/supplemental/10.1103/g88t-fddb for theoretical predictions and further experimental details, which includes Refs. [52, 53, 54, 55, 56].
- B. Smeltzer, L. Childless, and A. Gali, hyperfine interactions in the nitrogen-vacancy centre in diamond, New J. Phys. 13 025021 (2011).
- M. W. Doherty, N. B. Manson, P. Delaney, F. Jelezko, J. Wrachtrup, and L. C. Hollenberg, The nitrogen-vacancy colour centre in diamond, Phys. Rep. 528, 1 (2013).
- V. Jacques, P. Neumann, J. Beck, M. Markham, D. Twitchen, J. Meijer, F. Kaiser, G. Balasubramanian, F. Jelezko, and J. Wrachtrup, Dynamic polarization of single nuclear spins by optical pumping of nitrogen-vacancy color centers in diamond at room temperature, Phys. Rev. Lett. 102, 057403 (2009).
- R. Fischer, A. Jarmola, P. Kehayias, and D. Budker, Optical polarization of nuclear ensembles in diamond, Phys. Rev. B 87, 125207 (2013).
- A. Schweiger and G. Jeschke, Principles of Pulse Electron Paramagnetic Resonance (Oxford Academic, Oxford, 2023).
- S. Lourette, A. Jarmola, V. M. Acosta, A. G. Birdwell, D. Budker, M. W. Doherty, T. Ivanov, and V. S. Malinovsky, Temperature sensitivity of and ground-state manifolds, Phys. Rev. Appl. 19, 064084 (2023).
- S. Felton, A. M. Edmonds, M. E. Newton, P. M. Martineau, D. Fisher, and D. J. Twitchen, Electron paramagnetic resonance studies of the neutral nitrogen vacancy in diamond, Phys. Rev. B 77, 081201(R) (2008).
- L. Razinkovas, M. Maciaszek, F. Reinhard, M. W. Doherty, and A. Alkauskas, Photoionization of negatively charged NV centers in diamond: Theory and ab initio calculations, Phys. Rev. B 104, 235301 (2021).
- M. Pfender, N. Aslam, P. Simon, D. Antonov, G. Thiering, S. Burk, F. F. de Oliveira, A. Denisenko, H. Fedder, J. Meijer, J. A. Garrido, A. Gali, T. Teraji, J. Isoya, M. W. Doherty, A. Alkauskas, A. Gallo, A. Grüneis, P. Neumann, and J. Wrachtrup, Protecting a diamond quantum memory by charge state control, Nano Lett. 17, 5931 (2017).
- G. Waldherr, J. Beck, M. Steiner, P. Neumann, A. Gali, T. Frauenheim, F. Jelezko, and J. Wrachtrup, Dark states of single nitrogen-vacancy centers in diamond unraveled by single shot NMR, Phys. Rev. Lett. 106, 157601 (2011).
- P. Siyushev, H. Pinto, M. Vörös, A. Gali, F. Jelezko, and J. Wrachtrup, Optically controlled switching of the charge state of a single nitrogen-vacancy center in diamond at cryogenic temperatures, Phys. Rev. Lett. 110, 167402 (2013).
- S. Sangtawesin, C. A. McLellan, B. A. Myers, A. C. Bleszynski Jayich, D. D. Awschalom, and J. R. Petta, Hyperfine-enhanced gyromagnetic ratio of a nuclear spin in diamond, New J. Phys. 18, 083016 (2016).
- M. Chen, M. Hirose, and P. Cappellaro, Measurement of transverse hyperfine interaction by forbidden transitions, Phys. Rev. B 92, 020101(R) (2015).
- H. Duarte, H. T. Dinani, V. Jacques, and J. R. Maze, Effect of intersystem crossing rates and optical illumination on the polarization of nuclear spins close to nitrogen-vacancy centers, Phys. Rev. B 103, 195443 (2021).
- A. Gali, Identification of individual isotopes of nitrogen-vacancy center in diamond by combining the polarization studies of nuclear spins and first-principles calculations, Phys. Rev. B 80, 241204(R) (2009).
- V. Ivády, K. Szász, A. L. Falk, P. V. Klimov, D. J. Christle, E. Janzén, I. A. Abrikosov, D. D. Awschalom, and A. Gali, Theoretical model of dynamic spin polarization of nuclei coupled to paramagnetic point defects in diamond and silicon carbide, Phys. Rev. B 92, 115206 (2015).
- I. Takács and V. Ivády, Accurate hyperfine tensors for solid state quantum applications: Case of the NV center in diamond, Commun. Phys. 7, 178 (2024).
- B. Bürgler, T. F. Sjolander, O. Brinza, A. Tallaire, J. Achard, and P. Maletinsky, All-optical nuclear quantum sensing using nitrogen-vacancy centers in diamond, npj Quantum Inf. 9, 56 (2023).
- T. H. Taminiau, J. Cramer, T. van der Sar, V. V. Dobrovitski, and R. Hanson, Universal control and error correction in multi-qubit spin registers in diamond, Nat. Nanotechnol. 9, 171 (2014).
- F. Shi, X. Kong, P. Wang, F. Kong, N. Zhao, R.-B. Liu, and J. Du, Sensing and atomic-scale structure analysis of single nuclear-spin clusters in diamond, Nat. Phys. 10, 21 (2014).
- K. Herb, T. F. Segawa, L. A. Völker, J. M. Abendroth, E. Janitz, T. Zhu, and C. L. Degen, Multidimensional spectroscopy of nuclear spin clusters in diamond, Phys. Rev. Lett. 132, 133002 (2024).
- H. P. Bartling, M. H. Abobeih, B. Pingault, M. J. Degen, S. J. H. Loenen, C. E. Bradley, J. Randall, M. Markham, D. J. Twitchen, and T. H. Taminiau, Entanglement of spin-pair qubits with intrinsic dephasing times exceeding a minute, Phys. Rev. X 12, 011048 (2022).
- L. Nicolas, T. Delord, P. Jamonneau, R. Coto, J. Maze, V. Jacques, and G. Hétet, Coherent population trapping with a controlled dissipation: Applications in optical metrology, New J. Phys. 20, 033007 (2018).
- P. Jamonneau, G. Hétet, A. Dréau, J.-F. Roch, and V. Jacques, Coherent population trapping of a single nuclear spin under ambient conditions, Phys. Rev. Lett. 116, 043603 (2016).
- P. Jamonneau, A. Dréau, G. Hétet, J. F. Roch, J. R. Maze, and V. Jacques, Room-temperature polarization of individual nuclear spins in diamond via anisotropic hyperfine coupling and coherent population trapping, Eur. Phys. J. D 76, 228 (2022).
- P. Huillery, J. Leibold, T. Delord, L. Nicolas, J. Achard, A. Tallaire, and G. Hétet, Coherent microwave control of a nuclear spin ensemble at room temperature, Phys. Rev. B 103, L140102 (2021).
- S. Xu, M. Liu, T. Xie, Z. Zhao, Q. Shi, P. Yu, C.-K. Duan, F. Shi, and J. Du, High-precision measurements and first-principles explanation of the temperature-dependent and hyperfine interactions of single centers in diamond at room temperature, Phys. Rev. B 107, L140101 (2023).
- V. V. Soshenko, V. V. Vorobyov, S. V. Bolshedvorskii, O. Rubinas, I. Cojocaru, B. Kudlatsky, A. I. Zeleneev, V. N. Sorokin, A. N. Smolyaninov, and A. V. Akimov, Temperature drift rate for nuclear terms of the NV-center ground-state Hamiltonian, Phys. Rev. B 102, 125133 (2020).
- M. S. J. Barson, P. Reddy, S. Yang, N. B. Manson, J. Wrachtrup, and M. W. Doherty, Temperature dependence of the hyperfine structure of the negatively charged nitrogen-vacancy center in diamond, Phys. Rev. B 99, 094101 (2019).
- H. Wang, S. Wu, K. Jacobs, Y. Duan, D. R. Englund, and M. E. Trusheim, Cavity-enhanced solid-state nuclear spin gyroscope, Phys. Rev. Lett. 134, 183603 (2025).
- V. V. Soshenko, S. V. Bolshedvorskii, O. Rubinas, V. N. Sorokin, A. N. Smolyaninov, V. V. Vorobyov, and A. V. Akimov, Nuclear spin gyroscope based on the nitrogen vacancy center in diamond, Phys. Rev. Lett. 126, 197702 (2021).
- C. Findler, R. Blinder, K. Schüle, P. Balasubramanian, C. Osterkamp, and F. Jelezko, Detecting nitrogen-vacancy-hydrogen centers on the nanoscale using nitrogen-vacancy centers in diamond, Phys. Rev. Mater. 8, 026203 (2024).
- C. Pellet-Mary, M. Perdriat, P. Huillery, and G. Hétet, Relaxation processes in dipole-coupled nitrogen-vacancy centers in zero field: Application in magnetometry, Phys. Rev. Appl. 20, 034050 (2023).
- D. Pagliero, K. R. K. Rao, P. R. Zangara, S. Dhomkar, H. H. Wong, A. Abril, N. Aslam, A. Parker, J. King, C. E. Avalos, A. Ajoy, J. Wrachtrup, A. Pines, and C. A. Meriles, Multispin-assisted optical pumping of bulk nuclear spin polarization in diamond, Phys. Rev. B 97, 024422 (2018).
- R. Wunderlich, J. Kohlrautz, B. Abel, J. Haase, and J. Meijer, Optically induced cross relaxation via nitrogen-related defects for bulk diamond hyperpolarization, Phys. Rev. B 96, 220407(R) (2017).
- D. Shimon, K. A. Cantwell, L. Joseph, E. Q. Williams, Z. Peng, S. Takahashi, and C. Ramanathan, Large room temperature bulk DNP of via P1 centers in diamond, J. Phys. Chem. C 126, 17777 (2022).