- Open Access
Quantum Memory Enhanced Multipoint Correlation Spectroscopy for Statistically Polarized NMR
Phys. Rev. Lett. 135, 250801 – Published 15 December, 2025
DOI: https://doi.org/10.1103/1cj2-rxkm
Abstract
Nuclear magnetic resonance spectroscopy with solid-state spin sensors is a promising pathway for the detection of nuclear spins at the micro- and nanoscale. Although many nanoscale experiments rely on a single sensor spin for the detection of the signal, leveraging spin ensembles can enhance sensitivity, particularly in cases in which the signal merely originates from statistically polarized nuclear spins. In this Letter, we introduce multipoint correlation spectroscopy, which combines the advantages of two well-established methods—correlation spectroscopy and quantum heterodyne detection—to enable temporally efficient measurements of statistically polarized samples at the nanoscale with spin ensembles. We present a theoretical framework for this approach and demonstrate an experimental proof of concept with a nitrogen vacancy center in diamond. We achieve single hertz uncertainty in the estimated signal frequency, highlighting the potential applications of the technique for nanoscale nuclear magnetic resonance.
Physics Subject Headings (PhySH)
See Also
Efficient Detection of Statistical RF Fields with a Quantum Sensor
Article Text
Supplemental Material
References (63)
- C. Munuera-Javaloy, A. Tobalina, and J. Casanova, Phys. Rev. Lett. 130, 133603 (2023).
- R. D. Allert, K. D. Briegel, and D. B. Bucher, Chem. Commun. 58, 8165 (2022).
- P. Alsina-Bol’ivar, A. Biteri-Uribarren, C. Munuera-Javaloy, and J. Casanova, Phys. Rev. Res. 6, 043017 (2024).
- H. J. Mamin, M. Kim, M. H. Sherwood, C. T. Rettner, K. Ohno, D. D. Awschalom, and D. Rugar, Science 339, 557 (2013).
- T. Staudacher, F. Shi, S. Pezzagna, J. Meijer, J. Du, C. A. Meriles, F. Reinhard, and J. Wrachtrup, Science 339, 561 (2013).
- I. Schwartz, J. Rosskopf, S. Schmitt, B. Tratzmiller, Q. Chen, L. P. McGuinness, F. Jelezko, and M. B. Plenio, Sci. Rep. 9, 6938 (2019).
- N. Staudenmaier, A. Vijayakumar-Sreeja, S. Oviedo-Casado, G. Genov, D. Cohen, D. Dulog, T. Unden, N. Striegler, A. Marshall, J. Scheuer, C. Findler, J. Lang, I. Schwartz, P. Neumann, A. Retzker, and F. Jelezko, npj Quantum Inf. 8, 120 (2022).
- N. Staudenmaier, A. Vijayakumar-Sreeja, G. Genov, D. Cohen, C. Findler, J. Lang, A. Retzker, F. Jelezko, and S. Oviedo-Casado, Phys. Rev. Lett. 131, 150801 (2023).
- J. Du, F. Shi, X. Kong, F. Jelezko, and J. Wrachtrup, Rev. Mod. Phys. 96, 025001 (2024).
- A. O. Sushkov, I. Lovchinsky, N. Chisholm, R. L. Walsworth, H. Park, and M. D. Lukin, Phys. Rev. Lett. 113, 197601 (2014).
- Y. Wu, F. Jelezko, M. B. Plenio, and T. Weil, Angew. Chem., Int. Ed. Engl. 55, 6586 (2016).
- S. J. DeVience, L. M. Pham, I. Lovchinsky, A. O. Sushkov, N. Bar-Gill, C. Belthangady, F. Casola, M. Corbett, H. Zhang, M. Lukin et al., Nat. Nanotechnol. 10, 129 (2015).
- A. Laraoui, F. Dolde, C. Burk, F. Reinhard, J. Wrachtrup, and C. A. Meriles, Nat. Commun. 4, 1651 (2013).
- T. Staudacher, N. Raatz, S. Pezzagna, J. Meijer, F. Reinhard, C. A. Meriles, and J. Wrachtrup, Nat. Commun. 6, 8527 (2015).
- X. Kong, A. Stark, J. Du, L. P. McGuinness, and F. Jelezko, Phys. Rev. Appl. 4, 024004 (2015).
- S. Zaiser, T. Rendler, I. Jakobi, T. Wolf, S. Y. Lee, S. Wagner, V. Bergholm, T. Schulte-Herbrüggen, P. Neumann, and J. Wrachtrup, Nat. Commun. 7, 1 (2016).
- M. Pfender, N. Aslam, H. Sumiya, S. Onoda, P. Neumann, J. Isoya, C. A. Meriles, and J. Wrachtrup, Nat. Commun. 8, 1 (2017).
- S. Schmitt, T. Gefen, F. M. Stürner, T. Unden, G. Wolff, C. Müller, J. Scheuer, B. Naydenov, M. Markham, S. Pezzagna, J. Meijer, I. Schwarz, M. Plenio, A. Retzker, L. P. McGuinness, and F. Jelezko, Science 356, 832 (2017).
- J. M. Boss, K. S. Cujia, J. Zopes, and C. L. Degen, Science 356, 837 (2017).
- D. R. Glenn, D. B. Bucher, J. Lee, M. D. Lukin, H. Park, and R. L. Walsworth, Nature (London) 555, 351 (2018).
- N. Arunkumar, D. B. Bucher, M. J. Turner, P. TomHon, D. Glenn, S. Lehmkuhl, M. D. Lukin, H. Park, M. S. Rosen, T. Theis, and R. L. Walsworth, PRX Quantum 2, 010305 (2021).
- N. R. Neuling, R. D. Allert, and D. B. Bucher, Curr. Opin. Biotechnol. 83, 102975 (2023).
- T. Rosskopf, J. Zopes, J. M. Boss, and C. L. Degen, npj Quantum Inf. 3, 33 (2017).
- J. F. Barry, J. M. Schloss, E. Bauch, M. J. Turner, C. A. Hart, L. M. Pham, and R. L. Walsworth, Rev. Mod. Phys. 92, 015004 (2020).
- See Supplemental Material at http://link.aps.org/supplemental/10.1103/1cj2-rxkm, for details on the theory multipoint correlation spectroscopy and additional experimental results, which includes Refs. [26–59].
- P. Neumann, J. Beck, M. Steiner, F. Rempp, H. Fedder, P. R. Hemmer, J. Wrachtrup, and F. Jelezko, Science 329, 542 (2010).
- T. Gullion, D. B. Baker, and M. S. Conradi, J. Magn. Reson. 89, 479 (1990).
- C. L. Degen, F. Reinhard, and P. Cappellaro, Rev. Mod. Phys. 89, 035002 (2017).
- D. Suter and G. A. Álvarez, Rev. Mod. Phys. 88, 041001 (2016).
- G. T. Genov, D. Schraft, N. V. Vitanov, and T. Halfmann, Phys. Rev. Lett. 118, 133202 (2017).
- G. T. Genov, Y. Ben-Shalom, F. Jelezko, A. Retzker, and N. Bar-Gill, Phys. Rev. Res. 2, 033216 (2020).
- D. Louzon, G. T. Genov, N. Staudenmaier, F. Frank, J. Lang, M. L. Markham, A. Retzker, and F. Jelezko, Phys. Rev. Lett. 134, 120802 (2025).
- J. M. Binder, A. Stark, N. Tomek, J. Scheuer, F. Frank, K. D. Jahnke, C. Müller, S. Schmitt, M. H. Metsch, T. Unden, T. Gehring, A. Huck, U. L. Andersen, L. J. Rogers, and F. Jelezko, SoftwareX 6, 85 (2017).
- D. Cohen, R. Nigmatullin, M. Eldar, and A. Retzker, Adv. Quantum Technol. 3, 2000019 (2020).
- K. S. Liu, X. Ma, R. Rizzato, A. L. Semrau, A. Henning, I. D. Sharp, R. A. Fischer, and D. B. Bucher, Nano Lett. 22, 9876 (2022).
- W. Zheng, S. Zhang, J. Jiang, Y. He, R. Stöhr, A. Denisenko, J. Wrachtrup, X. C. Zeng, K. Bian, E.-G. Wang et al., arXiv:2412.15001.
- R. Maier, C.-I. Ho, H. Sumiya, S. Onoda, J. Isoya, V. Vorobyov, and J. Wrachtrup, following Letter, Phys. Rev. Lett. 135, 250802 (2025).
- D. Suter and F. Jelezko, Prog. Nucl. Magn. Reson. Spectrosc. 98–99, 50 (2017).
- V. Jacques, P. Neumann, J. Beck, M. Markham, D. Twitchen, J. Meijer, F. Kaiser, G. Balasubramanian, F. Jelezko, and J. Wrachtrup, Phys. Rev. Lett. 102, 057403 (2009).
- A. M. Souza, G. A. Álvarez, and D. Suter, Phil. Trans. R. Soc. A 370, 4748 (2012).
- S. Oviedo-Casado, A. Rotem, R. Nigmatullin, J. Prior, and A. Retzker, Sci. Rep. 10, 19691 (2020).
- E. Hahn, Phys. Rev. 80, 580 (1950).
- Z.-Y. Wang, J. E. Lang, S. Schmitt, J. Lang, J. Casanova, L. McGuinness, T. S. Monteiro, F. Jelezko, and M. B. Plenio, Phys. Rev. Lett. 122, 200403 (2019).
- M. Garwood and Y. Ke, J. Magn. Reson. 94, 511 (1991).
- A. Tannús and M. Garwood, NMR Biomed. 10, 423 (1997).
- T. Joas, F. Ferlemann, R. Sailer, P. J. Vetter, J. Zhang, R. S. Said, T. Teraji, S. Onoda, T. Calarco, G. Genov, M. M. Müller, and F. Jelezko, Phys. Rev. X 15, 021069 (2025).
- D. Daems, A. Ruschhaupt, D. Sugny, and S. Guérin, Phys. Rev. Lett. 111, 050404 (2013).
- L. Van-Damme, D. Schraft, G. T. Genov, D. Sugny, T. Halfmann, and S. Guérin, Phys. Rev. A 96, 022309 (2017).
- M. H. Levitt, Prog. Nucl. Magn. Reson. Spectrosc. 18, 61 (1986).
- G. T. Genov, D. Schraft, T. Halfmann, and N. V. Vitanov, Phys. Rev. Lett. 113, 043001 (2014).
- P. Rembold, N. Oshnik, M. M. Müller, S. Montangero, T. Calarco, and E. Neu, AVS Quantum Sci. 2, 024701 (2020).
- H. M. Lim, G. T. Genov, R. Sailer, A. Fahrurrachman, M. A. Majidi, F. Jelezko, and R. S. Said, Phys. Rev. Appl. 24, 054064 (2025).
- J. Yoon, K. Zhong, G. Wang, B. Li, D. Lee, and P. Cappellaro, arXiv:2504.12134.
- Y.-X. Liu, A. Ajoy, and P. Cappellaro, Phys. Rev. Lett. 122, 100501 (2019).
- A. Jarmola, A. Berzins, J. Smits, K. Smits, J. Prikulis, F. Gahbauer, R. Ferber, D. Erts, M. Auzinsh, and D. Budker, Appl. Phys. Lett. 107, 242403 (2015).
- P. J. Vetter, T. Reisser, M. G. Hirsch, T. Calarco, F. Motzoi, F. Jelezko, and M. M. Müller, npj Quantum Inf. 10, 96 (2024).
- P. J. Vetter, A. Marshall, G. T. Genov, T. F. Weiss, N. Striegler, E. F. Großmann, S. Oviedo-Casado, J. Cerrillo, J. Prior, P. Neumann et al., Phys. Rev. Appl. 17, 044028 (2022).
- J. Fuhrmann, C. Findler, M. Olney-Fraser, L. Kazak, and F. Jelezko, Adv. Funct. Mater. 2501661 (2025), 10.1002/adfm.202501661.
- B. Herzog, D. Cadeddu, F. Xue, P. Peddibhotla, and M. Poggio, Appl. Phys. Lett. 105, 043112 (2014).
- D. Wirtitsch, G. Wachter, S. Reisenbauer, M. Gulka, V. Ivády, F. Jelezko, A. Gali, M. Nesladek, and M. Trupke, Phys. Rev. Res. 5, 013014 (2023).
- D. A. Hopper, J. D. Lauigan, T.-Y. Huang, and L. C. Bassett, Phys. Rev. Appl. 13, 024016 (2020).
- L. M. Pham, S. J. DeVience, F. Casola, I. Lovchinsky, A. O. Sushkov, E. Bersin, J. Lee, E. Urbach, P. Cappellaro, H. Park et al., Phys. Rev. B 93, 045425 (2016).
- T. Spohn, Plot data for manuscript: “Quantum memory enhanced multipoint correlation spectroscopy for statistically polarized NMR”, Zenodo, 10.5281/zenodo.17659892 (2025).