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Surface Adsorbates Suppress Low-Frequency Noise for Shallow Nitrogen-Vacancy Centers

Zhiyang Yuan1, David A. Fehr2, Kalliope Zervas1, Sorawis Sangtawesin1, Lila V. H. Rodgers1, Patryk Gumann3, Michael E. Flatté2,4, and Nathalie P. de Leon1,*

  • *Contact author: npdeleon@princeton.edu
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PRX Quantum 7, 043026 – Published 6 November, 2026

DOI: https://doi.org/10.1103/jc77-2nvb

Abstract

Shallow nitrogen-vacancy (NV) centers in diamond are promising nanoscale quantum sensors, yet their coherence is strongly limited by surface-induced noise. Surface adsorbates are widely believed to be a major source of decoherence. Here, we test this assumption by characterizing shallow single NV centers under ultrahigh vacuum (UHV) conditions, where the diamond surface is kept free of adsorbates, and comparing their behavior to ambient conditions. Surprisingly, we observe a ∼4× reduction in the Hahn echo coherence time T2 in UHV. By combining Hahn echo measurements in the single-quantum and double-quantum (DQ) bases, we separate contributions from different noise sources and find that both electric and magnetic noise are enhanced in UHV. In contrast, T1 measurements reveal an increased DQ T1 in UHV, indicating suppressed electric field noise in the ∼100  MHz frequency regime. These results point to a modification of the surface noise spectrum upon adsorbate removal, with different frequency regimes arising from distinct microscopic mechanisms. Specifically, we find that the low-frequency noise is consistent with increased surface charge in UHV that can be compensated by surface adsorbates in ambient conditions. Our findings highlight a complex and previously underappreciated role of surface adsorbates in shaping the noise environment of shallow NV centers, with important implications for nanoscale quantum sensing.

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Popular Summary

Nitrogen-vacancy (NV) centers in diamond are versatile nanoscale quantum sensors. For the best sensitivity and resolution, they must sit close to the diamond surface, where surface noise limits their performance. Surface adsorbates are widely believed to be a major culprit. We tested this by annealing a diamond in a custom-built ultrahigh-vacuum chamber, which keeps the surface free of adsorbates, and comparing the same individual NV centers in vacuum and in air. Surprisingly, the clean surface shortened their coherence times. Removing adsorbates reshapes the surface noise: low-frequency electric and magnetic noise are stronger, while high-frequency electric noise is suppressed. These findings revise the common picture of surface adsorbates. Rather than acting only as a noise source, they can also stabilize the electrostatic environment by dissipating excess surface charge, a key consideration for engineering better quantum platforms.

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References (59)

  1. J. Du, F. Shi, X. Kong, F. Jelezko, and J. Wrachtrup, Single-molecule scale magnetic resonance spectroscopy using quantum diamond sensors, Rev. Mod. Phys. 96, 025001 (2024).
  2. J. R. Maze, P. L. Stanwix, J. S. Hodges, S. Hong, J. M. Taylor, P. Cappellaro, L. Jiang, M. V. G. Dutt, E. Togan, A. S. Zibrov, A. Yacoby, R. L. Walsworth, and M. D. Lukin, Nanoscale magnetic sensing with an individual electronic spin in diamond, Nature (London) 455, 644 (2008).
  3. G. Balasubramanian, I. Y. Chan, R. Kolesov, M. Al-Hmoud, J. Tisler, C. Shin, C. Kim, A. Wojcik, P. R. Hemmer, A. Krueger, T. Hanke, A. Leitenstorfer, R. Bratschitsch, F. Jelezko, and J. Wrachtrup, Nanoscale imaging magnetometry with diamond spins under ambient conditions, Nature (London) 455, 648 (2008).
  4. P. Maletinsky, S. Hong, M. S. Grinolds, B. Hausmann, M. D. Lukin, R. L. Walsworth, M. Loncar, and A. Yacoby, A robust scanning diamond sensor for nanoscale imaging with single nitrogen-vacancy centres, Nat. Nanotechnol. 7, 320 (2012).
  5. J. M. Taylor, P. Cappellaro, L. Childress, L. Jiang, D. Budker, P. R. Hemmer, A. Yacoby, R. Walsworth, and M. D. Lukin, High-sensitivity diamond magnetometer with nanoscale resolution, Nat. Phys. 4, 810 (2008).
  6. L. V. H. Rodgers, S. T. Nguyen, J. H. Cox, K. Zervas, Z. Yuan, S. Sangtawesin, A. Stacey, C. Jaye, C. Weiland, A. Pershin, A. Gali, L. Thomsen, S. A. Meynell, L. B. Hughes, A. C. B. Jayich, X. Gui, R. J. Cava, R. R. Knowles, and N. P. de Leon, Diamond surface functionalization via visible light–driven C–H activation for nanoscale quantum sensing, Proc. Natl. Acad. Sci. 121, e2316032121 (2024).
  7. J. Rovny, S. Gopalakrishnan, A. C. B. Jayich, P. Maletinsky, E. Demler, and N. P. de Leon, Nanoscale diamond quantum sensors for many-body physics, Nat. Rev. Phys. 6, 753 (2024).
  8. F. Casola, T. van der Sar, and A. Yacoby, Probing condensed matter physics with magnetometry based on nitrogen-vacancy centres in diamond, Nat. Rev. Mater. 3, 17088 (2018).
  9. R. Schirhagl, K. Chang, M. Loretz, and C. L. Degen, Nitrogen-vacancy centers in diamond: Nanoscale sensors for physics and biology, Annu. Rev. Phys. Chem. 65, 83 (2014).
  10. G. Kucsko, P. C. Maurer, N. Y. Yao, M. Kubo, H. J. Noh, P. K. Lo, H. Park, and M. D. Lukin, Nanometre-scale thermometry in a living cell, Nature (London) 500, 54 (2013).
  11. I. Lovchinsky, A. O. Sushkov, E. Urbach, N. P. de Leon, S. Choi, K. De Greve, R. Evans, R. Gertner, E. Bersin, C. Müller, L. McGuinness, F. Jelezko, R. L. Walsworth, H. Park, and M. D. Lukin, Nuclear magnetic resonance detection and spectroscopy of single proteins using quantum logic, Science 351, 836 (2016).
  12. H. J. Mamin, M. Kim, M. H. Sherwood, C. T. Rettner, K. Ohno, D. D. Awschalom, and D. Rugar, Nanoscale nuclear magnetic resonance with a nitrogen-vacancy spin sensor, Science 339, 557 (2013).
  13. S. Sangtawesin, B. L. Dwyer, S. Srinivasan, J. J. Allred, L. V. H. Rodgers, K. De Greve, A. Stacey, N. Dontschuk, K. M. O’Donnell, D. Hu, D. A. Evans, C. Jaye, D. A. Fischer, M. L. Markham, D. J. Twitchen, H. Park, M. D. Lukin, and N. P. de Leon, Origins of diamond surface noise probed by correlating single-spin measurements with surface spectroscopy, Phys. Rev. X 9, 031052 (2019).
  14. T. Rosskopf, A. Dussaux, K. Ohashi, M. Loretz, R. Schirhagl, H. Watanabe, S. Shikata, K. M. Itoh, and C. Degen, Investigation of surface magnetic noise by shallow spins in diamond, Phys. Rev. Lett. 112, 147602 (2014).
  15. Y. Romach, C. Müller, T. Unden, L. J. Rogers, T. Isoda, K. M. Itoh, M. Markham, A. Stacey, J. Meijer, S. Pezzagna, B. Naydenov, L. P. McGuinness, N. Bar-Gill, and F. Jelezko, Spectroscopy of surface-induced noise using shallow spins in diamond, Phys. Rev. Lett. 114, 017601 (2015).
  16. B. A. Myers, A. Das, M. Dartiailh, K. Ohno, D. D. Awschalom, and A. Bleszynski Jayich, Probing surface noise with depth-calibrated spins in diamond, Phys. Rev. Lett. 113, 027602 (2014).
  17. K. Ohno, F. Joseph Heremans, L. C. Bassett, B. A. Myers, D. M. Toyli, A. C. Bleszynski Jayich, C. J. Palmstrøm, and D. D. Awschalom, Engineering shallow spins in diamond with nitrogen delta-doping, Appl. Phys. Lett. 101, 082413 (2012).
  18. B. K. Ofori-Okai, S. Pezzagna, K. Chang, M. Loretz, R. Schirhagl, Y. Tao, B. A. Moores, K. Groot-Berning, J. Meijer, and C. L. Degen, Spin properties of very shallow nitrogen vacancy defects in diamond, Phys. Rev. B 86, 081406 (2012).
  19. D. Bluvstein, Z. Zhang, and A. C. B. Jayich, Identifying and mitigating charge instabilities in shallow diamond nitrogen-vacancy centers, Phys. Rev. Lett. 122, 076101 (2019).
  20. Z. Yuan, M. Fitzpatrick, L. V. H. Rodgers, S. Sangtawesin, S. Srinivasan, and N. P. de Leon, Charge state dynamics and optically detected electron spin resonance contrast of shallow nitrogen-vacancy centers in diamond, Phys. Rev. Res. 2, 033263 (2020).
  21. H. Yamano, S. Kawai, K. Kato, T. Kageura, M. Inaba, T. Okada, I. Higashimata, M. Haruyama, T. Tanii, K. Yamada, S. Onoda, W. Kada, O. Hanaizumi, T. Teraji, J. Isoya, and H. Kawarada, Charge state stabilization of shallow nitrogen vacancy centers in diamond by oxygen surface modification, Jpn. J. Appl. Phys. 56, 04CK08 (2017).
  22. R. Giri, R. H. Jensen, D. Khurana, J. Bocquel, I. P. Radko, J. Lang, C. Osterkamp, F. Jelezko, K. Berg-Sorensen, U. L. Andersen, and A. Huck, Charge stability and charge-state-based spin readout of shallow nitrogen-vacancy centers in diamond, ACS Appl. Electron. Mater. 5, 6603 (2023).
  23. M. Haruyama, Y. Okigawa, M. Okada, H. Nakajima, T. Okazaki, H. Kato, T. Makino, and T. Yamada, Charge stabilization of shallow nitrogen-vacancy centers using graphene/diamond junctions, Appl. Phys. Lett. 122, 141601 (2023).
  24. M. Kim, H. Mamin, M. Sherwood, K. Ohno, D. D. Awschalom, and D. Rugar, Decoherence of near-surface nitrogen-vacancy centers due to electric field noise, Phys. Rev. Lett. 115, 087602 (2015).
  25. A. Stacey, N. Dontschuk, J.-P. Chou, D. A. Broadway, A. K. Schenk, M. J. Sear, J.-P. Tetienne, A. Hoffman, S. Prawer, C. I. Pakes, A. Tadich, N. P. de Leon, A. Gali, and L. C. L. Hollenberg, Evidence for primal sp2 defects at the diamond surface: Candidates for electron trapping and noise sources, Adv. Mater. Interfaces 6, 1801449 (2019).
  26. F. Fávaro de Oliveira, D. Antonov, Y. Wang, P. Neumann, S. A. Momenzadeh, T. Häußermann, A. Pasquarelli, A. Denisenko, and J. Wrachtrup, Tailoring spin defects in diamond by lattice charging, Nat. Commun. 8, 15409 (2017).
  27. T. Yamamoto, T. Umeda, K. Watanabe, S. Onoda, M. L. Markham, D. J. Twitchen, B. Naydenov, L. P. McGuinness, T. Teraji, S. Koizumi, F. Dolde, H. Fedder, J. Honert, J. Wrachtrup, T. Ohshima, F. Jelezko, and J. Isoya, Extending spin coherence times of diamond qubits by high-temperature annealing, Phys. Rev. B 88, 075206 (2013).
  28. T. L. Barr and S. Seal, Nature of the use of adventitious carbon as a binding energy standard, J. Vac. Sci. Technol. a: 13, 1239 (1995).
  29. G. Greczynski and L. Hultman, X-ray photoelectron spectroscopy: Towards reliable binding energy referencing, Prog. Mater. Sci. 107, 100591 (2020).
  30. L. H. Grey, H.-Y. Nie, and M. C. Biesinger, Defining the nature of adventitious carbon and improving its merit as a charge correction reference for XPS, Appl. Surf. Sci. 653, 159319 (2024).
  31. P. Rivero, W. Shelton, and V. Meunier, Surface properties of hydrogenated diamond in the presence of adsorbates: A hybrid functional DFT study, Carbon 110, 469 (2016).
  32. V. Chakrapani, S. C. Eaton, A. B. Anderson, M. Tabib-Azar, and J. C. Angus, Studies of adsorbate-induced conductance of diamond surfaces, Electrochem. Solid-State Lett. 8, E4 (2005).
  33. C. E. Nebel, B. Rezek, D. Shin, and H. Watanabe, Surface electronic properties of H-terminated diamond in contact with adsorbates and electrolytes, Phys. Status Solidi A 203, 3273 (2006).
  34. Z. Yuan, S. Sangtawesin, L. V. H. Rodgers, K. Zervas, J. J. Allred, J. Rovny, P. Gumann, and N. P. de Leon, An integrated ultrahigh vacuum cluster tool for diamond surface science and single nitrogen-vacancy center measurements, arXiv:2606.13961.
  35. M. Kaviani, P. Deák, B. Aradi, T. Frauenheim, J.-P. Chou, and A. Gali, Proper surface termination for luminescent near-surface NV centers in diamond, Nano Lett. 14, 4772 (2014).
  36. L. M. Pham, S. J. DeVience, F. Casola, I. Lovchinsky, A. O. Sushkov, E. Bersin, J. Lee, E. Urbach, P. Cappellaro, H. Park, A. Yacoby, M. Lukin, and R. L. Walsworth, NMR technique for determining the depth of shallow nitrogen-vacancy centers in diamond, Phys. Rev. B 93, 045425 (2016).
  37. H. J. Mamin, M. H. Sherwood, M. Kim, C. T. Rettner, K. Ohno, D. D. Awschalom, and D. Rugar, Multipulse double-quantum magnetometry with near-surface nitrogen-vacancy centers, Phys. Rev. Lett. 113, 030803 (2014).
  38. F. Dolde, H. Fedder, M. W. Doherty, T. Nöbauer, F. Rempp, G. Balasubramanian, T. Wolf, F. Reinhard, L. C. L. Hollenberg, F. Jelezko, and J. Wrachtrup, Electric-field sensing using single diamond spins, Nat. Phys. 7, 459 (2011).
  39. D. R. Candido and M. E. Flatté, Interplay between charge and spin noise in the near-surface theory of decoherence and relaxation of C3v symmetry qutrit spin-1 centers, Phys. Rev. B 110, 024419 (2024).
  40. B. A. Myers, A. Ariyaratne, and A. B. Jayich, Double-quantum spin-relaxation limits to coherence of near-surface nitrogen-vacancy centers, Phys. Rev. Lett. 118, 197201 (2017).
  41. N. Bar-Gill, L. M. Pham, C. Belthangady, D. Le Sage, P. Cappellaro, J. R. Maze, M. D. Lukin, A. Yacoby, and R. Walsworth, Suppression of spin-bath dynamics for improved coherence of multi-spin-qubit systems, Nat. Commun. 3, 858 (2012).
  42. G. de Lange, Z. H. Wang, D. Ristè, V. V. Dobrovitski, and R. Hanson, Universal dynamical decoupling of a single solid-state spin from a spin bath, Science 330, 60 (2010).
  43. S. Lin, C. Weng, J. Wang, Y. Guo, Y. Yang, J. Zhao, P. Ma, Y. Chen, L. Lou, W. Zhu, and G. Wang, Diamond surface electric-field noise detection using shallow nitrogen-vacancy centers, Phys. Rev. B 106, 165406 (2022).
  44. J. N. Neethirajan, T. Hache, D. Paone, D. Pinto, A. Denisenko, R. Stöhr, P. Udvarhelyi, A. Pershin, A. Gali, J. Wrachtrup et al., Controlled surface modification to revive shallow NV− centers, Nano Lett. 23, 2563 (2023).
  45. K. R. Brown, J. Chiaverini, J. M. Sage, and H. Häffner, Materials challenges for trapped-ion quantum computers, Nat. Rev. Mater. 6, 892 (2021).
  46. A. Chatterjee, P. Stevenson, S. De Franceschi, A. Morello, N. P. de Leon, and F. Kuemmeth, Semiconductor qubits in practice, Nat. Rev. Phys. 3, 157 (2021).
  47. N. P. de Leon, K. M. Itoh, D. Kim, K. K. Mehta, T. E. Northup, H. Paik, B. S. Palmer, N. Samarth, S. Sangtawesin, and D. W. Steuerman, Materials challenges and opportunities for quantum computing hardware, Science 372, eabb2823 (2021).
  48. D. A. Hite, Y. Colombe, A. C. Wilson, D. T. C. Allcock, D. Leibfried, D. J. Wineland, and D. P. Pappas, Surface science for improved ion traps, MRS Bull. 38, 826 (2013).
  49. A. Laikhtman, A. Lafosse, Y. Le Coat, R. Azria, and A. Hoffman, Interaction of water vapor with bare and hydrogenated diamond film surfaces, Surf. Sci. 551, 99 (2004).
  50. Z. Xu, M. L. Palm, W. Huxter, K. Herb, J. M. Abendroth, K. Bouzehouane, O. Boulle, M. S. Gabor, J. Urrestarazu Larranaga, A. Morales, J. Rhensius, G. Puebla-Hellmann, and C. L. Degen, Minimizing sensor-sample distances in scanning nitrogen-vacancy magnetometry, ACS Nano 19, 8255 (2025).
  51. M. Loretz, S. Pezzagna, J. Meijer, and C. L. Degen, Nanoscale nuclear magnetic resonance with a 1.9-nm-deep nitrogen-vacancy sensor, Appl. Phys. Lett. 104, 033102 (2014).
  52. C. L. Degen, M. Poggio, H. J. Mamin, C. T. Rettner, and D. Rugar, Nanoscale magnetic resonance imaging, Proc. Natl. Acad. Sci. 106, 1313 (2009).
  53. A. Ajoy, Y.-X. Liu, K. Saha, L. Marseglia, J.-C. Jaskula, U. Bissbort, and P. Cappellaro, Quantum interpolation for high-resolution sensing, Proc. Natl. Acad. Sci. 114, 2149 (2017).
  54. F. N. Li, R. Akhvlediani, M. K. Kuntumalla, and A. Hoffman, Oxygen bonding configurations and defects on differently oxidized diamond surfaces studied by high resolution electron energy loss spectroscopy and x-ray photoelectron spectroscopy measurements, Appl. Surf. Sci. 465, 313 (2019).
  55. T. Haensel, J. Uhlig, R. J. Koch, S. I.-U. Ahmed, J. A. Garrido, D. Steinmüller-Nethl, M. Stutzmann, and J. A. Schaefer, Influence of hydrogen on nanocrystalline diamond surfaces investigated with HREELS and XPS, Phys. Status Solidi A 206, 2022 (2009).
  56. N. Dontschuk, L. V. H. Rodgers, J. P. Chou, D. A. Evans, K. M. O’Donnell, H. J. Johnson, A. Tadich, A. K. Schenk, A. Gali, N. P. de Leon, and A. Stacey, X-ray quantification of oxygen groups on diamond surfaces for quantum applications, Mater. Quantum Technol. 3, 045901 (2023).
  57. K. Bobrov, H. Shechter, M. Folman, and A. Hoffman, Deuterium adsorption-desorption from diamond (100) single crystal surfaces studied by TPD, Diam. Relat. Mater. 7, 170 (1998).
  58. F. Maier, M. Riedel, B. Mantel, J. Ristein, and L. Ley, Origin of surface conductivity in diamond, Phys. Rev. Lett. 85, 3472 (2000).
  59. J. Zikovsky, S. A. Dogel, A. J. Dickie, J. L. Pitters, and R. A. Wolkow, Reaction of a hydrogen-terminated Si (100) surface in uhv with ion-pump generated radicals, J. Vac. Sci. Technol. A 27, 248 (2009).

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PRX Quantum 7, 043026– Published 6 November, 2026
  • Received 2 August 2026
  • Accepted 8 October 2026
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