Reuse & Permissions

It is not necessary to obtain permission to reuse this article or its components as it is available under the terms of the Creative Commons Attribution 4.0 International license. This license permits unrestricted use, distribution, and reproduction in any medium, provided attribution to the author(s) and the published article's title, journal citation, and DOI are maintained. Please note that some figures may have been included with permission from other third parties. It is your responsibility to obtain the proper permission from the rights holder directly for these figures.

Export citation

Export citation

Choose format for download:

Download Citation
  • Editors' Suggestion
  • Open Access

Hot-Phonon-Induced Distortion of Diamond Defects on Ultrafast Timescales

Terng Junn Keat1, Jiahui Zhao1, Jack M. Woolley1, Partha Malakar2, Gregory M. Greetham2, Xuxu Wu1, Jonathan P. Goss3, Robin J. Cruddace1, Christopher B. Hartland1 et al.

Matthew W. Dale4, Vasilios G. Stavros5, Mark E. Newton1, and James Lloyd-Hughes1,*

  • 1Department of Physics, University of Warwick, Coventry, CV4 7AL, United Kingdom
  • 2Central Laser Facility, Research Complex at Harwell, STFC Rutherford Appleton Laboratory, Harwell Science and Innovation Campus, Didcot, OX11 0QX, United Kingdom
  • 3School of Mathematics, Statistics and Physics, Newcastle University, Newcastle upon Tyne, NE1 7RU, United Kingdom
  • 4De Beers Group, Belmont Road, Maidenhead, SL6 6JW, United Kingdom
  • 5School of Chemistry, University of Birmingham, Birmingham, B15 2TT, United Kingdom

  • *Contact author: j.lloyd-hughes@warwick.ac.uk

Phys. Rev. Lett. 135, 216902 – Published 18 November, 2025

DOI: https://doi.org/10.1103/mvdf-bdrx

Abstract

We investigated ultrafast defect-lattice dynamics in diamond using the Ns:H−C0 defect, an analog of bond-centered hydrogen in semiconductors. Combining synthesis, ultrafast vibrational spectroscopy, and ab initio calculations, we show that excitation of the defect’s stretch mode leads to the generation of localized phonons and the formation of a hot ground state, where the interatomic potential is transiently modified. Our results reveal unexpected nonequilibrium phonon effects despite diamond’s exceptionally high thermal conductivity, with implications for quantum defect engineering.

View figure in article

Physics Subject Headings (PhySH)

Article Text

Supplemental Material

References (53)

  1. J. R. Weber, W. F. Koehl, J. B. Varley, A. Janotti, B. B. Buckley, C. G. V. D. Walle, and D. D. Awschalom, Proc. Natl. Acad. Sci. U.S.A. 107, 8513 (2010).
  2. L. Rondin, J.-P. Tetienne, T. Hingant, J.-F. Roch, P. Maletinsky, and V. Jacques, Rep. Prog. Phys. 77, 056503 (2014).
  3. Y. Zhou, A. Rasmita, K. Li, Q. Xiong, I. Aharonovich, and W.-B. Gao, Nat. Commun. 8, 14451 (2017).
  4. M. Cho, J. Chem. Phys. 157, 124201 (2022).
  5. M. Cho, J. Chem. Phys. 159, 224104 (2023).
  6. A. Cox, M. E. Newton, and J. M. Baker, J. Phys. Condens. Matter 6, 551 (1994).
  7. S. Liggins, Identification of point defects in treated single crystal diamond, Ph.D. thesis, University of Warwick, 2010.
  8. J. P. Goss and P. R. Briddon, Phys. Chem. Chem. Phys. 13, 11488 (2011).
  9. F. Fuchs, C. Wild, K. Schwarz, W. Müller-Sebert, and P. Koidl, Appl. Phys. Lett. 66, 177 (1995).
  10. See Supplemental Material at http://link.aps.org/supplemental/10.1103/mvdf-bdrx for further details about experimental methods, theoretical methods, and supplemental results, which includes Refs. [7,11–21].
  11. D. J. L. Coxon, M. Staniforth, B. G. Breeze, S. E. Greenough, J. P. Goss, M. Monti, J. Lloyd-Hughes, V. G. Stavros, and M. E. Newton, J. Phys. Chem. Lett. 11, 6677 (2020).
  12. T. J. Keat, D. J. L. Coxon, R. J. Cruddace, V. G. Stavros, M. E. Newton, and J. Lloyd-Hughes, Diamond Relat. Mater 141, 110661 (2024).
  13. P. Donaldson, G. Greetham, D. Shaw, A. Parker, and M. Towrie, J. Phys. Chem. A 122, 780 (2018).
  14. G. Petretto, S. Dwaraknath, H. P. C. Miranda, D. Winston, M. Giantomassi, M. J. van Setten, X. Gonze, K. A. Persson, G. Hautier, and G.-M. Rignanese, Sci. Data 5, 180065 (2018).
  15. A. Nitzan, S. Mukamel, and J. Jortner, J. Chem. Phys. 60, 3929 (1974).
  16. G. Davies, J. Phys. C 7, 3737 (1974).
  17. K. Mohammed, G. Davies, and A. T. Collins, J. Phys. C 15, 2779 (1982).
  18. J. P. Goss, B. J. Coomer, T. D. Shaw, P. R. Briddon, M. Rayson, and S. öberg, Phys. Rev. B 63, 195208 (2001).
  19. G. Davies, S. C. Lawson, A. T. Collins, A. Mainwood, and S. J. Sharp, Phys. Rev. B 46, 13157 (1992).
  20. M. N. Ashfold, J. P. Goss, B. L. Green, P. W. May, M. E. Newton, and C. V. Peaker, Chem. Rev. 120, 5745 (2020).
  21. M. P. Grubb, A. J. Orr-Ewing, and M. N. R. Ashfold, Rev. Sci. Instrum. 85, 064104 (2014).
  22. J. P. Goss, R. Jones, M. I. Heggie, C. P. Ewels, P. R. Briddon, and S. Öberg, Phys. Rev. B 65, 1156207 (2002).
  23. T. J. Keat, D. J. L. Coxon, M. Staniforth, M. W. Dale, V. G. Stavros, M. E. Newton, and J. Lloyd-Hughes, Phys. Rev. Lett. 129, 237401 (2022).
  24. J. L. Warren, J. L. Yarnell, G. Dolling, and R. A. Cowley, Phys. Rev. 158, 805 (1967).
  25. P. Pavone, K. Karch, O. Schiitt, W. Windl, D. Strauch, P. Giannozzi, and S. Baroni, Phys. Rev. B 48, 3156 (1993).
  26. B. Mortazavi, F. Shojaei, X. Zhuang, and L. F. C. Pereira, Carbon Trends 3, 100036 (2021).
  27. E. V. Lavrov, J. Weber, F. Börrnert, C. G. V. de Walle, and R. Helbig, Phys. Rev. B 66, 165205 (2002).
  28. K. Ishioka, M. Hase, M. Kitajima, and H. Petek, Appl. Phys. Lett. 89, 231916 (2006).
  29. K. C. Lee, B. J. Sussman, M. R. Sprague, P. Michelberger, K. F. Reim, J. Nunn, N. K. Langford, P. J. Bustard, D. Jaksch, and I. A. Walmsley, Nat. Photonics 6, 41 (2012).
  30. P. G. Klemens, Phys. Rev. 148, 845 (1966).
  31. K. Ishioka and O. V. Misochko, Coherent lattice oscillations in solids and their optical control part I. fundamentals and optical detection techniques, in Progress in Ultrafast Intense Laser Science, Vol. 5 (Springer, Berlin, Heidelberg, 2009), pp. 23–46.
  32. M. Zukerstein, M. Kozák, F. Trojánek, and P. Malý, Diamond Relat. Mater. 90, 202 (2018).
  33. P. Udvarhelyi, V. O. Shkolnikov, A. Gali, G. Burkard, and A. Pályi, Phys. Rev. B 98, 075201 (2018).
  34. P. Dhara and S. Guha, Phys. Rev. Res. 6, 013055 (2024).
  35. J. J. Nakane, K. Tahara, K. Kutsuki, and A. Yamakage, Phys. Rev. B 110, 064428 (2024).
  36. X. Cheng, A. Thurn, G. Chen, G. S. Jones, J. E. Bennett, M. Coke, M. Adshead, C. P. Michaels, O. Balci, A. C. Ferrari, M. Atatüre, R. J. Curry, J. M. Smith, P. S. Salter, and D. A. Gangloff, Nat. Commun. 16, 5124 (2025).
  37. Y. V. Gorelkinskii and N. N. Nevinnyi, Physica B (Amsterdam) 170, 155 (1991).
  38. Y. V. Gorelkinskii and N. N. Nevinnyi, Mater. Sci. Eng. B 36, 133 (1996).
  39. M. Budde, G. Lüpke, C. P. Cheney, N. H. Tolk, and L. C. Feldman, Phys. Rev. Lett. 85, 1452 (2000).
  40. M. Budde, G. Lüpke, E. Chen, X. Zhang, N. H. Tolk, L. C. Feldman, E. Tarhan, A. K. Ramdas, and M. Stavola, Phys. Rev. Lett. 87, 145501 (2001).
  41. G. Lüpke, N. H. Tolk, and L. C. Feldman, J. Appl. Phys. 93, 2317 (2003).
  42. R. N. Pereira, T. Ohya, K. M. Itoh, and B. B. Nielsen, Physica B (Amsterdam) 340–342, 697 (2003).
  43. T. M. Gibbons, S. K. Estreicher, K. Potter, F. Bekisli, and M. Stavola, Phys. Rev. B 87, 115207 (2013).
  44. R. Atta-Fynn, D. A. Drabold, S. R. Elliott, and P. Biswas, Phys. Rev. B 95, 104205 (2017).
  45. H. Li, Y. Guo, and J. Robertson, Sci. Rep. 7, 16858 (2017).
  46. L. Weston, D. Wickramaratne, M. Mackoit, A. Alkauskas, and C. G. Van De Walle, Phys. Rev. B 97, 214104 (2018).
  47. J. Neugebauer and C. G. Van De Walle, Phys. Rev. Lett. 75, 4452 (1995).
  48. C. G. Van De Walle and J. Neugebauer, Annu. Rev. Mater. Res. 36, 179 (2006).
  49. P. Briddon, R. Jones, and G. M. S. Lister, J. Phys. C 21, L1027 (1988).
  50. J. L. Lyons and C. G. Van De Walle, J. Phys. Condens. Matter 28, 06LT01 (2016).
  51. E. Holzschuh, W. Kündig, P. F. Meier, B. D. Patterson, J. P. F. Sellschop, M. C. Stemmet, and H. Appel, Phys. Rev. A 25, 1272 (1982).
  52. T. L. Estle, S. Estreicher, and D. S. Marynick, Phys. Rev. Lett. 58, 1547 (1987).
  53. J. P. Goss, J. Phys. Condens. Matter 15, R551 (2003).

Outline

Information

Sign In to Your Journals Account

Filter

Filter

Article Lookup

Enter a citation