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Observation of Spin-Singlet Butterfly Rydberg Molecules in an Ultracold Atomic Rb Gas

Markus Exner1, Rohan Srikumar2, Richard Blättner1, Peter Schmelcher2,3, H. R. Sadeghpour4, Matthew T. Eiles5,6, and Herwig Ott1,*

  • *Contact author: ott@physik.uni-kl.de

Phys. Rev. Lett. 136, 243002 – Published 18 June, 2026

DOI: https://doi.org/10.1103/q5r1-whjr

Abstract

We report the observation of spin-singlet ultralong-range Rydberg butterfly molecules consisting of a ground-state atom bound to a Rydberg atom by P-wave scattering of Rb87 Rydberg electrons from Rb87(5  s) atoms. A three-photon excitation scheme enables the photoassociation of these molecules by weakly admixing Rb(18f7/2) states. The measured binding energies, kilo-Debye permanent electric dipole moments, and lifetimes are in excellent agreement with theory. Two long-lived vibrational levels, red detuned from the Rb(18f7/2) threshold, are observed. This experiment is a foundational step in the production of ultracold anions and heavy Rydberg ion-pair systems.

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References (52)

  1. J. P. Shaffer, S. T. Rittenhouse, and H. R. Sadeghpour, Nat. Commun. 9, 1965 (2018).
  2. M. T. Eiles, J. Phys. B 52, 113001 (2019).
  3. C. Fey, F. Hummel, and P. Schmelcher, Mol. Phys. 118, e1679401 (2020).
  4. F. B. Dunning, S. K. Kanungo, and S. Yoshida, J. Phys. B 57, 212002 (2024).
  5. V. Bendkowsky, B. Butscher, J. Nipper, J. P. Shaffer, R. Löw, and T. Pfau, Nature (London) 458, 1005 (2009).
  6. B. J. DeSalvo, J. A. Aman, F. B. Dunning, T. C. Killian, H. R. Sadeghpour, S. Yoshida, and J. Burgdörfer, Phys. Rev. A 92, 031403(R) (2015).
  7. M. Peper and J. Deiglmayr, Phys. Rev. Lett. 126, 013001 (2021).
  8. C. H. Greene, A. S. Dickinson, and H. R. Sadeghpour, Phys. Rev. Lett. 85, 2458 (2000).
  9. E. L. Hamilton, C. H. Greene, and H. R. Sadeghpour, J. Phys. B 35, L199 (2002).
  10. A. A. Khuskivadze, M. I. Chibisov, and I. I. Fabrikant, Phys. Rev. A 66, 042709 (2002).
  11. P. Giannakeas, M. T. Eiles, F. Robicheaux, and J. M. Rost, Phys. Rev. Lett. 125, 123401 (2020).
  12. W. Li, T. Pohl, J. M. Rost, S. T. Rittenhouse, H. R. Sadeghpour, J. Nipper, B. Butscher, J. B. Balewski, V. Bendkowsky, R. Löw, and T. Pfau, Science 334, 1110 (2011).
  13. D. Booth, S. T. Rittenhouse, J. Yang, H. R. Sadeghpour, and J. P. Shaffer, Science 348, 99 (2015).
  14. T. Niederprüm, O. Thomas, T. Eichert, C. Lippe, J. Pérez-Ríos, C. H. Greene, and H. Ott, Nat. Commun. 7, 12820 (2016).
  15. M. Althön, M. Exner, R. Blättner, and H. Ott, Nat. Commun. 14, 8108 (2023).
  16. M. Exner, R. Srikumar, R. Blättner, M. T. Eiles, P. Schmelcher, and H. Ott, Phys. Rev. Lett. 134, 223401 (2025).
  17. H. Saßmannshausen, F. Merkt, and J. Deiglmayr, Phys. Rev. Lett. 114, 133201 (2015).
  18. K. S. Kleinbach, F. Meinert, F. Engel, W. J. Kwon, R. Löw, T. Pfau, and G. Raithel, Phys. Rev. Lett. 118, 223001 (2017).
  19. F. Böttcher, A. Gaj, K. M. Westphal, M. Schlagmüller, K. S. Kleinbach, R. Löw, T. C. Liebisch, T. Pfau, and S. Hofferberth, Phys. Rev. A 93, 032512 (2016).
  20. T. Killian, T. Pattard, T. Pohl, and J. M. Rost, Phys. Rep. 449, 77 (2007).
  21. T. C. Killian, S. Kulin, S. D. Bergeson, L. A. Orozco, C. Orzel, and S. L. Rolston, Phys. Rev. Lett. 83, 4776 (1999).
  22. B. B. Zelener, E. V. Vilshanskaya, N. V. Morozov, S. A. Saakyan, A. A. Bobrov, V. A. Sautenkov, and B. V. Zelener, Phys. Rev. Lett. 132, 115301 (2024).
  23. R. S. Fletcher, X. L. Zhang, and S. L. Rolston, Phys. Rev. Lett. 96, 105003 (2006).
  24. W. Li, M. W. Noel, M. P. Robinson, P. J. Tanner, T. F. Gallagher, D. Comparat, B. Laburthe Tolra, N. Vanhaecke, T. Vogt, N. Zahzam, P. Pillet, and D. A. Tate, Phys. Rev. A 70, 042713 (2004).
  25. M. P. Robinson, B. Laburthe Tolra, M. W. Noel, T. F. Gallagher, and P. Pillet, Phys. Rev. Lett. 85, 4466 (2000).
  26. W. Li, P. J. Tanner, and T. F. Gallagher, Phys. Rev. Lett. 94, 173001 (2005).
  27. T. Pohl, T. Pattard, and J. M. Rost, Phys. Rev. Lett. 92, 155003 (2004).
  28. W. Oohara and R. Hatakeyama, Phys. Rev. Lett. 91, 205005 (2003).
  29. W. Oohara, R. Hatakeyama, and S. Ishiguro, Phys. Rev. E 68, 066407 (2003).
  30. N. Sato, T. Mieno, T. Hirata, Y. Yagi, R. Hatakeyama, and S. Iizuka, Phys. Plasmas 1, 3480 (1994).
  31. T. Pohl, D. Vrinceanu, and H. R. Sadeghpour, Phys. Rev. Lett. 100, 223201 (2008).
  32. A. Kirrander, S. Rittenhouse, M. Ascoli, E. E. Eyler, P. L. Gould, and H. R. Sadeghpour, Phys. Rev. A 87, 031402(R) (2013).
  33. S. Markson and H. R. Sadeghpour, J. Phys. B 49, 114006 (2016).
  34. F. Hummel, P. Schmelcher, H. Ott, and H. R. Sadeghpour, New J. Phys. 22, 063060 (2020).
  35. C. W. Walter, N. D. Gibson, D. J. Matyas, C. Crocker, K. A. Dungan, B. R. Matola, and J. Rohlén, Phys. Rev. Lett. 113, 063001 (2014).
  36. R. Tang, R. Si, Z. Fei, X. Fu, Y. Lu, T. Brage, H. Liu, C. Chen, and C. Ning, Phys. Rev. Lett. 123, 203002 (2019).
  37. M. T. Eiles and C. H. Greene, Phys. Rev. A 95, 042515 (2017).
  38. C. H. Greene and M. T. Eiles, Phys. Rev. A 108, 042805 (2023).
  39. See Supplemental Material A and B at http://link.aps.org/supplemental/10.1103/q5r1-whjr for a detailed explanation of the singlet spin admixture in molecular states, which includes Ref. [37]; for a detailed explanation of the signal profile calculation, which includes Refs. [5,40–43]; for an estimation of the radiative lifetime of these high-ℓ molecules.
  40. F. Engel, T. Dieterle, F. Hummel, C. Fey, P. Schmelcher, R. Löw, T. Pfau, and F. Meinert, Phys. Rev. Lett. 123, 073003 (2019).
  41. M. Peper, M. Trautmann, and J. Deiglmayr, Phys. Rev. A 107, 012812 (2023).
  42. J. Tallant, S. T. Rittenhouse, D. Booth, H. R. Sadeghpour, and J. P. Shaffer, Phys. Rev. Lett. 109, 173202 (2012).
  43. G. Breit and E. Wigner, Phys. Rev. 49, 519 (1936).
  44. M. Deiß, S. Haze, J. Wolf, L. Wang, F. Meinert, C. Fey, F. Hummel, P. Schmelcher, and J. Hecker Denschlag, Phys. Rev. Res. 2, 013047 (2020).
  45. H. Rivera-Rodríguez and R. Jáuregui, Phys. Rev. Res. 6, 013173 (2024).
  46. A. S. Coolidge, H. M. James, and R. D. Present, J. Chem. Phys. 4, 193 (1936).
  47. E. U. Condon, The Franck-Condon principle and related topics, in Selected Scientific Papers of E.U. Condon, edited by A. O. Barut, H. Odabasi, and A. van der Merwe (Springer, New York, 1991), pp. 515–529.
  48. R. Srikumar, M. Exner, R. Blättner, P. Schmelcher, M. T. Eiles, and H. Ott, Phys. Rev. Res. 7, 043103 (2025).
  49. M. T. Eiles and F. Hummel, Phys. Rev. A 109, 022811 (2024).
  50. M. T. Eiles, Phys. Rev. A 98, 042706 (2018).
  51. M. I. Chibisov, A. A. Khuskivadze, and I. I. Fabrikant, J. Phys. B 35, L193 (2002).
  52. M. S. Murillo, Phys. Plasmas 11, 2964 (2004).

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