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
  • Open Access

Observation of Resonant Monopole-Dipole Energy Transfer between Rydberg Atoms and Polar Molecules

J. Zou1, R. R. W. Wang2,3,*, R. González-Férez4, H. R. Sadeghpour2, and S. D. Hogan1,†

  • *Contact author: reuben.wang@cfa.harvard.edu
  • †Contact author: s.hogan@ucl.ac.uk

Phys. Rev. Lett. 136, 113402 – Published 20 March, 2026

DOI: https://doi.org/10.1103/k9d5-1jcc

Abstract

Resonant energy transfer (RET) between the equal parity 1s65s S13 and 1s66s S13 Rydberg levels in helium has been observed in low-temperature (∼80  mK) collisions with ammonia molecules that undergo inversion transitions in their X A11 ground electronic state. This hybrid Rydberg-atom–polar-molecule resonant energy transfer represents a monopole-dipole energy exchange reaction that necessarily requires spatial overlap of the Rydberg-electron and molecular wave functions. Calculations that account explicitly for the charge-dipole interaction between the Rydberg electron and the molecule provide a quantitative explanation of the observations. Total parity is conserved in the reaction through the mixing of collisional angular momentum in the atom-molecule complex. This work opens opportunities to expand the toolbox for quantum science with charge-dipole-mediated energy exchange in hybrid atom–polar-molecule platforms.

View figure in article

Physics Subject Headings (PhySH)

Article Text

Supplemental Material

References (68)

  1. G. A. Jones and D. S. Bradshaw, Resonance energy transfer: From fundamental theory to recent applications, Front. Phys. 7, 100 (2019).
  2. T. Forster, Energiewanderung und Fluoreszenz, Naturwissenschaften 33, 166 (1946).
  3. G. Cario and J. Franck, Über Zerlegung von Wasserstoffmolekülen durch angeregte Quecksilberatome, Z. Phys. 11, 161 (1922).
  4. M. Şener, J. Strümpfer, J. Hsin, D. Chandler, S. Scheuring, C. N. Hunter, and K. Schulten, Förster energy transfer theory as reflected in the structures of photosynthetic light-harvesting systems, Chem. Phys. Chem. 12, 518 (2011).
  5. T. Mirkovic, E. E. Ostroumov, J. M. Anna, R. van Grondelle, Govindjee, and G. D. Scholes, Light absorption and energy transfer in the antenna complexes of photosynthetic organisms, Chem. Rev. 117, 249 (2017).
  6. T. Ha, J. Fei, S. Schmid, N. K. Lee, R. L. Gonzalez, S. Paul, and S. Yeou, Fluorescence resonance energy transfer at the single-molecule level, Nat. Rev. Methods Primers 4, 21 (2024).
  7. J.-R. Li, W. G. Tobias, K. Matsuda, C. Miller, G. Valtolina, L. De Marco, R. R. W. Wang, L. Lassablière, G. Quéméner, J. L. Bohn, and J. Ye, Tuning of dipolar interactions and evaporative cooling in a three-dimensional molecular quantum gas, Nat. Phys. 17, 1144 (2021).
  8. L. Lassablière and G. Quéméner, Model for two-body collisions between ultracold dipolar molecules around a Förster resonance in an electric field, Phys. Rev. A 106, 033311 (2022).
  9. A. N. Carroll, H. Hirzler, C. Miller, D. Wellnitz, S. R. Muleady, J. Lin, K. P. Zamarski, R. R. W. Wang, J. L. Bohn, A. M. Rey, and J. Ye, Observation of generalized t−J spin dynamics with tunable dipolar interactions, Science 388, 381 (2025).
  10. A. Guttridge, D. K. Ruttley, A. C. Baldock, R. González-Férez, H. R. Sadeghpour, C. S. Adams, and S. L. Cornish, Observation of Rydberg blockade due to the charge-dipole interaction between an atom and a polar molecule, Phys. Rev. Lett. 131, 013401 (2023).
  11. L. R. B. Picard, A. J. Park, G. E. Patenotte, S. Gebretsadkan, D. Wellnitz, A. M. Rey, and K.-K. Ni, Entanglement and iSWAP gate between molecular qubits, Nature (London) 637, 821 (2025).
  12. J. Perrin, Fluorescence et induction moléculaire par résonance, C. R. Hebd. Séances Acad. Sci. 184, 1097 (1927).
  13. H. Kallmann and F. London, Über quantenmechanische Energieübertragung zwischen atomaren Systemen, Z. Phys. Chem. 2B, 207 (1929).
  14. F. Perrin, Théorie quantique des transferts d’activation entre molécules de même espèce. Cas des solutions fluorescentes, Ann. Phys. (N.Y.) 10, 283 (1932).
  15. C. S. E. van Ditzhuijzen, A. F. Koenderink, J. V. Hernández, F. Robicheaux, L. D. Noordam, and H. B. van Linden van den Heuvell, Spatially resolved observation of dipole-dipole interaction between Rydberg atoms, Phys. Rev. Lett. 100, 243201 (2008).
  16. S. Ravets, H. Labuhn, D. Barredo, L. Béguin, T. Lahaye, and A. Browaeys, Coherent dipole–dipole coupling between two single Rydberg atoms at an electrically-tuned Förster resonance, Nat. Phys. 10, 914 (2014).
  17. S. de Léséleuc, D. Barredo, V. Lienhard, A. Browaeys, and T. Lahaye, Optical control of the resonant dipole-dipole interaction between Rydberg atoms, Phys. Rev. Lett. 119, 053202 (2017).
  18. V. Zhelyazkova and S. D. Hogan, Electrically tuned Förster resonances in collisions of NH3 with Rydberg He atoms, Phys. Rev. A 95, 042710 (2017).
  19. F. Jarisch and M. Zeppenfeld, State resolved investigation of Förster resonant energy transfer in collisions between polar molecules and Rydberg atoms, New J. Phys. 20, 113044 (2018).
  20. J. Zou and S. D. Hogan, Probing van der Waals interactions and detecting polar molecules by Förster-resonance energy transfer with Rydberg atoms at temperatures below 100 mK, Phys. Rev. A 106, 043111 (2022).
  21. S. Patsch, M. Zeppenfeld, and C. P. Koch, Rydberg atom-enabled spectroscopy of polar molecules via Förster resonance energy transfer, J. Phys. Chem. Lett. 13, 10728 (2022).
  22. L. Zhu, J. Luke, R. Shaham, Y.-X. Liu, and K.-K. Ni, Probing dipolar interactions between Rydberg atoms and ultracold polar molecules, Phys. Rev. Lett. 135, 153001 (2025).
  23. B. Yan, S. A. Moses, B. Gadway, J. P. Covey, K. R. A. Hazzard, A. M. Rey, D. S. Jin, and J. Ye, Observation of dipolar spin-exchange interactions with lattice-confined polar molecules, Nature (London) 501, 521 (2013).
  24. L. Christakis, J. S. Rosenberg, R. Raj, S. Chi, A. Morningstar, D. A. Huse, Z. Z. Yan, and W. S. Bakr, Probing site-resolved correlations in a spin system of ultracold molecules, Nature (London) 614, 64 (2023).
  25. T. F. Gallagher, G. A. Ruff, and K. A. Safinya, Resonant electronic to vibrational energy transfer from Na to CH4 and CD4, Phys. Rev. A 22, 843 (1980).
  26. J. Deiglmayr, H. Saßmannshausen, P. Pillet, and F. Merkt, Observation of dipole-quadrupole interaction in an ultracold gas of Rydberg atoms, Phys. Rev. Lett. 113, 193001 (2014).
  27. W. Maineult, B. Pelle, R. Faoro, E. Arimondo, P. Pillet, and P. Cheinet, Dipole–quadrupole Förster resonance in cesium Rydberg gas, J. Phys. B 49, 214001 (2016).
  28. K. Wang, C. P. Williams, L. R. B. Picard, N. Y. Yao, and K.-K. Ni, Enriching the quantum toolbox of ultracold molecules with Rydberg atoms, PRX Quantum 3, 030339 (2022).
  29. C. Zhang and M. R. Tarbutt, Quantum computation in a hybrid array of molecules and Rydberg atoms, PRX Quantum 3, 030340 (2022).
  30. E. L. Church and J. Weneser, Electric-monopole transitions in atomic nuclei, Phys. Rev. 103, 1035 (1956).
  31. S. Zerguine, P. Van Isacker, A. Bouldjedri, and S. Heinze, Correlating radii and electric monopole transitions of atomic nuclei, Phys. Rev. Lett. 101, 022502 (2008).
  32. E. Kuznetsova, S. T. Rittenhouse, H. R. Sadeghpour, and S. F. Yelin, Rydberg-atom-mediated nondestructive readout of collective rotational states in polar-molecule arrays, Phys. Rev. A 94, 032325 (2016).
  33. S. T. Rittenhouse and H. R. Sadeghpour, Ultracold giant polyatomic Rydberg molecules: Coherent control of molecular orientation, Phys. Rev. Lett. 104, 243002 (2010).
  34. M. Schlagmüller, T. C. Liebisch, F. Engel, K. S. Kleinbach, F. Böttcher, U. Hermann, K. M. Westphal, A. Gaj, R. Löw, S. Hofferberth, T. Pfau, J. Pérez-Ríos, and C. H. Greene, Ultracold chemical reactions of a single Rydberg atom in a dense gas, Phys. Rev. X 6, 031020 (2016).
  35. P. Geppert, M. Althön, D. Fichtner, and H. Ott, Diffusive-like redistribution in state-changing collisions between Rydberg atoms and ground state atoms, Nat. Commun. 12, 3900 (2021).
  36. V. Zhelyazkova, F. B. V. Martins, J. A. Agner, H. Schmutz, and F. Merkt, Multipole-moment effects in ion–molecule reactions at low temperatures: Part I—ion-dipole enhancement of the rate coefficients of the He++NH3 and He++ND3 reactions at collisional energies Ecoll/kB near 0 K, Phys. Chem. Chem. Phys. 23, 21606 (2021).
  37. K. Gawlas and S. D. Hogan, Rydberg-state-resolved resonant energy transfer in cold electric-field-controlled intrabeam collisions of NH3 with Rydberg He atoms, J. Phys. Chem. Lett. 11, 83 (2020).
  38. T. Halfmann, J. Koensgen, and K. Bergmann, A source for a high-intensity pulsed beam of metastable helium atoms, Meas. Sci. Technol. 11, 1510 (2000).
  39. S. D. Hogan, Y. Houston, and B. Wei, Laser photoexcitation of Rydberg states in helium with n>400, J. Phys. B 51, 145002 (2018).
  40. K. A. Smith, F. G. Kellert, R. D. Rundel, F. B. Dunning, and R. F. Stebbings, Discrete energy transfer in collisions of Xe(nf) Rydberg atoms with NH3 molecules, Phys. Rev. Lett. 40, 1362 (1978).
  41. J. W. Simmons and W. Gordy, Structure of the inversion spectrum of ammonia, Phys. Rev. 73, 713 (1948).
  42. See Supplemental Material at http://link.aps.org/supplemental/10.1103/k9d5-1jcc for collision theory of charge-dipole mediated RET, which includes Refs. [43–48].
  43. E. Fermi and E. Teller, The capture of negative mesotrons in matter, Phys. Rev. 72, 399 (1947).
  44. G. W. F. Drake, High precision theory of atomic helium, Phys. Scr. 1999, 83 (1999).
  45. S. Green, Energy transfer in NH3-He collisions, J. Chem. Phys. 73, 2740 (1980).
  46. A. P. Hickman, Theory of angular momentum mixing in Rydberg-atom-rare-gas collisions, Phys. Rev. A 18, 1339 (1978).
  47. A. P. Hickman, Relation between low-energy-electron scattering and ℓ-changing collisions of Rydberg atoms, Phys. Rev. A 19, 994 (1979).
  48. A. Tsikritea, J. A. Diprose, T. P. Softley, and B. R. Heazlewood, Capture theory models: An overview of their development, experimental verification, and applications to ion–molecule reactions, J. Chem. Phys. 157, 060901 (2022).
  49. M. Matsuzawa, State-changing collision of a high-Rydberg atom with a polar molecule, Phys. Rev. A 20, 860 (1979).
  50. K. Aikawa, A. Frisch, M. Mark, S. Baier, R. Grimm, J. L. Bohn, D. S. Jin, G. M. Bruun, and F. Ferlaino, Anisotropic relaxation dynamics in a dipolar Fermi gas driven out of equilibrium, Phys. Rev. Lett. 113, 263201 (2014).
  51. R. R. W. Wang and J. L. Bohn, Anisotropic thermalization of dilute dipolar gases, Phys. Rev. A 103, 063320 (2021).
  52. J. Mizrahi, C. Senko, B. Neyenhuis, K. G. Johnson, W. C. Campbell, C. W. S. Conover, and C. Monroe, Ultrafast spin-motion entanglement and interferometry with a single atom, Phys. Rev. Lett. 110, 203001 (2013).
  53. A. Dareau, Y. Meng, P. Schneeweiss, and A. Rauschenbeutel, Observation of ultrastrong spin-motion coupling for cold atoms in optical microtraps, Phys. Rev. Lett. 121, 253603 (2018).
  54. V. Bharti, S. Sugawa, M. Kunimi, V. S. Chauhan, T. P. Mahesh, M. Mizoguchi, T. Matsubara, T. Tomita, S. de Léséleuc, and K. Ohmori, Strong spin-motion coupling in the ultrafast dynamics of Rydberg atoms, Phys. Rev. Lett. 133, 093405 (2024).
  55. R. R. W. Wang and J. L. Bohn, Theory of itinerant collisional spin dynamics in nondegenerate molecular gases, Phys. Rev. A 112, 043315 (2025).
  56. R. González-Férez, H. R. Sadeghpour, and P. Schmelcher, Rotational hybridization, and control of alignment and orientation in triatomic ultralong-range Rydberg molecules, New J. Phys. 17, 013021 (2015).
  57. V. Bendkowsky, B. Butscher, J. Nipper, J. P. Shaffer, R. Löw, and T. Pfau, Observation of ultralong-range Rydberg molecules, Nature (London) 458, 1005 (2009).
  58. L. Anderegg, L. W. Cheuk, Y. Bao, S. Burchesky, W. Ketterle, K.-K. Ni, and J. M. Doyle, An optical tweezer array of ultracold molecules, Science 365, 1156 (2019).
  59. L. Anderegg, S. Burchesky, Y. Bao, S. S. Yu, T. Karman, E. Chae, K.-K. Ni, W. Ketterle, and J. M. Doyle, Observation of microwave shielding of ultracold molecules, Science 373, 779 (2021).
  60. D. Bluvstein, H. Levine, G. Semeghini, T. T. Wang, S. Ebadi, M. Kalinowski, A. Keesling, N. Maskara, H. Pichler, M. Greiner, V. Vuletić, and M. D. Lukin, A quantum processor based on coherent transport of entangled atom arrays, Nature (London) 604, 451 (2022).
  61. D. K. Ruttley, A. Guttridge, S. Spence, R. C. Bird, C. R. Le Sueur, J. M. Hutson, and S. L. Cornish, Formation of ultracold molecules by merging optical tweezers, Phys. Rev. Lett. 130, 223401 (2023).
  62. D. K. Ruttley, A. Guttridge, T. R. Hepworth, and S. L. Cornish, Enhanced quantum control of individual ultracold molecules using optical tweezer arrays, PRX Quantum 5, 020333 (2024).
  63. D. K. Ruttley, T. R. Hepworth, A. Guttridge, and S. L. Cornish, Long-lived entanglement of molecules in magic-wavelength optical tweezers, Nature (London) 637, 827 (2025).
  64. A. Guttridge, T. R. Hepworth, D. K. Ruttley, A. A. T. Durst, M. T. Eiles, and S. L. Cornish, Individual assembly of two-species Rydberg molecules using optical tweezers, Phys. Rev. Lett. 134, 133401 (2025).
  65. D. Jaksch, J. I. Cirac, P. Zoller, S. L. Rolston, R. Côté, and M. D. Lukin, Fast quantum gates for neutral atoms, Phys. Rev. Lett. 85, 2208 (2000).
  66. M. D. Lukin, M. Fleischhauer, R. Cote, L. M. Duan, D. Jaksch, J. I. Cirac, and P. Zoller, Dipole blockade and quantum information processing in mesoscopic atomic ensembles, Phys. Rev. Lett. 87, 037901 (2001).
  67. C. Ates, T. Pohl, T. Pattard, and J. M. Rost, Antiblockade in Rydberg excitation of an ultracold lattice gas, Phys. Rev. Lett. 98, 023002 (2007).
  68. T. Amthor, C. Giese, C. S. Hofmann, and M. Weidemüller, Evidence of antiblockade in an ultracold Rydberg gas, Phys. Rev. Lett. 104, 013001 (2010).

Outline

Information

Sign In to Your Journals Account

Filter

Filter

Article Lookup

Enter a citation