Skip to main content

Thank you for visiting nature.com. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.

  • Letter
  • Published:

Molecular lattice clock with long vibrational coherence

Abstract

Atomic lattice clocks have spurred numerous ideas for tests of fundamental physics, detection of general relativistic effects and studies of interacting many-body systems. On the other hand, molecular structure and dynamics offer rich energy scales that are at the heart of new protocols in precision measurement and quantum information science. Here, we demonstrate a fundamentally distinct type of lattice clock that is based on vibrations in diatomic molecules, and present coherent Rabi oscillations between weakly and deeply bound molecules that persist for tens of milliseconds. This control is made possible by a state-insensitive magic lattice trap that weakly couples to molecular vibronic resonances and enhances the coherence time of light-induced clock state superpositions by several orders of magnitude. The achieved quality factor Q = 8 × 1011 results from 30 Hz narrow resonances for a 25 THz clock transition in Sr2 molecules. Our technique of extended coherent manipulation is applicable to long-term storage of quantum information in qubits based on ultracold polar molecules, while the vibrational clock enables precise probes of interatomic forces, tests of Newtonian gravitation at ultrashort range and model-independent searches for electron-to-proton mass ratio variations.

This is a preview of subscription content, access via your institution

Access options

Buy this article

Prices may be subject to local taxes which are calculated during checkout

Fig. 1: Vibrational molecular lattice clock.
Fig. 2: Magic lattice for the molecular clock.
Fig. 3: Coherent control of molecular clock states.
Fig. 4: Magic intensity ratio for a two-photon clock transition.

Similar content being viewed by others

Data availability

The data that support the plots within this paper and other findings of the study are available from the corresponding author upon reasonable request.

References

  1. Moses, S. A., Covey, J. P., Miecnikowski, M. T., Jin, D. S. & Ye, J. New frontiers for quantum gases of polar molecules. Nat. Phys. 13, 13–20 (2017).

    Article  Google Scholar 

  2. Barry, J. F., McCarron, D. J., Norrgard, E. B., Steinecker, M. H. & DeMille, D. Magneto-optical trapping of a diatomic molecule. Nature 512, 286–289 (2014).

    Article  ADS  Google Scholar 

  3. Cairncross, W. B. et al. Precision measurement of the electron’s electric dipole moment using trapped molecular ions. Phys. Rev. Lett. 119, 153001 (2017).

    Article  ADS  Google Scholar 

  4. Ospelkaus, S. et al. Quantum-state controlled chemical reactions of ultracold potassium–rubidium molecules. Science 327, 853–857 (2010).

    Article  ADS  Google Scholar 

  5. McDonald, M. et al. Photodissociation of ultracold diatomic strontium molecules with quantum state control. Nature 534, 122–126 (2016).

    Article  ADS  Google Scholar 

  6. Yan, B. et al. Observation of dipolar spin-exchange interactions with lattice-confined polar molecules. Nature 501, 521–525 (2013).

    Article  ADS  Google Scholar 

  7. Park, J. W., Yan, Z. Z., Loh, H., Will, S. A. & Zwierlein, M. W. Second-scale nuclear spin coherence time of ultracold 23Na40K molecules. Science 357, 372–375 (2017).

    Article  ADS  Google Scholar 

  8. Chou, C. et al. Preparation and coherent manipulation of pure quantum states of a single molecular ion. Nature 545, 203–207 (2017).

    Article  ADS  Google Scholar 

  9. Campbell, S. L. et al. A Fermi-degenerate three-dimensional optical lattice clock. Science 358, 90–94 (2017).

    Article  ADS  Google Scholar 

  10. McGrew, W. F. et al. Atomic clock performance enabling geodesy below the centimetre level. Nature 564, 87–90 (2018).

    Article  ADS  Google Scholar 

  11. Nemitz, N. et al. Frequency ratio of Yb and Sr clocks with 5 × 10−17 uncertainty at 150 seconds averaging time. Nat. Photon. 10, 258–261 (2016).

    Article  ADS  Google Scholar 

  12. Godun, R. M. et al. Frequency ratio of two optical clock transitions in 171Yb+ and constraints on the time variation of fundamental constants. Phys. Rev. Lett. 113, 210801 (2014).

    Article  ADS  Google Scholar 

  13. Huntemann, N. et al. Improved limit on a temporal variation of m p/m e from comparisons of Yb+ and Cs atomic clocks. Phys. Rev. Lett. 113, 210802 (2014).

    Article  ADS  Google Scholar 

  14. Chou, C. W., Hume, D. B., Rosenband, T. & Wineland, D. J. Optical clocks and relativity. Science 329, 1630–1633 (2010).

    Article  ADS  Google Scholar 

  15. Kolkowitz, S. et al. Gravitational wave detection with optical lattice atomic clocks. Phys. Rev. D 94, 124043 (2016).

    Article  ADS  Google Scholar 

  16. Kolkowitz, S. et al. Spin–orbit-coupled fermions in an optical lattice clock. Nature 542, 66–70 (2017).

    Article  ADS  Google Scholar 

  17. Borkowski, M. Optical lattice clocks with weakly bound molecules. Phys. Rev. Lett. 120, 083202 (2018).

    Article  ADS  Google Scholar 

  18. Zelevinsky, T., Kotochigova, S. & Ye, J. Precision test of mass-ratio variations with lattice-confined ultracold molecules. Phys. Rev. Lett. 100, 043201 (2008).

    Article  ADS  Google Scholar 

  19. Schiller, S., Bakalov, D. & Korobov, V. I. Simplest molecules as candidates for precise optical clocks. Phys. Rev. Lett. 113, 023004 (2014).

    Article  ADS  Google Scholar 

  20. Hanneke, D., Carollo, R. A. & Lane, D. A. High sensitivity to variation in the proton-to-electron mass ratio in \({\mathrm{O}}_{2}^{+}\). Phys. Rev. A 94, 050101(R) (2016).

    Article  ADS  Google Scholar 

  21. Salumbides, E. J. et al. Bounds on fifth forces from precision measurements on molecules. Phys. Rev. D 87, 112008 (2013).

    Article  ADS  Google Scholar 

  22. Salumbides, E. J., Dickenson, G. D., Ivanov, T. I. & Ubachs, W. QED effects in molecules: test of rotational quantum states of H2. Phys. Rev. Lett. 107, 043005 (2011).

    Article  ADS  Google Scholar 

  23. Ye, J., Kimble, H. J. & Katori, H. Quantum state engineering and precision metrology using state-insensitive light traps. Science 320, 1734–1738 (2008).

    Article  ADS  Google Scholar 

  24. McGuyer, B. H. et al. Precise study of asymptotic physics with subradiant ultracold molecules. Nat. Phys. 11, 32–36 (2015).

    Article  Google Scholar 

  25. Kotochigova, S. & DeMille, D. Electric-field-dependent dynamic polarizability and state-insensitive conditions for optical trapping of diatomic polar molecules. Phys. Rev. A 82, 063421 (2010).

    Article  ADS  Google Scholar 

  26. Neyenhuis, B. et al. Anisotropic polarizability of ultracold polar 40K87Rb molecules. Phys. Rev. Lett. 109, 230403 (2012).

    Article  ADS  Google Scholar 

  27. Li, M., Petrov, A., Makrides, C., Tiesinga, E. & Kotochigova, S. Pendular trapping conditions for ultracold polar molecules enforced by external electric fields. Phys. Rev. A 95, 063422 (2017).

    Article  ADS  Google Scholar 

  28. Rosenband, T., Grimes, D. G. & Ni, K.-K. Elliptical polarization for molecular stark shift compensation in deep optical traps. Opt. Express 26, 19821–19825 (2018).

    Article  ADS  Google Scholar 

  29. Kajita, M., Gopakumar, G., Abe, M. & Hada, M. Elimination of the Stark shift from the vibrational transition frequency of optically trapped 174Yb6Li molecules. Phys. Rev. A 84, 022507 (2011).

    Article  ADS  Google Scholar 

  30. Skomorowski, W., Pawłowski, F., Koch, C. P. & Moszynski, R. Rovibrational dynamics of the strontium molecule in the \({\mathrm{A}}^1\mathop {\sum}\nolimits_{u}^{+}\), \({\mathrm{c}}^3\mathop {\Pi}\nolimits_{\mathrm{u}}\) and \({\mathrm{A}}^1\mathop {\sum}\nolimits_{u}^{+}\) manifold from state-of-the-art ab initio calculations. J. Chem. Phys. 136, 194306 (2012).

    Article  ADS  Google Scholar 

  31. Reinaudi, G., Osborn, C. B., McDonald, M., Kotochigova, S. & Zelevinsky, T. Optical production of stable ultracold 88Sr2 molecules. Phys. Rev. Lett. 109, 115303 (2012).

    Article  ADS  Google Scholar 

  32. McDonald, M., McGuyer, B. H., Iwata, G. Z. & Zelevinsky, T. Thermometry via light shifts in optical lattices. Phys. Rev. Lett. 114, 023001 (2015).

    Article  ADS  Google Scholar 

  33. McGuyer, B. H. et al. High-precision spectroscopy of ultracold molecules in an optical lattice. New J. Phys. 17, 055004 (2015).

    Article  ADS  Google Scholar 

  34. Sobelman, I. I Atomic Spectra and Radiative Transitions (Springer, 1979).

  35. Craig, D. P. & Thirunamachandran, T. Molecular Quantum Electrodynamics (Academic Press, 1984).

Download references

Acknowledgements

We acknowledge support from NSF grant no. PHY-1349725 and ONR grant no. N00014-17-1-2246, as well as Polish National Science Center grant no. 2016/20/W/ST4/00314.

Author information

Authors and Affiliations

Authors

Contributions

S.S.K., C.-H.L., K.H.L., C.L. and T.Z. designed and performed the experiments and interpreted the data. I.M. and R.M. carried out the theoretical analysis.

Corresponding author

Correspondence to T. Zelevinsky.

Ethics declarations

Competing interests

The authors declare no competing interests.

Additional information

Peer review information: Nature Physics thanks David Leibrandt, Nicola Poli and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

Publisher’s note: Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Supplementary information

Supplementary Information

Supplementary Figs. 1–3.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Kondov, S.S., Lee, CH., Leung, K.H. et al. Molecular lattice clock with long vibrational coherence. Nat. Phys. 15, 1118–1122 (2019). https://doi.org/10.1038/s41567-019-0632-3

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/s41567-019-0632-3

This article is cited by

Search

Quick links

Nature Briefing

Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.

Get the most important science stories of the day, free in your inbox. Sign up for Nature Briefing