Abstract
In the field of cold quantum matter, control of the motional degrees of freedom of both neutral and charged gas-phase molecules has been achieved for a wide range of species1,2,3,4,5,6,7,8,9,10,11. However, cooling of the internal degrees of freedom remains challenging. Recently, transfer to the internal ground state by sophisticated optical techniques has been demonstrated for neutral alkali dimers created in single quantum states from ultracold atoms12,13,14,15. Here we demonstrate cooling of the rotational degree of freedom of heteronuclear diatomic molecules with a thermal distribution of internal states, using a simple, robust and general optical-pumping scheme with two low-power continuous-wave lasers. With trapped and translationally cooled hydrogen deuteride (HD+) molecular ions as a model system, we achieve 78(4)% rovibrational ground-state population. The rotationally, vibrationally and translationally cold molecular ion ensemble is suitable for a number of applications, such as generation of long-lived coherences or frequency metrology of fundamental constants16,17.
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References
Bethlem, H. L. & Meijer, G. Production and application of translationally cold molecules. Int. Rev. Phys. Chem. 22, 73–128 (2003).
Rieger, T., Junglen, T., Rangwala, S. A., Pinkse, P. W. H. & Rempe, G. Continuous loading of an electrostatic trap for polar molecules. Phys. Rev. Lett. 173002 (2005).
Campbell, W. C. & Doyle, J. M. in Cold Molecules (eds Krems, R. V., Stwalley, W. C. & Friedrich, B.) 473–508 (CRC Press, 2009).
Fioretti, A. et al. Formation of cold Cs2 molecules through photoassociation. Phys. Rev. Lett. 80, 4402–4405 (1998).
Hodby, E. et al. Production efficiency of ultracold Feshbach molecules in bosonic and fermionic systems. Phys. Rev. Lett. 94, 120402 (2005).
Jochim, S. et al. Bose–Einstein condensation of molecules. Science 302, 2101–2103 (2003).
Regal, C. A., Ticknor, C., Bohn, J. L. & Jin, D. S. Creation of ultracold molecules from a Fermi gas of atoms. Nature 424, 47–50 (2003).
Weinstein, J. D., deCarvalho, R., Guilett, T., Friedrich, B. & Doyle, J. D. Magnetic trapping of calcium monohydride molecules at millikelvin temperatures. Nature 395, 148–150 (1998).
Mølhave, K. & Drewsen, M. Formation of translationally cold MgH+ and MgD+ molecules in an ion trap. Phys. Rev. A 62, 011401(R).
Roth, B., Koelemeij, J. C. J., Daerr, H. & Schiller, S. Rovibrational spectroscopy of trapped molecular hydrogen ions at millikelvin temperatures. Phys. Rev. A 74, 040501(R) (2006).
Offenberg, D., Zhang, C. B., Wellers, Ch., Roth, B. & Schiller, S. Translational cooling and storage of protonated proteins in an ion trap at subkelvin temperatures. Phys. Rev. A 78, 061401(R) (2008).
Danzl, J. G. et al. Quantum gas of deeply bound ground state molecules. Science 321, 1062–1066 (2008).
Deiglmayr, J. et al. Formation of ultracold polar molecules in the rovibrational ground state. Phys. Rev. Lett. 101, 133004 (2008).
Lang, F., Winkler, K., Strauss, C., Grimm, R. & Denschlag, J. H. Ultracold triplet molecules in the rovibrational ground state. Phys. Rev. Lett. 101, 133005 (2008).
Ni, K.-K. et al. A high phase-space-density gas of polar molecules. Science 322, 231–235 (2009).
Schiller, S. & Korobov, V. Tests of time independence of the electron and nuclear masses with ultracold molecules. Phys. Rev. A 71, 032505 (2005).
Koelemeij, J. C. J., Roth, B., Wicht, A., Ernsting, I. & Schiller, S. Vibrational spectroscopy of HD+ with 2-ppb accuracy. Phys. Rev. Lett. 98, 173002 (2007).
Krems, R. V., Stwalley, W. C. & Friedrich, B. (eds) in Cold Molecules (CRC Press, 2009).
Morigi, G., Pinkse, P. W. H., Kowalewski, M. & de Vivie-Riedle, R. Cavity cooling of internal molecular motion. Phys. Rev. Lett. 99, 073001 (2007).
Hudson, E. R. Method for producing ultracold molecular ions. Phys. Rev. A 79, 032716 (2009).
Vogelius, I. S., Madsen, L. B. & Drewsen, M. Blackbody-radiation-assisted laser cooling of molecular ions. Phys. Rev. Lett. 89, 173003 (2002).
Højbjerre, K., Hansen, A. K., Skyt, P. S., Staanum, P. F. & Drewsen, M. Rotational state resolved photodissociation spectroscopy of translationally and vibrationally cold MgH+ ions: Toward rotational cooling of molecular ions. New J. Phys. 11, 055026 (2009).
Koelemeij, J. C. J., Roth, B. & Schiller, S. Blackbody thermometry with cold molecular ions and application to ion-based frequency standards. Phys. Rev. A 76, 023413 (2007).
Vogelius, I. S., Madsen, L. B. & Drewsen, M. Rotational cooling of heteronuclear molecular ions with 1Σ, 2Σ, Σ, and 1Π electronic ground states. Phys. Rev. A 70, 053412 (2004).
Morigi, G. & Eschner, J. Doppler cooling of a Coulomb crystal. Phys. Rev. A 64, 063407 (2001).
Wineland, D. J. & Itano, W. M. Laser cooling of atoms. Phys. Rev. A 20, 1521–1540 (1979).
Korobov, V. I. Leading-order relativistic and radiative corrections to the rovibrational spectrum of H2+ and HD+. Phys. Rev. A 74, 052506 (2006).
Bakalov, D., Korobov, V. I. & Schiller, S. High-precision calculation of the hyperfine structure of the HD+ ion. Phys. Rev. Lett. 97, 243001 (2006).
Colbourn, E. A. & Bunker, P. R. Accurate theoretical vibration–rotation energies and transition moments for HD+, HT+, and DT+. J. Mol. Spectrosc. 63, 155–163 (1976).
Zhang, C.-B., Offenberg, D, Roth, B., Wilson, M. A. & Schiller, S. Molecular-dynamics simulations of cold-single species and multispecies ion ensembles in a linear Paul trap. Phys. Rev. A 76, 012719 (2007).
Acknowledgements
The authors thank M. Hansen, S. Vasilyev, E. Zlobina for contributions to the experimental set-up and A. Nevsky for helpful discussions. This work is supported by the Deutsche Forschungsgemeinschaft under grant SCHI 431/11-1.
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T.S. and B.R. planned and carried out the experiments, S.S. and H.D. participated, T.S. carried out data evaluation and numerical simulations, B.R. participated, S.S. and H.D. developed the quantum cascade laser and distributed feedback diode laser system, S.S. conceived the study, developed the rate equation model and analytic treatment, I.E. developed a near-infrared diode laser system and participated in preliminary and complementary investigations; T.S. wrote the paper, B.R. and S.S. participated.
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Schneider, T., Roth, B., Duncker, H. et al. All-optical preparation of molecular ions in the rovibrational ground state. Nature Phys 6, 275–278 (2010). https://doi.org/10.1038/nphys1605
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DOI: https://doi.org/10.1038/nphys1605
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