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Journal of the Optical Society of America B

Journal of the Optical Society of America B


  • Vol. 20, Iss. 5 — May. 1, 2003
  • pp: 1083–1090

Formation of ultracold molecules by photoassociation: theoretical developments

Olivier Dulieu and Françoise Masnou-Seeuws  »View Author Affiliations

JOSA B, Vol. 20, Issue 5, pp. 1083-1090 (2003)

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In recent years several groups of researchers have succeeded in making samples of cold molecules, at temperatures below 1 K, and of ultracold molecules, at temperatures below 1 mK. We concentrate on the formation of Cs2 dimers. Starting with laser-cooled atoms, photoassociation forms molecules in an excited electronic state. Various mechanisms are presented for stabilizing these molecules by spontaneous emission into a bound level of the ground electronic state. The design of new formation schemes requires precise knowledge of molecular potential curves that is well beyond the accuracy of ab initio calculations. We show that analytical long-range potentials can be fitted on photoassociation spectra and yield, through the determination of the C3 long-range coefficient, a value of the radiative lifetime of the 6P3/2 cesium level with an unprecedented accuracy. For short-range potentials it is possible to avoid explicit calculations by using asymptotic methods that generalize to long-range molecules the quantum-defect concepts developed for Rydberg atoms. Considering two coupled channels, we show how generalized Lu–Fano plots can extract precise information from experimental spectra.

© 2003 Optical Society of America

OCIS Codes
(020.7010) Atomic and molecular physics : Laser trapping
(300.6320) Spectroscopy : Spectroscopy, high-resolution

Olivier Dulieu and Françoise Masnou-Seeuws, "Formation of ultracold molecules by photoassociation: theoretical developments," J. Opt. Soc. Am. B 20, 1083-1090 (2003)

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  1. J. Higgins, C. Callegari, J. Reho, F. Stienkemeier, W. E. Ernst, M. Gutowski, and G. Scoles, “Helium cluster isolation spectroscopy of alkali dimers in the triplet manifold,” J. Phys. Chem. A 102, 4952–4965 (1998).
  2. J. J. Hudson, B. E. Sauer, M. R. Tarbutt, and E. A. Hinds, “Measurement of the electron electric dipole moment using YbF molecules,” Phys. Rev. Lett. 89, 023003, 1–4 (2002).
  3. J. D. Weinstein, R. deCarvalho, T. Guillet, B. Friedrich, and J. M. Doyle, “Magnetic trapping of calcium monohydride molecules at millikelvin temperatures,” Nature 395, 148–150 (1998).
  4. J. M. Doyle and B. Friedrich, “Molecules are cool,” Nature 401, 749–751 (1999).
  5. H. L. Bethlem, G. Berden, and G. Meijer, “Decelerating neutral dipolar molecules,” Phys. Rev. Lett. 83, 1558–1561 (1999).
  6. H. L. Bethlem, G. Berden, A. J. A. van Roij, F. M. H. Crompvoets, and G. Meijer, “Trapping neutral molecules in a traveling potential well,” Phys. Rev. Lett. 84, 5744–5747 (2000).
  7. H. L. Bethlem, G. Berden, F. M. H. Crompvoets, R. T. Jongma, A. J. A. van Roij, and G. Meijer, “Electrostatic trapping of ammonia molecules,” Nature 406, 491–494 (2000).
  8. H. L. Bethlem, G. Berden, F. M. H. Crompvoets, R. T. Jongma, S. Y. T. van de Meerakker, and G. Meijer, “Deceleration and trapping of ammonia using time-varying electric fields,” Phys. Rev. A 65, 053416, 1–20 (2002).
  9. F. M. H. Crompvoets, H. L. Bethlem, R. T. Jongma, and G. Meijer, “A prototype storage ring for neutral molecules,” Nature 411, 174–176 (2001).
  10. A. Fioretti, D. Comparat, A. Crubellier, O. Dulieu, F. Masnou-Seeuws, and P. Pillet, “Formation of Cs2 cold molecules through photoassociation,” Phys. Rev. Lett. 80, 4402–4405 (1998).
  11. A. N. Nikolov, E. E. Eyler, X. T. Wang, J. Li, H. Wang, W. C. Stwalley, and P. L. Gould, “Observation of ultracold ground state potassium molecules,” Phys. Rev. Lett. 82, 703–706 (1999).
  12. A. N. Nikolov, J. R. Enscher, E. E. Eyler, H. Wang, W. C. Stwalley, and P. L. Gould, “Efficient production of ground state potassium molecules at sub-mK temperatures by two-step photoassociation,” Phys. Rev. Lett. 84, 246–249 (2000).
  13. C. Gabbanini, A. Fioretti, A. Lucchesini, S. Gozzini, and M. Mazzoni, “Cold rubidium molecules formed in a magneto-optical trap,” Phys. Rev. Lett. 84, 2814–2817 (2000).
  14. H. R. Thorsheim, J. Weiner, and P. S. Julienne, “Laser-induced photoassociation of ultracold sodium atoms,” Phys. Rev. Lett. 58, 2420–2423 (1987).
  15. A. Fioretti, D. Comparat, C. Drag, C. Amiot, O. Dulieu, F. Masnou-Seeuws, and P. Pillet, “Photoassociative spectroscopy of the Cs2 0g long-range state,” Eur. J. Phys. D 5, 389–403 (1999).
  16. C. M. Dion, C. Drag, O. Dulieu, B. Laburthe Tolra, F. Masnou-Seeuws, and P. Pillet, “Resonant coupling in the formation of ultracold ground state molecules via photoassociation,” Phys. Rev. Lett. 86, 2253–2256 (2001).
  17. R. Co⁁té and A. Dalgarno, “Photoassociation intensities and radiative trap loss in lithium,” Phys. Rev. A 58, 498–508 (1998).
  18. C. M. Dion, O. Dulieu, D. Comparat, W. de Souza Melo, N. Vanhaecke, P. Pillet, R. Beuc, S. Milošević, and G. Pichler, “Photoionization and detection of ultracold Cs2 molecules through diffuse bands,” Eur. J. Phys. D 18, 365–370 (2002).
  19. C. Drag, B. Laburthe Tolra, O. Dulieu, D. Comparat, M. Vatasescu, S. Boussen, S. Guibal, A. Crubellier, and P. Pillet, “Experimental versus theoretical rates for photoassociation and for formation of ultracold molecules,” IEEE J. Quantum Electron. 36, 1378 (2000).
  20. J. Vala, O. Dulieu, F. Masnou-Seeuws, and R. Kosloff, “Coherent control of cold molecule formation through photoassociation using a chirped pulsed laser field,” Phys. Rev. A 63, 013412, 1–12 (2001).
  21. N. Vanhaecke, W. de Souza Melo, B. Laburthe Tolra, D. Comparat, and P. Pillet, “Accumulation of cold cesium molecules via photoassociation in a mixed atomic and molecular trap,” Phys. Rev. Lett. 89, 063001, 1–4 (2002).
  22. E. Tiesinga, C. J. Williams, and P. S. Julienne, “Photoassociative spectroscopy of highly excited vibrational levels of alkali dimers: Green’s function approach for eigenvalue solvers,” Phys. Rev. A 57, 4257–4267 (1998).
  23. V. Kokoouline, O. Dulieu, R. Kosloff, and F. Masnou-Seeuws, “Mapped Fourier methods for long-range molecules: application to perturbations in the Rb2(0u+) photoassociation spectrum,” J. Chem. Phys. 110, 9865–9876 (1999).
  24. V. Kokoouline, O. Dulieu, R. Kosloff, and F. Masnou-Seeuws, “Theoretical treatment of channel mixing in excited Rb2 and Cs2 ultracold molecules. II. Determination of predissociation lifetimes with coordinate mapping,” Phys. Rev. A 62, 032716, 1–10 (2000).
  25. N. Spiess, “Ab initio calculations for Cs2,” Ph.D dissertation (Universität Kaiserslautern, Kaiserslautern, Germany, 1989).
  26. M. Foucrault, Ph. Millié, and J. P. Daudey, “Non-perturbative method for corevalence correlation in pseudopotential calculations: application to the Rb2 and Cs2 molecules,” J. Chem. Phys. 96, 1257–1264 (1992).
  27. A. Allouche, M. Korek, K. Fakherddin, A. Chaalan, M. Dagher, F. Taher, and M. Aubert-Frécon, “Theoretical electronic structure of RbCs revisited,” J. Phys. B 33, 2307–2316 (2000).
  28. M. Marinescu and A. Dalgarno, “Analytical interaction potentials of the long range alkali-metal dimers,” Z. Phys. D 36, 239–258 (1996).
  29. C. Amiot, O. Dulieu, R. F. Gutterres, and F. Masnou-Seeuws, “Determination of the Cs2 0g(P3/2) potential curve and Cs 6p1/2, 3/2 radiative lifetimes from photoassociation spectroscopy,” Phys. Rev. A 66, 052506, 1–9 (2002).
  30. L. Young, W. T. Hill III, S. J. Sibener, S. D. Price, C. E. Tanner, C. E. Wieman, and S. R. Leone, “Precision lifetime measurements of Cs 6p 2P1/2 and Cs 6p 2P3/2 levels by single-photon counting,” Phys. Rev. A 50, 2174–2181 (1994).
  31. R. J. Rafac, C. E. Tanner, A. E. Livingston, K. W. Kukla, H. G. Berry, and C. A. Kurtz, “Fast-beam laser lifetime measurements of the cesium 6p2 P1/2, 3/2 states,” Phys. Rev. A 60, 3648–3662 (1999).
  32. A. Derevianko and S. G. Porsev, “Determination of lifetimes of 6PJ levels and ground-state polarizability of Cs from van der Waals coefficient C6,” Phys. Rev. A 65, 053403 (2002).
  33. C. Drag, B. Laburthe Tolra, B. T’Jampens, D. Comparat, M. Allegrini, A. Crubellier, and P. Pillet, “Photoassociative spectroscopy as a self-sufficient tool for the determination of the Cs triplet scattering length,” Phys. Rev. Lett. 85, 1408–1411 (2000).
  34. P. J. Leo, C. J. Williams, and P. S. Julienne, “Collision properties of ultracold 133Cs atoms,” Phys. Rev. Lett. 85, 2721–2724 (2000).
  35. E. I. Dashevskaya, A. I. Voronin, and E. E. Nikitin, “Theory of excitation transfer in collisions between alkali atoms. I. Identical partners,” Can. J. Phys. 47, 1237–1246 (1969).
  36. E. I. Dashevskaya and E. E. Nikitin, “Polarization transfer and relaxation induced in collisions of excited alkali atoms,” Can. J. Phys. 54, 709–719 (1976).
  37. P. S. Julienne and J. Vigué, “Cold collisions of ground and excited state alkali-metal atoms,” Phys. Rev. A 44, 4464–4485 (1991).
  38. C. Amiot, O. Dulieu, and J. Vergès, “Resolution of the apparent disorder of the Rb2 A 1Σu+(0u+) and b 3Πu(0u+) spectra: a case of fully coupled electronic states,” Phys. Rev. Lett. 83, 2316–2319 (1999).
  39. R. J. Le Roy and R. B. Bernstein, “Dissociation energy and long-range potential of diatomic molecules from vibrational spacings of higher levels,” J. Chem. Phys. 52, 3869–3874 (1970).
  40. V. N. Ostrovsky, V. Kokoouline, E. Luc-Koenig, and F. Masnou-Seeuws, “Lu–Fano plots for potentials with non-Coulomb tails: application to vibrational spectra of long-range diatomic molecules,” J. Phys. B 34, L27–L38 (2001).
  41. K. T. Lu and U. Fano, “Graphic analysis of perturbed Rydberg Series,” Phys. Rev. A 2, 81–86 (1970).
  42. V. Kokoouline, C. Drag, P. Pillet, and F. Masnou-Seeuws, “Lu–Fano plots for interpretation of the photoassociation spectra,” Phys. Rev. A 65, 062710, 1–10 (2002).
  43. A. Fioretti, E. Arimondo, and A. Crubellier, “Flux enhancement model for cold cesium fine-structure changing collisions,” Eur. J. Phys. D 12, 219–225 (2000).
  44. M. Lintz and M. A. Bouchiat, “Dimer destruction in a Cs vapor by a laser close to atomic resonance,” Phys. Rev. Lett. 80, 2570–2573 (1998).
  45. P. Pellegrini, O. Dulieu, and F. Masnou-Seeuws, “Formation of Cs2 molecules via Feshbach resonances stabilized by spontaneous emission: theoretical treatment with the Fourier grid method,” Eur. J. Phys. 20, 77–86 (2002).

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