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arXiv:1107.0547 · Physical Chemistry Chemical Physics

Formation of ultracold metastable RbCs molecules by short-range photoassociation

C. Gabbanini, Olivier Dulieu

Published Jan 1, 2011• 47 citations
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Abstract

Ultracold metastable RbCs molecules are observed in a double species magneto-optical trap through photoassociation near the Rb(5S(1/2)) + Cs(6P(3/2)) dissociation limit followed by radiative stabilization. The molecules are formed in their lowest triplet electronic state and are detected by resonance enhanced two-photon ionization through the previously unobserved (3)(3)Π ← a (3)Σ(+) band. The large rotational structure of the observed photoassociation lines is assigned to the lowest vibrational levels of the 0(+) or 0(-) excited states correlated to the Rb(5P(1/2)) + Cs(6S(1/2)) dissociation limit. This demonstrates the possibility of inducing direct photoassociation in heteronuclear alkali-metal molecules at a short internuclear distance, as pointed out earlier [J. Deiglmayr et al., Phys. Rev. Lett., 2008, 101, 13304].

DOI
10.1039/c1cp21497g

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Acta Physica Sinica•Jan 1, 2012•3 citations
Ultracold metastable RbCs molecules are observed in a double species magneto-optical trap through photoassociation near the Rb(5S(1/2)) + Cs(6P(3/2)) dissociation limit followed by radiative stabilization. The molecules are formed in their lowest triplet electronic state and are detected by resonance enhanced two-photon ionization through the previously unobserved (3)(3)Π ← a (3)Σ(+) band. The large rotational structure of the observed photoassociation lines is assigned to the lowest vibrational levels of the 0(+) or 0(-) excited states correlated to the Rb(5P(1/2)) + Cs(6S(1/2)) dissociation limit. This demonstrates the possibility of inducing direct photoassociation in heteronuclear alkali-metal molecules at a short internuclear distance, as pointed out earlier [J. Deiglmayr et al., Phys. Rev. Lett., 2008, 101, 13304].
The formation of ultracold metastable RbCs molecules is observed in a double species magneto-optical trap through photoassociation below the 85 Rb(5S 1/2 ) + 133 Cs(6P 3/2 ) dissociation limit followed by spontaneous emission. The molecules are detected by resonance enhanced two-photon ionization. Using accurate quantum chemistry calculations of the potential energy curves and transition dipole moment, we interpret the observed photoassociation process as occurring at short internuclear distance, in contrast with most previous cold atom photoassociation studies. The vibrational levels excited by photoassociation belong to the 5th 0 + or the 4th 0 − electronic states correlated to the Rb(5P 1/2, 3/2 ) + Cs(6S 1/2 ) dissociation limit. The computed vibrational distribution of the produced molecules shows that they are stabilized in deeply bound vibrational states of the lowest triplet state. We also predict that a noticeable fraction of molecules is produced in the lowest level of the electronic ground state.
We have produced ultracold polar RbCs molecules via photoassociation starting from laser-cooled 85 Rb and 133 Cs atoms in a dual-species, forced dark magneto-optical trap. The formed electronically excited RbCs* molecules correlated to the Rb(5S 1/2 ) + Cs(6P 1/2 ) dissociation limit are observed by trap loss spectroscopy. Following the decay of these excited RbCs* molecules, the formed ground state molecules are directly ionized by a two-photon single-color pulse dye laser, which is a new ionization mechanism for ground state RbCs molecules and thence detected by time-of-flight mass spectroscopy.
We have experimentally studied the formation of ultracold RbCs molecules by photoassociation at short internuclear range followed by spontaneous emission. The observation of new excited levels with respect to our previous work [Gabbanini and Dulieu, Phys. Chem. Chem. Phys. 13, 18905 (2011)] on both sides of the Rb(5S1/2)+Cs(6P3/2)\text{Rb}(5{S}_{1/2})+\text{Cs}(6{P}_{3/2})Rb(5S1/2​)+Cs(6P3/2​) dissociation limit gives information on the state responsible for molecule formation. The molecules are mainly formed in deeply bound levels of the electronic triplet ground state. The observed photoassociation transitions present differences in terms of saturation.
We investigate the production of ultracold ground state X 1 σ + (v = 0) RbCs molecules in the lowest vibrational level via short-range photoassociation followed by spontaneous emission. The starting point is the laser cooled 85 Rb and 133 Cs atoms in a dual species, forced dark magneto-optical trap. The special intermediate level (5)0 + (v = 10) correlated to the (2) 3 π electric state is achieved by the photoassociation process. The formed ground state X 1 σ + (v = 0) molecule is resonantly excited to the 2 1 π intermediate state by a 651 nm pulse laser and is ionized by a 532 nm pulse laser and then detected by the time-of-flight mass spectrum. Saturation of the photoionization spectroscopy at large ionization laser energy is observed and the ionization efficiency is obtained from the fitting. The production of ultracold ground state 85 Rb 133 Cs molecules is facilitative for the further research about the manipulation of ultracold molecules in the rovibrational ground state.
Ultracold polar RbCs molecules are produced via photoassociation in a laser-cooled mixture of 85 Rb and 133 Cs atoms. The a 3 Σ + state molecules which decay from electronically excited (2)0 − state RbCs molecules are detected by resonance-enhanced two-photon ionization. The new rovibrational levels ( v = 189, 190) in the (2)0 − state are also observed, which exist in theory and have not been observed in experiments yet. The corresponding rotational constants are measured by photoassociation spectroscopy, which are consistent with theoretical calculations using a nonrigid rotor model.
Ultracold polar RbCs molecules are produced via photoassociation in a dual dark-SPOT magneto-optical trap, in which ultracold rubidium and cesium atoms with high densities are formed by laser cooling and trapping. The a3∑+ triplet metastable state ultracold RbCs molecules with 104/s production rate are detected using resonance-enhanced two-photon ionization. The ultra-high resolution rovibrational spectra of (2)0+, (3)0- and (2)0- rovibrational states are observed by scanning the photoassociation laser frequency. The rotational constants of (2)0+, (3)0- and (2)0- vibrational states are 0.00349 cm-1, 0.00649 cm-1 and 0.00372 cm-1 by fitting respectively.