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Physical Review A

Formation of ultracold Cs2 molecules through the double-minimum Cs2 31Σu+ state

Marin Pichler, William C. Stwalley, Robert Beuc, Goran Pichler

Published Jan 15, 2004• 12 citations
Publisher

Abstract

We present a simple model of ultracold cesium dimer formation in which the photoassociation into rovibrational levels of the double-minimum ${\mathrm{Cs}}_{2}$ $3{}^{1}{\ensuremath{\Sigma}}_{u}^{+}$ state above its internal barrier enables spontaneous or stimulated emission into the lowest rovibrational levels of the ${\mathrm{Cs}}_{2}$ $1(X){}^{1}{\ensuremath{\Sigma}}_{g}^{+}$ ground electronic state. The transition dipole moment should be sufficiently large for observation of such spectral transitions. The use of the ${\mathrm{Cs}}_{2}$ $3{}^{1}{\ensuremath{\Sigma}}_{u}^{+}$ double-minimum potential could be extended to molecular Bose-Einstein condensates in which an optical trap can be employed for trapping of both atomic and molecular species.

DOI
10.1103/physreva.69.013403

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We present a simple model of ultracold cesium dimer formation in which the photoassociation into rovibrational levels of the double-minimum Cs2{\mathrm{Cs}}_{2}Cs2​ 31\ensuremathΣu+3{}^{1}{\ensuremath{\Sigma}}_{u}^{+}31\ensuremathΣu+​ state above its internal barrier enables spontaneous or stimulated emission into the lowest rovibrational levels of the Cs2{\mathrm{Cs}}_{2}Cs2​ 1(X)1\ensuremathΣg+1(X){}^{1}{\ensuremath{\Sigma}}_{g}^{+}1(X)1\ensuremathΣg+​ ground electronic state. The transition dipole moment should be sufficiently large for observation of such spectral transitions. The use of the Cs2{\mathrm{Cs}}_{2}Cs2​ 31\ensuremathΣu+3{}^{1}{\ensuremath{\Sigma}}_{u}^{+}31\ensuremathΣu+​ double-minimum potential could be extended to molecular Bose-Einstein condensates in which an optical trap can be employed for trapping of both atomic and molecular species.
We study the rovibronic transitions in NaK 2 between its electronic ground state 1 2 A ′ and its second excited state 3 2 A ′ , to identify possible pathways for the creation of ultracold ground-state triatomic molecules. Our methodology relies on the computation of potential energy surfaces and transition dipole moment surfaces for the relevant electronic states using methods. Rovibrational energy levels and wave functions are determined using the discrete variable representation approach. A double-well structure of the potential energy surface is identified for both states, and the related transition strengths between the rovibrational levels are derived. Our calculations show that the formation of ultracold ground-state NaK 2 molecules is expected when starting from an excited electronic state of NaK 2 , which can be created by photoassociation of NaK and K, as observed by optical means by Cao, [].
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.
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.
The double-minimum 3 $^{1}\mathrm{\ensuremath{\Sigma}}_{\mathrm{u}}^{\phantom{\rule{0.28em}{0ex}}\phantom{\rule{0.16em}{0ex}}+}$ state in 85Rb2^{85}\mathrm{Rb}_{2}85Rb2​ and 85Rb87Rb^{85}\mathrm{Rb}\phantom{\rule{0.16em}{0ex}}^{87}\mathrm{Rb}85Rb87Rb was investigated by analyzing rotationally resolved spectra of the 3 $^{1}\mathrm{\ensuremath{\Sigma}}_{\mathrm{u}}^{\phantom{\rule{0.28em}{0ex}}\phantom{\rule{0.16em}{0ex}}+}\ensuremath{\longleftarrow}\mathrm{X}^{1}\mathrm{\ensuremath{\Sigma}}_{\mathrm{g}}^{+}$ band system simplified by polarization labeling. A total of 3665 transitions to rovibrational levels located in the inner well and above the internal barrier were identified and an accurate potential energy curve of the state reaching up to $R\ensuremath{\approx}21$ \AA{} was constructed using the inverted perturbation approach, making this state the best characterized double-minimum state in alkali dimers. The possibility of formation of ultracold rubidium dimers in the absolute ground state by photoassociation into levels of the 3 $^{1}\mathrm{\ensuremath{\Sigma}}_{\mathrm{u}}^{\phantom{\rule{0.28em}{0ex}}\phantom{\rule{0.16em}{0ex}}+}$ state above the internal barrier followed by spontaneous or stimulated emission is discussed.
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.
Using a nonselective broadband detection scheme we discovered an efficient mechanism of formation of ultracold Cs2{\mathrm{Cs}}_{2}Cs2​ molecules in deeply bound vibrational levels (v=1−−9)(v=1--9)(v=1−−9) of their electronic ground state $X\phantom{\rule{0.2em}{0ex}}^{1}\ensuremath{\Sigma}_{g}^{+}$. They are formed by a one-photon photoassociation of ultracold cesium atoms in a manifold of excited electronic states, followed by a two-step spontaneous emission cascade. This process creates about 105−−106moleculespersecond{10}^{5}--{10}^{6}\phantom{\rule{0.3em}{0ex}}\text{molecules}\phantom{\rule{0.3em}{0ex}}\text{per}\phantom{\rule{0.3em}{0ex}}\text{second}105−−106moleculespersecond. This detection scheme is an advancement compare to previous ones and could be generalized to other molecular species for the systematic investigation of cold molecule formation mechanisms.