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Physical Review Letters

Formation of Cold Cs2 Molecules through Photoassociation

A. Fioretti, D. Comparat, A. Crubellier, Olivier Dulieu, Françoise Masnou-Seeuws, P. Pillet

Published May 18, 1998• 545 citations
Publisher

Abstract

We have performed photoassociative spectroscopy of cold Cs atoms in a vapor-cell magneto-optical trap, within $10{\mathrm{cm}}^{\ensuremath{-}1}$ below the dissociation limit $6s^{2}S_{1/2}+6p^{2}P_{3/2}$. Our detection method is based on pulsed-laser photoionization of ${\mathrm{Cs}}_{2}$ molecules, selectively detected through a time-of-flight mass spectrometer. Temporal and spatial analysis of ${\mathrm{Cs}}_{2}^{+}$ ions show for the first time the formation of translationally cold ${\mathrm{Cs}}_{2}$ triplet ground state molecules, at a temperature $T\ensuremath{\sim}300\ensuremath{\mu}\mathrm{K}$.

DOI
10.1103/physrevlett.80.4402

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We report on the observation of translationally cold Cs2 molecules at temperatures in the 300–70 μK range, produced by the photoassociation of cold Cs atoms in a vapor-cell magneto-optical trap. The detection method is based on pulsed-laser photoionization of Cs2 molecules into Cs2+ ions, selectively detected through a time-of-flight mass spectrometer. This technique, together with the usual trap-loss method, enables us to perform the spectroscopy of the long-range attractive molecular states below the 6s 2S1/2+6p 2P3/2 dissociation limit.
We report on the formation of translationally cold Cs2 ground-state molecules through photoassociation of laser-cooled cesium atoms in a magneto-optical trap. The cold molecules are obtained after spontaneous decay of photoassociated molecules, and detected after pulsed-laser photoionization into Cs2+ ions. Photoassociation spectra of cesium attractive molecular states below the 6S1/2+6P3/2 dissociation limits are reported, obtained with both ion detection and trap-loss method. A temperature as low as 20−5+15 has been measured for the molecular cloud.
PHOTOASSOCIATIVE SPECTROSCOPY OF Cs2Cs_{2}Cs2​ MOLECULE
We report the spectroscopy of molecular 1g,0u+,0g−1_{g}, 0^{+}_{u}, 0^{-}_{g}1g​,0u+​,0g−​ and 1u1_{u}1u​ state potentials below the dissociattion limit 6s2S1/2+6p2P3/26s^{2}S_{1/2}+6p^{2}P_{3/2}6s2S1/2​+6p2P3/2​ by using the molecular photoassociation technique of cold Cs atoms, in a vapor-cell magneto-optical trap. The 1g1_{g}1g​ and 0g+0^{+}_{g}0g+​ states are detected by trap losses. The 0g−0^{-}_{g}0g−​ and 1u1_{u}1u​ states, which lead to the formation of cold molecules [1], are detected by photoionizing them into Cs2+Cs_{2}^{+}Cs2+​ and detecting with a time-of-flight mass spectrometer, while the lgl_{g}lg​ and 0u+0^{+}_{u}0u+​ states are detected by trap losses. We give the spectra of the whole series 0g−0^{-}_{g}0g−​ and 1u1_{u}1u​. The 0g−0^{-}_{g}0g−​ series is analyzed in a RKR approach and the hyperfine structure of the 1u1_{u}1u​ series will be discussed. The observed modulation of intensities of the lines is due to Franck Condon factors characterizing the photoassociative transition between the initial state of two free atoms and the finalro-vibrational level. The intensity modulation can give access to the scattering lengths of the ground state. This possibility will be discussed.
We have observed translationally cold electronic ground-state cesium dimers produced directly in a magneto-optical trap and also by photoassociation of cold atoms in this trap. These neutral molecules were detected using photoionization and time-of-flight spectroscopy. Initial experiments indicated a cold molecular formation rate of about $600{\mathrm{s}}^{\mathrm{\ensuremath{-}}1},$ with no photoassociation laser present. The measured translational temperature of the neutral cesium dimers was approximately 100 \ensuremath{\mu}K.
In the molecular photoassociation process, two free cold atoms absorb one photon by a resonant way, to create an excited molecule in a well defined ro-vibrational state. The photoassociative spectroscopy of alkaline dimers yields accurate determinations for the long-range parts of molecular potential curves correlated to the first s + p asymptote. In contrast to atoms, laser cooling of molecules is very difficult because of the lack of a closed two-level scheme for recycling the population. The molecular photoassociation of cold atoms opens also a promising alternative for the formation of cold ground state molecules. Photoassociation of cold cesium atoms has permitted the first observation of translationally cold ground state molecules. The case of the cesium atom is very favorable because the 0 g - and 1 u purely long-range states below the dissociation limit 6s 1/2 +6p 3/2 present Condon points at intermediate distances. Such configurations offer rather efficient channels for the creation of singlet or triplet ground state Cs 2 molecules after spontaneous decay.
We demonstrate the formation of cold ground-state Cs2{\mathrm{Cs}}_{2}Cs2​ molecules (presumably in a single well-defined rovibrational level) by stimulated Raman photoassociation (PA) in a Cs vapor cell magneto-optical trap. Autler-Townes measurements allow us to precisely define the experimental conditions. The efficiency of the process is comparable to that of the formation of cold molecules obtained after spontaneous deexcitation of photoassociated molecules. Stimulated Raman PA should provide samples where the molecules are cold not only translationally, but are also in a selected rovibrational level.