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Quantum Electronics and Laser Science Conference

Formation and spectroscopy of ultracold Cs/sub 2/ molecules

P. Pillet

Published Jan 20, 2003• 0 citations
Publisher

Abstract

Summary form only given. 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 a promising alternative for the formation of cold molecules. The photoassociative spectra are obtained by the usual trap-loss method as well as by pulsed laser photoionization of Cs/sub 2/ molecules into Cs/sub 2//sup +/ ions. Different schemes to obtain formation of cold molecules through photoassociation will be discussed.

DOI
10.1109/qels.1999.807465

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Summary form only given. 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 a promising alternative for the formation of cold molecules. The photoassociative spectra are obtained by the usual trap-loss method as well as by pulsed laser photoionization of Cs/sub 2/ molecules into Cs/sub 2//sup +/ ions. Different schemes to obtain formation of cold molecules through photoassociation will be discussed.
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.
In contrast to atoms, laser cooling of molecules is very difficult because of the lack of a closed two-level scheme for population recycling. Molecular photoassociation of cold atoms has permitted the first observation of the formation of cold ground state Cs 2 molecules. In this scheme, two free cold atoms absorb one photon, to form an electronically excited molecule in a well-defined ro-vibrational state, which yields translationally cold molecules, after spontaneous decay, in their ground state or in their lowest triplet state.
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.
We report on the spectra of the long-range attractive molecular states of the Cs/sub 2/ dimer below the dissociation limits 6s+6p/sub 1/2/ and 6s+6p/sub 3/2/ which are accessible by molecular photoassociation of cold Cs atoms. For the states O/sub u//sup +/ and O/sub g//sup -/(6s+6p/sub 3/2/), we have performed trap-loss measurements, which are in good agreement with the theoretical calculations, performed in a perturbative approach. For the O/sub g//sup -/ and 1/sub u/(6s+6p/sub 3/2/) states, we observe, after spontaneous decay of the electronically excited molecules, the formation of translationally cold molecules. A rate of formation of cold molecules of the order of /spl sim/10/sup 6/ molecules per second is obtained in the case of the state O/sub g//sup $/.
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 6s2S1/2+6p2P3/26s^{2}S_{1/2}+6p^{2}P_{3/2}6s2S1/2​+6p2P3/2​. Our detection method is based on pulsed-laser photoionization of Cs2{\mathrm{Cs}}_{2}Cs2​ molecules, selectively detected through a time-of-flight mass spectrometer. Temporal and spatial analysis of Cs2+{\mathrm{Cs}}_{2}^{+}Cs2+​ ions show for the first time the formation of translationally cold Cs2{\mathrm{Cs}}_{2}Cs2​ triplet ground state molecules, at a temperature $T\ensuremath{\sim}300\ensuremath{\mu}\mathrm{K}$.
The cold-molecule field concerns the physics and the applications of molecular systems with translational temperature well below the 1 К range. The possibility of controlling all the motion as well as the internal quantum state of a sample of molecules is a long-term goal that opens the possibility for many new experiments and measurements ranging from fundamental constants to quantum chemistry and quantum computation. Although, direct laser cooling of the translational degree of freedom of molecules is still waiting for further technological or theoretical breakthroughs and ideas, many different techniques have proven to be successful in producing different types of cold as well as ultracold (i.e. T < 1 mK) molecules. In this chapter, we will concentrate on the description of one of these techniques: the photoassociation of laser cooled atoms. We will report on the status of the art of this technique for the case of cesium atoms, describing all the main experimental findings. In particular, we will illustrate the different photoassociation schemes for molecule formation, the detection schemes through photoionization, the molecule trapping in a magnetic or dipolar trap, the vibrational cooling into a single vibrational state and finally the present prospects for rotational cooling.