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Physica Scripta

Formation of Ultra-Cold Cs2Molecules Through Photoassociation

P. Pillet

Published Jan 1, 2003• 3 citations
Publisher

Abstract

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.

DOI
10.1238/physica.regular.068ac0048

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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.
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.
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.
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.
Recent experiments on formation of translationally cold ground state molecules, their subsequent broadband vibrational cooling and study of rotations are presented together with the related modeling. We produce cold molecules by photoassociating pairs of cold cesium atoms that can decay into ground state molecules in different vibrational levels. Then we laser cool the vibrational degree of freedom by selecting a single target vibrational level. Our method is based on repeated optical pumping by laser light with a spectrum broad enough to excite all populated vibrational levels but limited in its frequency bandwidth with a spatial light modulator. In such a way we are able to eliminate transitions from the selected level, in which molecules accumulate. Results for vibrational cooling into the v = 0, v = 1, v = 2 and v = 7 level of the singlet X 1Σ g ground electronic state are presented. Depletion spectroscopy is performed to study the rotational distribution of the created molecules. In the theoretical modeling of the process we are able to reproduce our results and investigate the prospects for a ‘complete’ cooling of molecules, including also their rotational degree of freedom.
The possibility of controlling all the motion as well as the internal quantum state of a sample of molecules is a long term goal in the cold molecules field. Although many different techniques have been used to produce ultra-cold molecules, in this paper, we will concentrate on the optical pumping technique successfully used to achieve rotational and vibrational cooling of Cs2molecules. We will review the different photo-association schemes for molecule formation, the detection schemes through photoionization, the ro-vibrational cooling into a single level and finally the electronic conversion. In addition, we will present a theoretical model for both ro-vibrational cooling and electronic conversion that can be used for the preparation of different experiments.
The methods producing cold molecules from cold atoms tend to leave molecular ensembles with substantial residual internal energy. For instance, cesium molecules initially formed via photoassociation of cold cesium atoms are in several vibrational levels nu of the electronic ground state. We applied a broadband femtosecond laser that redistributes the vibrational population in the ground state via a few electronic excitation/spontaneous emission cycles. The laser pulses are shaped to remove the excitation frequency band of the nu = 0 level, preventing re-excitation from that state. We observed a fast and efficient accumulation ( approximately 70% of the initially detected molecules) in the lowest vibrational level, nu = 0, of the singlet electronic state. The validity of this incoherent depopulation pumping method is very general and opens exciting prospects for laser cooling and manipulation of molecules.