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Bulletin of the American Physical Society

Manipulation of the vibration of cold ground-state Cesium molecules

Matthieu Viteau, Amodsen Chotia, M. Allegrini, D. Comparat, P. Pillet

Published Mar 12, 2008• 0 citations
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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.

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The use of a broadband, frequency shaped femtosecond laser on translationally cold cesium molecules has recently demonstrated to be a very efficient method of cooling also the vibrational degree of freedom. A sample of cold molecules, initially distributed over several vibrational levels, has thus been transfered into a single selected vibrational level of the singlet X1g ground electronic state. 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. In this paper we briefly report the main experimental results and then address, in a detailed way by computer simulations, the perspectives for a complete" cooling of the molecules, including also the rotational degree of freedom. Since the pumping process strongly depends on the relative shape of the ground and excited potential curves, ro-vibrational cooling through different excited states is theoretically compared.

Chinese Journal of Chemical Physics•Apr 1, 2009•6 citations
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.
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 use of a broadband, frequency shaped femtosecond laser on translationally cold cesium molecules has recently demonstrated to be a very efficient method of cooling also the vibrational degree of freedom. A sample of cold molecules, initially distributed over several vibrational levels, has thus been transfered into a single selected vibrational level of the singlet X1g ground electronic state. 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. In this paper we briefly report the main experimental results and then address, in a detailed way by computer simulations, the perspectives for a complete" cooling of the molecules, including also the rotational degree of freedom. Since the pumping process strongly depends on the relative shape of the ground and excited potential curves, ro-vibrational cooling through different excited states is theoretically compared.