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Triplet-singlet conversion in ultracold Cs$_2$ and production of ground state molecules

Nadia Bouloufa-Maafa, Marin Pichler, M Aymar, Olivier Dulieu

Published Nov 10, 2010• 0 citations
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Abstract

We propose a process to convert ultracold metastable Cs$_2$ molecules in their lowest triplet state into (singlet) ground state molecules in their lowest vibrational levels. Molecules are first pumped into an excited triplet state, and the triplet-singlet conversion is facilitated by a two-step spontaneous decay through the coupled $A^{1}\Sigma_{u}^{+} \sim b ^{3}\Pi_{u}$ states. Using spectroscopic data and accurate quantum chemistry calculations for Cs$_2$ potential curves and transition dipole moments, we show that this process has a high rate and competes favorably with the single-photon decay back to the lowest triplet state. In addition, we demonstrate that this conversion process represents a loss channel for vibrational cooling of metastable triplet molecules, preventing an efficient optical pumping cycle down to low vibrational levels.

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We demonstrate the conversion of cold Cs2{}_{2}2​ molecules initially distributed over several vibrational levels of the lowest triplet state ${a}^{3}\phantom{\rule{0.16em}{0ex}}{\ensuremath{\Sigma}}_{u}^{+}$ into the singlet ground state ${X}^{1}\phantom{\rule{0.16em}{0ex}}{\ensuremath{\Sigma}}_{g}^{+}$. This conversion is realized by a broadband laser exciting the molecules to a well-chosen state from which they may decay to the singlet state through two sequential single-photon emission steps: The first photon populates levels with mixed triplet-singlet character, making possible a second spontaneous emission down to several vibrational levels of the ${X}^{1}\phantom{\rule{0.16em}{0ex}}{\ensuremath{\Sigma}}_{g}^{+}$ states. By adding an optical scheme for vibrational cooling, a substantial fraction of molecules are transferred to the ground vibrational level of the singlet state. The efficiency of the conversion process, with and without vibrational cooling, is discussed at the end of the article. The presented conversion is general in scope and could be extended to other molecules.
Using resonance-enhanced two-photon ionization, we detect ultracold, metastable RbCs molecules formed in their lowest triplet state $a\text{ }^{3}\ensuremath{\Sigma}^{+}$ via photoassociation in a laser-cooled mixture of 85Rb^{85}\mathrm{Rb}85Rb and 133Cs^{133}\mathrm{Cs}133Cs atoms. We obtain extensive bound-bound excitation spectra of these molecules, which provide detailed information about their vibrational distribution, as well as spectroscopic data on several RbCs molecular states including $a\text{ }^{3}\ensuremath{\Sigma}^{+}$, $(2)\text{ }^{3}\ensuremath{\Sigma}^{+}$, and $(1)\text{ }^{1}\ensuremath{\Pi}$. Analysis of this data allows us to predict strong transitions from observed levels to the absolute vibronic ground state of RbCs, potentially allowing the production of stable, ultracold polar molecules at rates in excess of ${10}^{6}\text{ }{\mathrm{s}}^{\ensuremath{-}1}$.
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Ultracold collisions between Cs atoms and Cs2{\mathrm{Cs}}_{2}Cs2​ dimers in the electronic ground state are observed in an optically trapped gas of atoms and molecules. The Cs2{\mathrm{Cs}}_{2}Cs2​ molecules are formed in the triplet ground state by cw photoassociation through the outer well of the ${0}_{g}^{\ensuremath{-}}({P}_{3/2})$ excited electronic state. Inelastic atom-molecule collisions converting internal excitation into kinetic energy lead to a loss of Cs2{\mathrm{Cs}}_{2}Cs2​ molecules from the dipole trap. Rate coefficients are determined for collisions involving Cs atoms in either the F=3F=3F=3 or F=4F=4F=4 hyperfine ground state, and Cs2{\mathrm{Cs}}_{2}Cs2​ molecules in either highly vibrationally excited states (${v}^{\ensuremath{'}}=32--47$) or in low vibrational states (${v}^{\ensuremath{'}}=4--6$) of the $a\text{ }^{3}\ensuremath{\Sigma}_{u}^{+}$ triplet ground state. The rate coefficients $\ensuremath{\beta}\ensuremath{\sim}{10}^{\ensuremath{-}10}\text{ }\text{ }{\mathrm{cm}}^{3}/\mathrm{s}$ are found to be largely independent of the vibrational and rotational excitation indicating unitary limited cross sections.
Production and state-selective detection of ultracold molecular rubidium (85Rb2) in the singlet ground state and the metastable triplet state are described. Ultracold 85Rb2 molecules are produced via photoassociation followed by radiative decay. State-selective detection of high-ν ground-state and metastable-state molecules is carried out by resonant Two-photon ionization (R2PI) with a pulsed laser. The spectra of both the ground singlet and metastable triplet states are investigated. Spectroscopy of several intermediate excited states, some of which are observed for the first time, is also studied. Mixing between excited singlet and triplet states is observed in both the singlet and triplet spectra. A proposal for producing ν = 0 ground-state molecules by utilizing this singlet-triplet mixing is given. Magnetic trapping and filtering of metastable triplet-state molecules is also described, and a scheme for optical trapping of molecules is proposed.^