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arXiv:physics/0509123 · Physical Review Letters

Experimental Investigation of Ultracold Atom-Molecule Collisions

Peter Frøhlich Staanum, Stephan Kraft, Jörg Lange, Roland Wester, Matthias Weidemüller

Published Jan 19, 2006• 145 citations
arXivHTMLPDF

Abstract

Ultracold collisions between Cs atoms and ${\mathrm{Cs}}_{2}$ dimers in the electronic ground state are observed in an optically trapped gas of atoms and molecules. The ${\mathrm{Cs}}_{2}$ 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 ${\mathrm{Cs}}_{2}$ molecules from the dipole trap. Rate coefficients are determined for collisions involving Cs atoms in either the $F=3$ or $F=4$ hyperfine ground state, and ${\mathrm{Cs}}_{2}$ 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.

DOI
10.1103/physrevlett.96.023201

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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 0g\ensuremath−(P3/2){0}_{g}^{\ensuremath{-}}({P}_{3/2})0g\ensuremath−​(P3/2​) 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{v}^{\ensuremath{'}}=32--47v\ensuremath′=32−−47) or in low vibrational states (v\ensuremath′=4−−6{v}^{\ensuremath{'}}=4--6v\ensuremath′=4−−6) of the a 3\ensuremathΣu+a\text{ }^{3}\ensuremath{\Sigma}_{u}^{+}a 3\ensuremathΣu+​ triplet ground state. The rate coefficients \ensuremathβ\ensuremath∼10\ensuremath−10  cm3/s\ensuremath{\beta}\ensuremath{\sim}{10}^{\ensuremath{-}10}\text{ }\text{ }{\mathrm{cm}}^{3}/\mathrm{s}\ensuremathβ\ensuremath∼10\ensuremath−10  cm3/s are found to be largely independent of the vibrational and rotational excitation indicating unitary limited cross sections.
In this thesis properties of ultracold alkali dimers are studied both theoretically and experimentally. In the first, theoretical, part, the prospects for the formation of ultracold LiCs dimers in deeply bound vibrational levels using photoassociation (PA) are investigated. Furthermore a previous systematic investigation of the structure of all alkali dimers is extended by the ab initio calculation of static dipole polarizabilities. An extensive comparison with other published results supports the reliability of the chosen method. Based on these results an experimental scheme for the creation of an sample of oriented ultracold dipolar molecules is developed. In the second, experimental part the formation of LiCs ground state molecules by PA is investigated. PA spectroscopy is used to improve the accuracy of the potential energy curve for the B1P and the value of the dissociation energy of the X1S+ state significantly. The rovibrational distribution of ground state molecules is probed in a combination of resonance-enhanced multi-photon ionization and depletion spectroscopy. A simple scheme is found to form ultracold polar LiCs molecules in the absolute ground state X1S+,v''=0,J''=0. In a quasi-electrostatic trap created by a CO2 laser, LiCs molecules are formed and stored. A lifetime of 24(3)s, limited by collisions with background gas, is observed and rate coefficients for inelastic collisions between LiCs in high vibrational states and Cs atoms are determined. The long storage time facilitates the observation of radiative decay of polar molecules towards lower vibrational levels.
We report on the observation of photoassociation resonances in ultracold collisions between ^{23}Na^{40}K molecules and ^{40}K atoms. We perform photoassociation in a long-wavelength optical dipole trap to form deeply bound triatomic molecules in electronically excited states. The atom-molecule Feshbach resonance is used to enhance the free-bound Franck-Condon overlap. The photoassociation into well-defined quantum states of excited triatomic molecules is identified by observing resonantly enhanced loss features. These loss features depend on the polarization of the photoassociation lasers, allowing us to assign rotational quantum numbers. The observation of ultracold atom-molecule photoassociation resonances paves the way toward preparing ground-state triatomic molecules, provides a new high-resolution spectroscopy technique for polyatomic molecules, and is also important to atom-molecule Feshbach resonances.
Cold inelastic collisions between confined cesium (Cs) atoms and Cs2{\mathrm{Cs}}_{2}Cs2​ molecules are investigated inside a CO2{\mathrm{CO}}_{2}CO2​ laser dipole trap. Inelastic atom-molecule collisions can be observed and measured with a rate coefficient of $\ensuremath{\sim}2.6\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}11}\text{ }\text{ }{\mathrm{cm}}^{3}\text{ }{\mathrm{s}}^{\ensuremath{-}1}$, mainly independent of the molecular rovibrational state populated. Lifetimes of purely atomic and molecular samples are essentially limited by rest gas collisions. The pure molecular trap lifetime ranges 0.3--1 s, 4 times smaller than the atomic one, as is also observed in a pure magnetic trap. We give an estimation of the inelastic molecule-molecule collision rate to be $\ensuremath{\sim}{10}^{\ensuremath{-}11}\text{ }\text{ }{\mathrm{cm}}^{3}\text{ }{\mathrm{s}}^{\ensuremath{-}1}$.
Abstract Understanding ultracold collisions involving molecules is of fundamental importance for current experiments, where inelastic collisions typically limit the lifetime of molecular ensembles in optical traps. Here we present a broad study of optically trapped ultracold RbCs molecules in collisions with one another, in reactive collisions with Rb atoms, and in nonreactive collisions with Cs atoms. For experiments with RbCs alone, we show that by modulating the intensity of the optical trap, such that the molecules spend 75% of each modulation cycle in the dark, we partially suppress collisional loss of the molecules. This is evidence for optical excitation of molecule pairs mediated via sticky collisions. We find that the suppression is less effective for molecules not prepared in the spin-stretched hyperfine ground state. This may be due either to longer lifetimes for complexes in the dark or to laser-free decay pathways. For atom–molecule mixtures, RbCs + Rb and RbCs + Cs, we demonstrate that the rate of collisional loss of molecules scales linearly with the density of atoms. This indicates that, in both cases, the loss of molecules is rate-limited by two-body atom–molecule processes. For both mixtures, we measure loss rates that are below the thermally averaged universal limit.
We report the measurement of collision rate coefficient for collisions between ultracold Cs atoms and low-energy Cs+\mathrm{C}{\mathrm{s}}^{+}Cs+ ions. The experiments are performed in a hybrid trap consisting of a magneto-optical trap (MOT) for Cs atoms and a Paul trap for Cs+\mathrm{C}{\mathrm{s}}^{+}Cs+ ions. The ion-atom collisions impart kinetic energy to the ultracold Cs atoms, resulting in their escape from the shallow MOT and, therefore, in a reduction in the number of Cs atoms in the MOT. By monitoring, using fluorescence measurements, the Cs atom number, and the MOT loading dynamics and then fitting the data to a rate equation model, the ion-atom collision rate is derived. The $\mathrm{Cs}\ensuremath{-}\mathrm{C}{\mathrm{s}}^{+}$ collision rate coefficient $9.3(\ifmmode\pm\else\textpm\fi{}0.4)(\ifmmode\pm\else\textpm\fi{}1.2)(\ifmmode\pm\else\textpm\fi{}3.5)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}14}\phantom{\rule{0.16em}{0ex}}{\mathrm{m}}^{3}\phantom{\rule{0.28em}{0ex}}{\mathrm{s}}^{\ensuremath{-}1}$, measured for an ion distribution with most probable collision energy of 95 meV $(\ensuremath{\approx}{\mathrm{k}}_{\mathrm{B}}\phantom{\rule{4pt}{0ex}}1100\phantom{\rule{4pt}{0ex}}\mathrm{K})$, is in fair agreement with theoretical calculations. As an intermediate step, we also determine the photoionization cross section of Cs 6P3/26{P}_{3/2}6P3/2​ atoms at 473 nm wavelength to be $2.28(\ifmmode\pm\else\textpm\fi{}0.33)\phantom{\rule{4pt}{0ex}}\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}21}\phantom{\rule{0.16em}{0ex}}{\mathrm{m}}^{2}$.