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arXiv:0801.4804 · Physical Review Letters

Inelastic Collisions of Ultracold Heteronuclear Molecules in an Optical Trap

Eric R. Hudson, Nathan Gilfoy, Svetlana Kotochigova, Jeremy Sage, David P. DeMille

Published May 20, 2008• 119 citations
arXivHTMLPDF

Abstract

Ultracold RbCs molecules in high-lying vibrational levels of the a3Sigma+ ground electronic state are confined in an optical trap. Inelastic collision rates of these molecules with both Rb and Cs atoms are determined for individual vibrational levels, across an order of magnitude of binding energies. The long-range dispersion coefficients for the collision process are calculated and used in a model that accurately reproduce the observed scattering rates.

DOI
10.1103/physrevlett.100.203201

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Ultracold RbCs molecules in high-lying vibrational levels of the a3Sigma+ ground electronic state are confined in an optical trap. Inelastic collision rates of these molecules with both Rb and Cs atoms are determined for individual vibrational levels, across an order of magnitude of binding energies. The long-range dispersion coefficients for the collision process are calculated and used in a model that accurately reproduce the observed scattering rates.
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.
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.
The production and research of ultracold heteronuclear molecules have aroused the great interest recently. On the one hand, these molecules are extremely popular in experiments for exploring the collision dynamic behaviors in threshold, photoassociative spectrum and strong dipole-dipole interactions. On the other hand, ultracold polar molecules populated at deeply bound levels in the singlet ground state are the right candidates to investigate quantum memories for quantum simulation, and to study strongly interacting quantum degenerate gases. The precise knowledge of cold collision processes between two different types of alkali atoms is necessary for understanding and utilizing ultracold heteronuclear molecules, sympathetic cooling, and thus formation of two species BEC. The goal of the present investigation is to study the collisions between ultracold sodium atoms and cesium atoms. We systematically demonstrate simultaneously trapping ultracold sodium and cesium atoms in a dual-species magneto-optical trap (MOT). The sodium atom trap loss rate coefficient Na-Cs is measured as a function of Na trapping laser intensity. At low intensities, the trap loss is dominated by ground-state hyperfine-changing collisions, while at high intensities, collisions involving excited atoms are more important. A strong interspecies collision-induced loss for Na atoms in the MOT is observed. In order to obtain the trap loss coefficient Na-Cs, we proceed in two steps. First, the Cs repumping laser is blocked to avoid the formation of ultraold Cs atoms. The loading process of Na atoms is recorded when the Cs trapping laser is on. Second, the loading curves of the Na atoms are obtained as Cs atoms are present with the repumping laser beams. The total losses PNa and PNa' are acquired by fitting the two loading curves of trapped Na atoms. Thus, the trap loss coefficient Na-Cs can be derived from the difference between total losses PNa and PNa' divided by the density of the Cs atoms. The coefficient Na-Cs decreases in a range of 5-10mW/cm2, which originates from the hyperfine-state changing (HFC) collision. A Doppler model is used to calculate the Na atom trap depth, in that the atom trap depth and exoergic energy determine the behavior of the collisional trap loss rate coefficient. The three corresponding calculated critical intensities of Na trapping laser are 7.98, 14.82, 16.2 mW/cm2 respectively in the Na-Cs HFC collision process. The first calculated critical intensity value agrees well with the experimental result. Our work provides a valuable insight into HFC collision between Na and Cs atoms and also paves the way for the production of ultracold NaCs molecules using Photoassociation (PA) technology. Furthermore, the experimental results lay a great basis for the obtainments of high sensitive heteronuclear NaCs molecular PA spectrum and the creation of deeply bound ground state molecules.
The formation of ultracold metastable RbCs molecules is observed in a double species magneto-optical trap through photoassociation below the 85 Rb(5S 1/2 ) + 133 Cs(6P 3/2 ) dissociation limit followed by spontaneous emission. The molecules are detected by resonance enhanced two-photon ionization. Using accurate quantum chemistry calculations of the potential energy curves and transition dipole moment, we interpret the observed photoassociation process as occurring at short internuclear distance, in contrast with most previous cold atom photoassociation studies. The vibrational levels excited by photoassociation belong to the 5th 0 + or the 4th 0 − electronic states correlated to the Rb(5P 1/2, 3/2 ) + Cs(6S 1/2 ) dissociation limit. The computed vibrational distribution of the produced molecules shows that they are stabilized in deeply bound vibrational states of the lowest triplet state. We also predict that a noticeable fraction of molecules is produced in the lowest level of the electronic ground state.
Universal collisions describe the reaction of molecules and atoms as dominated by long-range interparticle interactions. Here, we calculate the universal inelastic rate coefficients for a large group of ultracold polar molecules in their lower ro-vibrational states colliding with one of their constituent atoms. The rate coefficients are solely determined by values of the dispersion coefficient and reduced mass of the collisional system. We use the ab initio coupled-cluster linear response method to compute dynamic molecular polarizabilities and obtain the dispersion coefficients for some of the collisional partners and use values from the literature for others. Our polarizability calculations agree well with available experimental measurements. Comparison of our inelastic rate coefficients with results of numerically exact quantum-mechanical calculations leads us to conjecture that collisions with heavier atoms can be expected to be more universal.