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arXiv:cond-mat/0110565 · Physical Review Letters

Superchemistry: Dynamics of Coupled Atomic and Molecular Bose-Einstein Condensates

Daniel J. Heinzen, R. H. Wynar, P. D. Drummond, Karen V. Kheruntsyan

Published May 29, 2000• 335 citations
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Abstract

We analyze the dynamics of a dilute, trapped Bose-condensed atomic gas coupled to a diatomic molecular Bose gas by coherent Raman transitions. This system is shown to result in a new type of "superchemistry," in which giant collective oscillations between the atomic and the molecular gas can occur. The phenomenon is caused by stimulated emission of bosonic atoms or molecules into their condensate phases.

DOI
10.1103/physrevlett.84.5029

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We analyze the dynamics of a dilute, trapped Bose-condensed atomic gas coupled to a diatomic molecular Bose gas by coherent Raman transitions. This system is shown to result in a new type of "superchemistry," in which giant collective oscillations between the atomic and the molecular gas can occur. The phenomenon is caused by stimulated emission of bosonic atoms or molecules into their condensate phases.
Summary form only given. Coherent conversion of an atomic to a molecular Bose-Einstein condensate (BEC) is a first step towards 'superchemistry', which is the atom optics analog of frequency conversion in nonlinear optics. A number of studies of this have shown that direct conversion via Raman photo-association appears feasible, based on stimulated free-bound and bound-bound transitions in the presence of two laser fields E/sup (1)/=E/sub 0//sup (1)/ cos(/spl omega//sup (1)/t) and E/sup (2)/=E/sub 0//sup (2)/ cos(/spl omega//sup (2)/t). Here pairs of atoms from the two-atom continuum are transferred-via an excited bound molecular state-to a bound molecular state of lower energy. Raman photo-association allows coupling to a single molecular state, which can be selected by the Raman laser frequencies /spl omega//sup (1)/ and /spl omega//sup (2)/. However, practical calculations using available lasers and transitions indicate that coherent transfer is often limited by spontaneous emission from the intermediate molecular excited electronic state. A possible route towards minimizing losses and decoherence from spontaneous emission is to use the stimulated Raman adiabatic passage (STIRAP) method (Drummond et al, Phys. Rev. Lett. vol. 81, p. 3055, 1998) in which a counter-intuitive pulse sequence is used where the first input pulse couples the molecular levels, even when there are no molecules present.
We show that a molecular Bose-Einstein condensate in a trap is stabilized against stimulated dissociation if the trap size is smaller than the resonance healing length (Planck's 2/2mgsqrt[n]);1/2. The condensate shape determines the critical atom-molecule coupling frequency. We discuss an experiment for triggering dissociation by a sudden change of coupling or trap parameters. This effect demonstrates one of the unique collective features of "superchemistry" in that the yield of a chemical reaction depends critically on the size and shape of the reaction vessel.
We study the dynamics of the atomic and molecular Bose-Einstein condensates (BECs) of 87Rb^{87}\text{R}\text{b}87Rb in a spherically symmetric trap coupled by stimulated Raman photoassociation process. Considering the higher order nonlinearity in the atom-atom interaction we analyze the dynamics of the system using coupled modified Gross-Pitaevskii (MGP) equations and compare it with mean-field coupled Gross-Pitaevskii (GP) dynamics. Considerable differences in the dynamics are obtained in these two approaches at large scattering length, i.e., for large values of peak-gas parameter ${x}_{pk}\ensuremath{\ge}{10}^{\ensuremath{-}3}$. We show how the dynamics of the coupled system is affected when the atom-molecule and molecule-molecule interactions are considered together with the atom-atom interaction and also when the strengths of these three interactions are increased. The effect of detuning on the efficiency of conversion of atomic fractions into molecules is demonstrated and the feasibility of maximum molecular BEC formation by varying the Raman detuning parameter at different values of time is explored. Thus by varying the Raman detuning and the scattering length for atom-atom interaction one can control the dynamics of the coupled atomic-molecular BEC system. We have also solved coupled Gross-Pitaevskii equations for atomic to molecular condensate formation through magnetic Feshbach resonance in a BEC of 85Rb^{85}\text{R}\text{b}85Rb. We found similar features for oscillations between atomic and molecular condensates noted in previous theoretical study and obtained fairly good agreement with the evolution of total atomic condensate observed experimentally.
We analyze the coherent multimode dynamics of a system of coupled atomic and molecular Bose gases. Starting from an atomic Bose-Einstein condensate with a small thermal component, we observe a complete depletion of the atomic and molecular condensate modes on a short time scale due to a significant population of excited states. Giant coherent oscillations between the two condensates for typical parameters are almost completely suppressed. Our results cast serious doubts on the common use of the 2-mode model for the description of coupled ultracold atomic-molecular systems and should be considered when planning future experiments with ultracold molecules.
Abstract Recent advances in the precise control of ultracold atomic systems have led to the realisation of Bose–Einstein condensates (BECs) and degenerate Fermi gases. An important challenge is to extend this level of control to more complicated molecular systems. One route for producing ultracold molecules is to form them from the atoms in a BEC. For example, a two-photon stimulated Raman transition in a 87Rb BEC has been used to produce 87Rb2 molecules in a single rotational-vibrational state1, and ultracold molecules have also been formed2 through photoassociation of a sodium BEC. Although the coherence properties of such systems have not hitherto been probed, the prospect of creating a superposition of atomic and molecular condensates has initiated much theoretical work3, 4, 5, 6, 7. Here we make use of a time-varying magnetic field near a Feshbach resonance8, 9, 10, 11, 12 to produce coherent coupling between atoms and molecules in a 85Rb BEC. A mixture of atomic and molecular states is created and probed by sudden changes in the magnetic field, which lead to oscillations in the number of atoms that remain in the condensate. The oscillation frequency, measured over a large range of magnetic fields, is in excellent agreement with the theoretical molecular binding energy, indicating that we have created a quantum superposition of atoms and diatomic molecules—two chemically different species.