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Physical Review A

Multimode model of the formation of molecular Bose-Einstein condensates by Bose-stimulated Raman adiabatic passage

J. J. Hope, M. K. Olsen, Lev I. Plimak

Published Mar 12, 2001• 49 citations
Publisher

Abstract

We investigate the conversion of a Bose-Einstein condensate (BEC) of a weakly interacting gas into a molecular BEC (MBEC) by Bose-stimulated Raman adiabatic passage (STIRAP). This method of producing an MBEC does not experience large spontaneous losses while the condensate is in an excited electronic state, and it is robust with respect to small changes in the physical parameters. We show that the atomic interactions affect the quantum statistics of the resulting field, although they do not interfere with the production of the MBEC. We demonstrate that STIRAP is still feasible when we include the spatial degrees of freedom that cause the Bose-enhanced coupling rate to vary across the condensate. The complete conversion is destroyed by spatial effects unless the time scale of the coupling is much faster than the propagation time, which in practice requires submillisecond conversion.

DOI
10.1103/physreva.63.043603

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We investigate the conversion of a Bose-Einstein condensate (BEC) of a weakly interacting gas into a molecular BEC (MBEC) by Bose-stimulated Raman adiabatic passage (STIRAP). This method of producing an MBEC does not experience large spontaneous losses while the condensate is in an excited electronic state, and it is robust with respect to small changes in the physical parameters. We show that the atomic interactions affect the quantum statistics of the resulting field, although they do not interfere with the production of the MBEC. We demonstrate that STIRAP is still feasible when we include the spatial degrees of freedom that cause the Bose-enhanced coupling rate to vary across the condensate. The complete conversion is destroyed by spatial effects unless the time scale of the coupling is much faster than the propagation time, which in practice requires submillisecond conversion.
The process of stimulated Raman adiabatic passage (STIRAP) provides a possible route for the generation of a coherent molecular Bose-Einstein condensate (BEC) from an atomic BEC. We analyze this process in a three-dimensional mean-field theory, including atom-atom interactions and nonresonant intermediate levels. We find that the process is feasible, but at larger Rabi frequencies than anticipated from a crude single-mode lossless analysis, due to two-photon dephasing caused by the atomic interactions. We then identify optimal strategies in STIRAP allowing one to maintain high conversion efficiencies with smaller Rabi frequencies and under experimentally less demanding conditions.
We theoretically examine Raman photoassociation of a Bose-Einstein condensate, revisiting stimulated Raman adiabatic passage (STIRAP). Due to collisional mean-field shifts, efficient molecular conversion requires strong coupling and low density, either of which can bring about rogue photodissociation to noncondensate modes. We demonstrate explicitly that rogue transitions are negligible for low excited-state fractions and photodissociation that is slower than the STIRAP time scale. Moreover, we derive a reduced-parameter model of collisions, and thereby find that a gain in the molecular conversion efficiency can be obtained by adjusting the atom-atom scattering length with off-resonant magnetoassociation. This gain saturates when the atom-atom scattering length is tuned to a specific fraction of either the molecule-molecule or atom-molecule scattering length. We conclude that a fully optimized STIRAP scheme may offer the best chance for achieving coherent conversion from an atomic to a molecular condensate with photoassociation.
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.
The adiabaticity of the stimulated Raman adiabatic passage (STIRAP) for the 87Rb atom–molecule conversion in a condensate system is investigated in terms of a newly defined adiabatic fidelity. The evolution of the dark state in the STIRAP is simulated numerically by considering the interparticle interactions and spontaneous emissions of the excited molecular state. We find that these terms will reduce the adiabatic fidelity; however, one can still achieve higher adiabatic fidelity through optimizing the external parameters of the STIRAP. Our discussions are helpful in obtaining higher conversion efficiency from an atomic Bose–Einstein condensate to its molecular counterpart in experiment.
We produce 84 Sr 2 molecules using Bose-enhanced Raman photoassociation. We apply the stimulated Raman adiabatic passage (STIRAP) technique on a Bose-Einstein condensate (BEC) to produce more than 8 × 10 3 ultracold molecules. This chemical reaction is only made possible because of the Bose enhancement of the optical transition dipole moment between the initial atomic state and an intermediate molecular state. We study the effect of Bose enhancement by measuring the transition Rabi frequency in a BEC and by comparing it with measurements for two atoms in sites of a Mott insulator. By breaking the dimers' bond and directly observing the separated atoms, we measure the molecular inelastic collision rate parameters. We discuss the possibility of applying Bose-enhanced STIRAP to convert a BEC of atoms into a BEC of molecules, and argue that the required efficiency for STIRAP is within experimental reach.
Ultracold atoms in the atomic Bose-Einstein condensate (ABEC) state can form molecular Bose-Einstein condensate (MBEC) through photoassociation.In the atom-molecule Bose-Einstein condensates (BECs), two or more atoms in the ABEC can combine to form a molecule in the MBEC and again a molecule from a MBEC can decompose to atoms in the ABEC.The Bose-stimulated Raman adiabatic passage is an efficient mechanism for conversion of an atomic BEC to a molecular BEC.A three-mode atom-molecule Bose-Einstein condensates system can be prepared through the photoassociative Bose-stimulated Raman adiabatic passage.In our system, three modes are one ABEC, one excited MBEC, and one stable MBEC.The intramodal interactions due to the  (3) nonlinearity is present in all three BEC modes along with ABEC-excited MBEC and excited MBEC-stable MBEC intermodal couplings.The quantum mechanical Hamiltonian of the system is constructed considering all three intraspecies interactions and intermodal couplings among the modes.The Hamiltonian of the system is solved analytically using a special intuitive approach which is more general and gives more accurate result than the well-known short time approximation method.The correctness of the solution is verified through the equal time commutation relation.Staring from a three-mode composite coherent state we compute the time evolution of the field annihilation operators of all three modes in presence of all possible interactions and couplings.Using these solutions, we investigate the quantum entanglement properties of the system for all three two-mode combinations.Entanglement is found for two combinations of modes, where as one combination is always separable.Also, we study the dependence of the entanglement properties of the system with the interaction and coupling constants.