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arXiv:physics/0403070 · Physical Review A

Improved efficiency of stimulated Raman adiabatic passage in photoassociation of a Bose-Einstein condensate

Matt Mackie, Kari Härkönen, Anssi Collin, Kalle‐Antti Suominen, Juha Javanainen

Published Jul 28, 2004• 39 citations
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Abstract

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.

DOI
10.1103/physreva.70.013614

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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.
Collective two-color photoassociation of a freely interacting 87Rb^{87}\mathrm{Rb}87Rb Bose-Einstein condensate is theoretically examined, focusing on stimulated Raman adiabatic passage (STIRAP) from an atomic to a stable molecular condensate. In particular, Drummond et al. [Phys. Rev. A. 65, 063619 (2002)] have predicted that particle-particle interactions can limit the efficiency of collective atom-molecule STIRAP, and that optimizing the laser parameters can partially overcome this limitation. We suggest that the molecular conversion efficiency can be further improved by treating the initial condensate density as an optimization parameter.
We analyze coherent two-color photoassociation of a Bose-Einstein condensate, focusing on stimulated Raman adiabatic passage (STIRAP) in free-bound-bound transitions from atoms to molecules. This problem raises an interest because STIRAP has been predicted to be absent in the nondegenerate case [Javanainen and Mackie, Phys. Rev. A 58, R789 (1998)]. Nevertheless, we find that Bose stimulation enhances the free-bound dipole matrix element for an atomic condensate, and photoassociative STIRAP turns out to be a viable mechanism for converting an atomic condensate to a molecular condensate with near-unit efficiency.
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.
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.
Although photoassociation and the Feshbach resonance are feasible means in principle for creating a molecular Bose–Einstein condensate (MBEC) from an already quantum-degenerate gas of atoms, collision-induced mean-field shifts and irreversible decay place practical constraints on the efficient Raman delivery of stable molecules. Focusing on stimulated Raman adiabatic passage, we propose that the efficiency of both mechanisms for producing a stable MBEC can be improved by treating the density of the initial atom condensate as an optimization parameter.
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.