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

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 timescale. 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.