Theory of coherent photoassociation of a Bose-Einstein condensate

We study coherent photoassociation, phenomena analogous to coherent optical transients in few-level systems, which may take place in photoassociation of an atomic Bose-Einstein condensate but not in a nondegenerate gas. We develop a second-quantized Hamiltonian to describe photoassociation, and apply the Hamiltonian both in the momentum representation and in the position representation (field theory). Solution of the two-mode problem including only one mode each for the atomic and molecular condensates displays analogs of Rabi oscillations and rapid adiabatic passage. A classical version of the field theory for atoms and molecules is used to demonstrate that, in the presence of photoassociating light, a joint-atom molecule is unstable against growth of density fluctuations. Experimental complications, including spontaneous emission and unwanted "rogue" photodissociation from a photoassociated molecule are analyzed. A two-color Raman scheme is studied as a method to set up an effective two-mode scheme with reduced spontaneous emission losses. We discuss photoassociation rates and photoassociation Rabi frequencies for high-lying vibrational states in alkalis both on the basis of molecular-structure calculations, and by comparing with an experiment [Wynar et al., Science 287, 1016 (2000)].