Ultracold photoassociation is a process in which two cold atoms combine to form a molecule. This process is crucially dependent on the atom pair density at close distance termed the photoassociation window. We explore the possibilities for increasing the pair density at the photoassociation window by using a prepulse to accelerate the pairs of atoms at large interatomic separation toward each other. We show that the signal of a subsequent photoassociation pulse could be enhanced by a factor of one to two orders of magnitude with respect to the conventional continuous wave experiment. For neutral encounters on the ground potential surface which scales as $R^{-6}$ the acceleration becomes negligible. The electronic excited state potentials scale for homonuclear $S\to P$ transitions more favorably as $R^{-3}$. A possible pump-dump mechanism for acceleration, excites a pair of atoms at large distance employing the natural acceleration on the excited state. Then a dump pulse moves the population back to the ground surface. By controlling the phase and the amplitude of the light field this scenario can be optimized. In addition the momentum partitioned between the ground and excited surfaces can also be controlled. The possibility for pure quantum light-induced acceleration due to a gradient of the transition dipole is analyzed. Significant acceleration can be obtained only for pulses with intensities above ${10}^{14}\mathrm{W}∕{\mathrm{cm}}^2$ and pulse duration of $10\mathrm{ps}$.

• Received 30 April 2007

DOI:https://doi.org/10.1103/PhysRevA.76.053408