Photoassociation dynamics controlled by a spectral π-jump laser pulse

The formation of ultracold Cs2 molecules via photoassociation (PA) with a spectral π-jump laser pulse is theoretically investigated by solving the time-dependent Schrodinger equation using the mapped Fourier grid method. Numerical calculations show that the population distributions of associated molecules mainly result from the off-resonant excitation of the π-jump laser pulse. Compared with the transform-limited pulse, an efficient population accumulation in the PA process is achieved with the π-jump pulse. An oscillation pattern appears in the population on the vibrational levels of the state owing to the action of the post-half-pulse in the π-jump pulse. The PA efficiency is related to the Rabi angle of the laser pulse. A π-jump pulse can be used to enhance more effectively the PA efficiency than a transform-limited pulse with the same Rabi angle.