We consider the formation of cold ground-state polar molecules in a low vibrational level by laser fields. Starting from a pair of cold colliding atoms of dissimilar species, we propose a strategy consisting of three steps. In the first step, a pump pulse induces the molecule formation by photoassociating the atomic pair in a high or intermediate vibrational level of an excited electronic molecular state. This step is followed by a dump pulse in an intermediate vibrational level of the ground state. The last step corresponds to the vibrational cooling or vibrational stabilization process. Taking advantage of the permanent dipole moment, an infrared chirped pulse induces downward transitions among the vibrational levels of the ground electronic state, reaching the ground vibrational level. We perform the strategy with with fixed-shaped pulses and also with an optimized chirped pulse for the stabilization step. To perform the optimization, we introduce an optimal control technique in which the optimization of the chirping is carried out in the time domain. This methodology has the benefit of limiting the pulse amplitude while focusing only on the frequency of the field. The proposed scheme is an alternative to the use of two pairs of pump-dump pulses or to the direct photoassociation and vibrational stabilization in the ground state.
Local control theory (LCT) is employed to achieve molecular photoassociation with shaped laser pulses. Within LCT, the control fields are constructed from the response of the system to the perturbation which makes them accessible to a straightforward interpretation. This is shown regarding the ground-state collision of H+F and H+I atoms. Different objectives are defined, which aim at the formation of vibrational cold or hot associated molecules, respectively. Results are presented for s-wave scattering, where the rotational degree of freedom is ignored and also for full scale calculations including rotations, in order to describe more realistic conditions.
In recent experiments on ultracold matter, molecules have been produced from ultracold atoms by photoassociation, Feshbach resonances, and three-body recombination. The created molecules are translationally cold, but vibrationally highly excited. This will eventually lead them to be lost from the trap due to collisions. We propose shaped laser pulses to transfer these highly excited molecules to their ground vibrational level. Optimal control theory is employed to find the light field that will carry out this task with minimum intensity. We present results for the sodium dimer. The final target can be reached to within
99 provided the initial guess field is physically motivated. We find that the optimal fields contain the transition frequencies required by a good Franck-Condon pumping scheme. The analysis identifies the ranges of intensity and pulse duration which are able to achieve this task before any other competing processes take place. Such a scheme could produce stable ultracold molecular samples or even stable molecular Bose-Einstein condensates.