Driving wave packet recurrences with optimally modulated laser pulses

In the weak-field limit, laser pulses optimized to induce vibrational wave packet recurrences in excited state potentials were calculated for Morse os cillators and for a real system [the X (1)Sigma(+) and A (3)Pi(1) states of IBr]. The performance of the optimized pulses was studied via simulated wa ve packet propagation. Such optimal light fields may be computationally gen erated given only the form of the electronic potential surfaces, knowledge of the particular ground state supplying population, and simple molecular c onstants. Thus it should be possible to use the modulation of light fields experimentally optimized to achieve recurrences in order to obtain substant ial information regarding previously uncharacterized potential surfaces in both diatomic and polyatomic molecules. Moreover, it should be possible to generalize this approach to the strong-field limit. (C) 2000 American Insti tute of Physics. [S0021-9606(00)00404-9].