A quantum control of photodissocation of NaI to neutral atom fragments, NaI → NaI* → Na+I, was theoretically studied by using a locally optimized control method. The purpose of this control was to obtain as many neutral fragments as possible within one cycle of the nuclear vibration. The control was based on a pump-and-dump scheme. Weak and strong laser-field cases were used. The optimal dump pulses in both cases were shown to be of a linear time-dependent up-chirp type by analyzing their time- and frequency-resolved power spectra. This confirms the result predicted using a non-optimal control method in a previous paper (Chem. Phys. Lett., 231, 50 (1994)). The nuclear wavepacket propagations were also analyzed to see how photodissociation takes place when controlled pulses are used.
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