We present an optimal control approach to the process of molecular isotope separation by exciting vibrational wave packets with femtosecond laser pulses. In the weak-field limit, we developed an optimization procedure for designing shaped laser pulses leading to the best selectivity in the two-photon ionization processes. Several control scenarios are identified, which mainly belong to two groups. The first takes advantage of the revival phenomenon, which allows one to find times at which excited wave packets of different isotopes are well localized and spatially separated in the intramolecular space. The second is based on isotopically selective quantum interference between several wave packets excited in the same molecular potential by a designed sequence of laser pulses. Simulations have been done for the isotopic mixture of ⁷⁹Br₂ and ⁸¹Br₂ molecules, which was used in the first experiments on wave-packet isotope separation.
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Leibscher et al. (2001) studied this question.
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