New strategy for optimal control of femtosecond pump-dump processes applicable to systems of moderate complexity
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New pump-dump optimal control strategy applicable to the systems of moderate complexity has been developed which allows to drive the system to the desired objective in the ground state via electronically excited state. The strategy is based on the concept of the intermediate target in the excited state whose role is to select appropriate Franck-Condon window at a given time delay between pump and dump pulses in order to reach optimally the objective. The concept was applied on the isomerization process in Na3F2 employing our ab initio Wigner distribution approach. The pump and dump pulses have been found which suppress the radiationless transition through the conical intersection and drive the system via electronically excited state to the second isomer in the ground state with the maximal yield.
PACS.31.15.Qg Molecular dynamics and other numerical methods 31.15.Ar Ab initio calculations
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