Abstract
Optimal control theory (OCT) including nonresonant multiphoton transitions (NMT) in the femtosecond time regime has been implemented. The NMT process is modelled using an effective time-dependent Schrödinger equation, which considers a reduced space of the two levels which are involved in the transition, coupled to a density of high-lying off-resonant states. The specification of OCT to two-photon transitions is done within the rotating wave approximation. As an application, the transfer and displacement of a wavepacket in the organometallic system CpMn(CO)3, from the ground to an electronically excited state using two nonresonant photons, is simulated.
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