Vibrationally State-Selective Spin−Orbit Transfer with Strong Nonresonant Pulses

By dynamic Stark shift using strong nonresonant pulses, we show that it is in principle possible to prepare arbitrary superposition states of mixed multiplicity. By a proper choice of parameters, the transfer of population is shown to follow the Rabi formula, where the initial and target states are now vibrational states of two light-induced molecular potentials of different multiplicity. Starting from nonstationary wave packets, the spin transfer can proceed via parallel transfer using a single pulse or by sequential transfer using a pulse sequence. A simple model is proposed to analyze the properties of both schemes and the feasibility of their experimental implementation for spin-orbit transitions in Rb2.