Vibrationally state-selective spin-orbit transfer with strong nonresonant pulses

J Phys Chem A. 2007 Apr 12;111(14):2670-8. doi: 10.1021/jp066825y. Epub 2007 Mar 20.

Abstract

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.