The feasibility of a novel technique for efficient and selective population transfer from a thermally populated level 1 via an intermediate state 2 to level 3 is experimentally demonstrated. It is shown for sodium dimers that the process of on- or near-resonance stimulated Raman scattering with only partially overlapping laser beams is, in particular, useful for the selective population of high vibrational levels of particles in a molecular beam. This is achieved when the interaction with the Stokes laser, coupling levels 2 and 3, begins earlier than the interaction with the pump laser. The phenomenon, which is closely related to the formation of ‘‘trapped states,’’ is quantitatively explained using the basis of eigenstates of molecules strongly coupled to the radiation fields. The similarity and difference to related techniques such as rapid adiabatic passage phenomena in two-level systems, off-resonant stimulated Raman scattering, or stimulated emission pumping is briefly discussed.

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