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We present a general and highly efficient scheme for performing narrow-bandRaman transitions between molecular vibrational levels using a coherent trainof weak pump-dump pairs of shaped ultrashort pulses. The use of weak pulsespermits an analytic description within the framework of coherent control in theperturbative regime, while coherent accumulation of many pulse pairs enablesnear unity transfer efficiency with a high spectral selectivity, thus forming apowerful combination of pump-dump control schemes and the precision of thefrequency comb. The concept is presented analytically and its feasibility androbustness are verified by simulations of dynamics in Rb$_2$. We considerapplication of this concept to the formation of stable, deeply bound, ultracoldmolecules.Comment: 4+ pages, 3 figures, pacs correcte

Precise Control of Molecular Dynamics with a Femtosecond Frequency Comb