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We propose a method of stimulated laser decelerating of diatomic molecules by counter-propagating π-trains of ultrashort laser pulses. The decelerating cycles occur on the rovibrational transitions inside the same ground electronic manifold, thus avoiding the common problem of radiative branching in Doppler cooling of molecules. By matching the frequency comb spectrum of the pulse trains to the spectrum of the R-branch rovibrational transitions we show that stimulated deceleration can be carried out on several rovibrational transitions simultaneously. This enables an increase in the number of cooled molecules with only a single laser source. The exerted optical force does not rely on the decay rates in a system and can be orders of magnitude larger than the typical values of scattering force obtained in conventional Doppler laser cooling schemes.

Stimulated deceleration of diatomic molecules on multiple rovibrational transitions with coherent pulse trains