Precise control of molecular dynamics with a femtosecond frequency comb

Avi Pe'er, Evgeny A. Shapiro, Matthew C. Stowe, Moshe Shapiro, Jun Ye

Research output: Contribution to journalArticlepeer-review

76 Scopus citations


We present a general and highly efficient scheme for performing narrow-band Raman transitions between molecular vibrational levels using a coherent train of weak pump-dump pairs of shaped ultrashort pulses. The use of weak pulses permits an analytic description within the framework of coherent control in the perturbative regime, while coherent accumulation of many pulse pairs enables near unity transfer efficiency with a high spectral selectivity, thus forming a powerful combination of pump-dump control schemes and the precision of the frequency comb. Simulations verify the feasibility and robustness of this concept, with the aim to form deeply bound, ultracold molecules.

Original languageEnglish
Article number113004
JournalPhysical Review Letters
Issue number11
StatePublished - 16 Mar 2007
Externally publishedYes


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