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Phys Rev Lett. 2007 Mar 16;98(11):113004. Epub 2007 Mar 16.

Precise control of molecular dynamics with a femtosecond frequency comb.

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JILA, National Institute of Standards and Technology, University of Colorado, Boulder, Colorado 80309-0440, USA.


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.

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