Electromagnetically induced transparency spectroscopy.

We propose a method based on the electromagnetically induced transparency (EIT) phenomenon for the detection of molecules which exist as a small minority in the presence of a majority of absorbers. The EIT effect we employ effectively eliminates the absorption of the majority species in the spectral region where it overlaps with the absorption of the minority species. The method can also be used to enhance local-modes transitions which overlap spectrally with a background of other local-modes transitions of the same molecule. The general theory is applied to the case of sparse and congested background spectra within the same molecule and to the recording of the spectra of isotopomers (of chlorine and methanol) that are in minority relative to other isotopomers which constitute the majority of molecules present.

Piecewise adiabatic population transfer in a molecule via a wave packet.

We propose a class of schemes for robust population transfer between quantum states that utilize trains of coherent pulses, thus forming a generalized adiabatic passage via a wave packet. We study piecewise stimulated Raman adiabatic passage with pulse-to-pulse amplitude variation, and piecewise chirped Raman passage with pulse-to-pulse phase variation, implemented with an optical frequency comb. In the context of production of ultracold ground-state molecules, we show that with almost no knowledge of the excited potential, robust high-efficiency transfer is possible.

Precise control of molecular dynamics with a femtosecond frequency comb.

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.