Coherent optical bichromatic forces have been shown to be effective tools for rapidly slowing and cooling simple atomic systems. While previous estimates suggest that these forces may also be effective for rapidly decelerating molecules or complex atoms, a quantitative treatment for multilevel systems has been lacking. We describe detailed numerical modeling of bichromatic forces by direct numerical solution for the time-dependent density matrix in the rotating-wave approximation. We describe both the general phenomenology of an arbitrary few-level system and the specific requirements for slowing and cooling on a many-level transition in calcium monofluoride (CaF), one of the molecules of greatest current experimental interest. We show that it should be possible to decelerate a cryogenic buffer-gas-cooled beam of CaF nearly to rest without a repumping laser and within a longitudinal distance of about 1 cm. We also compare a full 16-level simulation for the CaF $B\leftrightarrow X$ system with a simplified numerical model and with a semiquantitative estimate based on two-level systems. The simplified model performs nearly as well as the complete version, whereas the two-level model is useful for making order-of-magnitude estimates, but nothing more.

• Received 11 September 2015

DOI:https://doi.org/10.1103/PhysRevA.93.013419