Cavity cooling of translational and ro-vibrational motion of molecules: ab initio-based simulations for OH and NO

We present detailed calculations at the basis of our recent proposal for simultaneous cooling the rotational, vibrational and external molecular degrees of freedom. In this method, the molecular rovibronic states are coupled by an intense laser and an optical cavity via coherent Raman processes enhanced by the strong coupling with the cavity modes. For a prototype system, OH, we showed that the translational motion is cooled to few micro Kelvin and the molecule is brought to the internal ground state in about a second. Here, we investigate numerically the dependence of the cooling scheme on the molecular polarizability, selecting NO as a second example. Furthermore, we demonstrate the general applicability of the proposed cooling scheme to initially vibrationally and rotationally hot molecular systems.