Production of ultracold CaCCH and SrCCH molecules by direct laser cooling: A theoretical study based on accurate ab initio calculations.

Laser cooling of polyatomic molecules to the ultracold regime may enable some new science and technology applications; however, the related study is still at its very early stage. Here, by means of accurate ab initio and dynamical calculations, we identify two new candidate tetratomic molecules that are suitable for laser cooling and demonstrate the feasibility and advantage of two laser cooling schemes that are able to produce ultracold CaCCH and SrCCH molecules. The internally contracted multiconfiguration reference configuration interaction method is applied, and excellent agreement is achieved between the computed and experimental spectroscopic data. We find that the XΣ →AΠ transitions for both candidates feature diagonal Franck-Condon factors, short radiative lifetimes, and no interference from intermediate electronic states. In addition, the crossings with higher electronic states do not interfere. We further construct feasible laser cooling schemes for CaCCH and SrCCH, each of which allows scattering 10 photons for direct laser cooling. The estimated Doppler temperatures for both CaCCH and SrCCH are on the order of μK.