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Recent theoretical investigations have indicated that rapid optical cyclingshould be feasible in complex polyatomic molecules with diverse constituents,geometries and symmetries. However, as a composite molecular mass grows, sodoes the required number of photon scattering events necessary to decelerateand confine molecular beams using laser light. Utilizing coherent momentumexchange between light fields and molecules can suppress spontaneous emissionand significantly reduce experimental complexity for slowing and trapping.Working with BaH as a test species, we have identified a robust, experimentallyviable configuration to achieve large molasses-like cooling forces formolecules using polychromatic optical fields addressing both $X-A$ and $X-B$electronic transitions, simultaneously. Using numerical solutions of thetime-dependent density matrix as well as Monte Carlo simulations, wedemonstrate that creation of Suppressed Emission Rate (SupER) molasses withlarge capture velocities ($\sim 40$ m/s) is generically feasible for polyatomicmolecules of increasing complexity that have an optical cycling center.Proposed SupER molasses are anticipated to not only extend quantum control tonovel molecular species with abundant vibrational decay channels, but alsosignificantly increase trapped densities for previously laser-cooled diatomicand triatomic species.

Large molasses-like cooling forces for molecules using polychromatic optical fields: A theoretical description