Isotopologue-selective laser cooling of molecules

Direct laser cooling of molecules has made significant progress in recent years. However, the selective cooling and manipulation of molecules based on their isotopic composition, which is ubiquitous in atomic laser cooling, has not yet been achieved. Here, we demonstrate such isotopologue-selective laser cooling of molecules, using barium monofluoride (BaF) as an example. The manipulation of the rare and previously uncooled 136BaF is achieved within a molecular beam containing several isotopologues of significantly higher natural abundance. Our results enable intense molecular beams and high fidelity detection of select low-abundance isotopologues or isotopic mixtures. Such beams are a first step towards isotopologue-selective molecular trapping and will be useful for applications in trace gas analysis, cold chemistry and precision tests of fundamental symmetries.