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We show that weakly bound He-containing van der Waals molecules can beproduced and magnetically trapped in buffer-gas cooling experiments, andprovide a general model for the formation and dynamics of these molecules. Ouranalysis shows that, at typical experimental parameters, thermodynamics favorsthe formation of van der Waals complexes composed of a helium atom bound tomost open-shell atoms and molecules, and that complex formation occurs quicklyenough to ensure chemical equilibrium. For molecular pairs composed of a Heatom and an S-state atom, the molecular spin is stable during formation,dissociation, and collisions, and thus these molecules can be magneticallytrapped. Collisional spin relaxations are too slow to affect trap lifetimes.However, helium-3-containing complexes can change spin due to adiabaticcrossings between trapped and untrapped Zeeman states, mediated by theanisotropic hyperfine interaction, causing trap loss. We provide a detailedmodel for Ag3He molecules, using ab initio calculation of Ag-He interactionpotentials and spin interactions, quantum scattering theory, and direct MonteCarlo simulations to describe formation and spin relaxation in this system. Thecalculated rate of spin-change agrees quantitatively with experimentalobservations, providing indirect evidence for molecular formation inbuffer-gas-cooled magnetic traps.

Formation and dynamics of van der Waals molecules in buffer-gas traps