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Magneto-optical trapping (MOT) is a key technique on the route towardsultracold molecular ensembles. However, the realization and optimization ofmagneto-optical traps with their wide parameter space is particularlydifficult. Here, we present a very general method for the optimization ofmolecular magneto-optical trap operation by means of Bayesian optimization(BO). As an example for a possible application, we consider the optimization ofa calcium fluoride (CaF) MOT for maximum capture velocity. We find that boththe $X^2\Sigma^+\,$ to $A^2\Pi_{1/2}\,$ and the $X^2\Sigma^+\,$ to$B^2\Sigma^+\,$ transition to allow for capture velocities larger than $20$ m/swith $24$ m/s and $23$ m/s respectively at a total laser power of $200$ mW. Inour simulation, the optimized capture velocity depends logarithmically on thebeam power within the simulated power range of $25$ to $400$ mW. Applied toheavy molecules such as BaH and BaF with their low capture velocity MOTs itmight offer a route to far more robust magneto-optical trapping.

Maximizing the capture velocity of molecular magneto-optical traps with Bayesian optimization