Optical cycling of MgF molecules within the hyperfine states in X(N=1) state.

Achieving laser cooling of molecules necessitates the establishment of a closed optical cycling transition. In contrast to atoms, molecules exhibit additional vibrational and rotational structures, which must be carefully addressed-alongside hyperfine splittings-when designing the laser frequency scheme for efficient optical cycling. In this work, we investigated optical cycling in MgF molecules on the laser cooling transition, namely [Formula: see text] transition between the electronic ground state ([Formula: see text]) and the electronic excited state ([Formula: see text]). The ground state comprises four hyperfine levels, of which two are unresolved within the excited-state linewidth; the two hyperfine levels in the excited state are also unresolved. Consequently, three laser frequencies suffice to address all transitions. This was realized by generating three independently tunable frequency components using acousto-optic modulators (AOMs). With optimized detunings, power ratios, and total beam power, simultaneous application of all three frequency components increased the total number of scattered photons by up to [Formula: see text] relative to the sum of the individual single-frequency signals. Applying a tilted magnetic field to remix the dark Zeeman states increased the photon yield by an additional factor of [Formula: see text], leading to an overall enhancement of about sevenfold. These results provide quantitative benchmarks for MgF optical cycling and practical guidance for future molecular slowing and magneto-optical trapping experiments.