Laser cooling of molecules with complex hyperfine structure

An important effort is currently underway to extend optical cycling and laser cooling to more molecular species. While established methods exist for addressing molecular vibrations and rotations, substantial challenges remain when multiple nuclear spins in the molecules lead to a complex, resolved hyperfine structure. This is particularly relevant for many molecular species considered for precision tests of fundamental symmetries, as well as for most fermionic diatomics. In this talk, I will provide a detailed introduction to the use of optical spectra generated via serrodyne waveforms to address this complexity. I will discuss our experimental implementation of these serrodynes, characterize their properties, and outline procedures to find optimized sideband configurations that generate strong laser cooling forces. I will present experiments demonstrating the application of these techniques to various isotopologues of barium monofluoride and explore their prospects for the cooling of other species relevant to the study of fundamental symmetries.