Laser Cooling of CaOH and CaOCH₃: Optical Cycling and Branching Ratios

Polyatomic molecules possess several unique features that have no direct analogues in atoms and can open new scientific possibilities in quantum simulation, ultracold chemistry, and precision measurements. Recent progress in laser cooling has brought several diatomic species into the ultracold regime via magneto-optical trapping (MOT) and sub-Doppler cooling. Here, we report on progress to extend these techniques to polyatomic molecules. Following our work creating a 1D MOT for CaOH, we now report white-light radiative slowing of a beam of CaOH, enabled by realizing a highly closed optical cycling scheme. Similarly, following our work on Sisyphus laser cooling of the symmetric top molecule CaOCH₃, we present progress towards radiative slowing and trapping of that species, and discuss the possibility of creating optical tweezer arrays of these and other, more complex, molecules.