Rovibrational optical pumping of a molecular beam

Cooling the rotation and the vibration of molecules by broadband light sources was possible for trapped molecular ions or ultracold molecules. Because of a low power spectral density, the cooling timescale has never fell below than a few milliseconds. Here we report on rotational and vibrational cooling of a supersonic beam of barium monofluoride molecules in less than 440 $\mu$s. Vibrational cooling was optimized by enhancing the spectral power density of a semiconductor light source at the underlying molecular transitions allowing us to transfer all the populations of $v''=1-3$ into the vibrational ground state ($v''=0$). Rotational cooling, that requires an efficient vibrational pumping, was then achieved. According to a Boltzmann fit, the rotation temperature was reduced by almost a factor of 10. In this fashion, the population of the lowest rotational levels increased by more than one order of magnitude.