A novel method to determine the phase-space distribution of a pulsed molecular beam

We demonstrate a novel method to determine the longitudinal phase-space distribution of a cryogenic buffer gas beam of barium-fluoride molecules based on a two-step laser excitation scheme. The spatial resolution is achieved by a transversely aligned laser beam that drives molecules from the ground state $X^2\Sigma^+$ to the $A^2\Pi_{1/2}$ state around 860 nm, while the velocity resolution is obtained by a laser beam that is aligned counter-propagating with respect to the molecular beam and that drives the Doppler shifted $A^2\Pi_{1/2}$ to $D^2\Sigma^+$ transition around 797 nm. Molecules in the $D$-state are detected virtually background-free by recording the fluorescence from the $D-X$ transition at 413 nm. As molecules in the ground state do not absorb light at 797 nm, problems due to due to optical pumping are avoided. Furthermore, as the first step uses a narrow transition, this method can also be applied to molecules with hyperfine structure. The measured phase-space distributions, reconstructed at the source exit, show that the average velocity and velocity spread vary significantly over the duration of the molecular beam pulse. Our method gives valuable insight into the dynamics in the source and helps to reduce the velocity and increase the intensity of cryogenic buffer gas beams. In addition, transition frequencies are reported for the $X-A$ and $X-D$ transitions in barium fluoride with an absolute accuracy below 0.3 MHz.