The possibility of probing the collisions of aligned Rydberg atoms by stimulated emission is assessed with studies of a polarized state and a new measurement of a collisional alignment effect in atomic Ca. The stimulated emission method uses a laser to dump the desired state to a lower level which subsequently fluoresces. The technique can be used to obtain populations and polarization dependent information. First, the method is tested by applying it to an aligned Ca(4s17d¿1D2) state. Alignment curves are measured when the initial state is prepared with both parallel and perpendicular relative polarizations. The experimentally observed alignment compares well with that derived from theoretical considerations of a saturated stimulated transition. Second, a two-vector collisional alignment experiment (initial state and relative velocity vector) is performed to study the energy transfer process Ca(4s7d¿1D2)+He¿Ca(4s6f¿1F3)+He+¿E=17.7 cm-1, and alignment effects are measured by both stimulated emission and conventional direct fluorescence detection. A preference for the ¿m¿=1 and 2 initial states is observed in the relative cross sections. Essentially identical data are obtained with the two detection methods when elliptically polarized light is used for the stimulated emission detection method. The stimulated emission technique can provide alignment and population information of the final states, making it an excellent new tool for both three-vector correlation experiments and state-to-state Rydberg transitions.
Spain, E. M., Dalberth, M. J., Kleiber, P. D., Leone, S. R., Op De Beek, S. S., & Driessen, J. P. J. (1996). Alignment probing of Rydberg states by stimulated emission. Journal of Chemical Physics, 102(24), 9522-9531. https://doi.org/10.1063/1.468767