Elucidating the roles of collision energy and photon momentum transfer in the formation of ultralong-range Rydberg molecules

Spectroscopic measurements of the rotational distribution of $^{84}\mathrm{Sr}$ and $^{86}\mathrm{Sr}\phantom{\rule{4pt}{0ex}}\phantom{\rule{0.16em}{0ex}}5sns{\phantom{\rule{0.16em}{0ex}}}^{1}{S}_{0}$ ultralong-range Rydberg molecular dimers created via photoassociation in a cold gas are reported. The dimers are produced by two-photon excitation via the $5s5p$ $^{1}P_{1}$ intermediate state. The use of singlet states permits detailed study of the roles that the initial atom-atom interaction, photon momentum transfer during Rydberg excitation, and sample temperature play in determining the spectral line shape and final dimer rotational distribution. The results are in good agreement with the predictions of a model that includes these effects. The present work further highlights the sensitivity of ultralong-range Rydberg molecule formation to the state of the initial cold gas.