Electrically Dressed Ultralong-Range Polar Rydberg Molecules

Abstract

We investigate the impact of an electric field on the structure of ultralong-range polar diatomic Rydberg molecules. Both the s-wave and p-wave interactions of the Rydberg electron and the neutral ground state atom are taken into account. In the presence of the electric field the angular degree of freedom between the electric field and the internuclear axis acquires vibrational character and we encounter two-dimensional oscillatory adiabatic potential energy surfaces with an antiparallel equilibrium configuration. The electric field allows to shift the corresponding potential wells in such a manner that the importance of the p-wave interaction can be controlled and the individual wells are energetically lowered at different rates. As a consequence the equilibrium configuration and corresponding energetically lowest well move to larger internuclear distances for increasing field strength. For strong fields the admixture of non-polar molecular Rydberg states leads to the possibility of exciting the large angular momentum polar states via two-photon processes from the ground state of the atom. The resulting properties of the electric dipole moment and the vibrational spectra are analyzed with varying field strength.