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The internal electric field of a Rydberg atom electron can bind a polarmolecule to form a giant ultralong-range stable polyatomic molecule. Suchmolecules not only share their properties with Rydberg atoms, they possess hugepermanent electric dipole moments and in addition allow for coherent control ofthe polar molecule orientation. In this work, we include additional Rydbergmanifolds which couple to the nearly degenerate set of Rydberg states employedin [S. T. Rittenhouse and H. R. Sadeghpour, Phys. Rev. Lett. 104, 243002(2010)]. The coupling of a set of $(n+3)s$ Rydberg states with the $n(l>2)$nearly degenerate Rydberg manifolds in alkali metal atoms leads to pronouncedavoided crossings in the Born-Oppenheimer potentials. Ultimately, these avoidedcrossings enable the formation of the giant polyatomic Rydberg molecules withstandard two-photon laser photoassociation techniques.

Ultralong-range polyatomic Rydberg molecules formed by a polar perturber