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Ultralong-range polyatomic Rydberg molecules formed by a polar perturber

The internal electric field of a Rydberg atom electron can bind a polar molecule to form a giant ultralong-range stable polyatomic molecule. Such molecules not only share their properties with Rydberg atoms, they possess huge permanent electric dipole moments and in addition allow for coherent control of the polar molecule orientation. In this work, we include additional Rydberg manifolds which couple to the nearly degenerate set of Rydberg states employed in [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 pronounced avoided crossings in the Born-Oppenheimer potentials. Ultimately, these avoided crossings enable the formation of the giant polyatomic Rydberg molecules with standard two-photon laser photoassociation techniques.