Ultralong-range polyatomic Rydberg molecules formed by a polar perturber

TL;DR

This paper explores the formation of ultralong-range polyatomic Rydberg molecules with giant electric dipole moments, achieved by coupling Rydberg states and utilizing avoided crossings for stable molecule creation.

Contribution

It introduces a new theoretical framework including additional Rydberg manifolds to predict and analyze the formation of giant polyatomic Rydberg molecules.

Findings

Pronounced avoided crossings in Born-Oppenheimer potentials.

Formation of stable polyatomic molecules via two-photon photoassociation.

Enhanced control over molecular properties through Rydberg state coupling.

Abstract

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.