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Molecular Physics

How do ultralong-range homonuclear Rydberg molecules get their permanent dipole moments?

H. R. Sadeghpour, Seth T. Rittenhouse

Published Jun 28, 2013• 12 citations
Publisher

Abstract

Cold and ultracold Rydberg atoms are in considerable vogue for their ability to creating strong interactions, stemming from their exaggerated and readily tunable properties. Ultralong-range Rydberg molecules have been predicted to form from the interaction of ultracold Rydberg atoms with ground-state atoms and polar molecules. In this work, we discuss and demonstrate how such molecules, which are homonuclear, form substantially large permanent electric dipole moments. A corollary benefit of such strong hybridisation is the realisation of high angular momentum degenerate Rydberg molecules (so-called trilobite molecules) with standard photoassociation techniques.

DOI
10.1080/00268976.2013.811555

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Cold and ultracold Rydberg atoms are in considerable vogue for their ability to creating strong interactions, stemming from their exaggerated and readily tunable properties. Ultralong-range Rydberg molecules have been predicted to form from the interaction of ultracold Rydberg atoms with ground-state atoms and polar molecules. In this work, we discuss and demonstrate how such molecules, which are homonuclear, form substantially large permanent electric dipole moments. A corollary benefit of such strong hybridisation is the realisation of high angular momentum degenerate Rydberg molecules (so-called trilobite molecules) with standard photoassociation techniques.
Permanent electric dipole moments are important for understanding symmetry breaking in molecular physics, control of chemical reactions, and realization of strongly correlated many-body quantum systems. However, large molecular permanent electric dipole moments are challenging to realize experimentally. We report the observation of ultralong-range Rydberg molecules with bond lengths of ~100 nanometers and kilo-Debye permanent electric dipole moments that form when an ultracold ground-state cesium (Cs) atom becomes bound within the electronic cloud of an extended Cs electronic orbit. The electronic character of this hybrid class of "trilobite" molecules is dominated by degenerate Rydberg manifolds, making them difficult to produce by conventional photoassociation. We used detailed coupled-channel calculations to reproduce their properties quantitatively. Our findings may lead to progress in ultracold chemistry and strongly correlated many-body physics.
Ultra-cold long-range Rydberg-ground molecule consisting of a Rydberg atom and one or more ground-state atoms is formed by low-energy scattering between the Rydberg electron and ground-state atoms located inside the Rydberg electron’s wave function. The low-energy scattering interaction, initially investigated by Fermi and Omont, has been predicted to lead to molecular binding in a novel type of Rydberg molecules, including the trilobite and butterfly molecules. Their unconventional binding mechanism, which is unlike covalent, or ionic, or van der Waals bonds, results in loosely bound molecules with bond lengths on the order of thousands of Bohr radius. This kind of molecule with large size and huge permanent electric dipole moment is a good candidate for realizing the certain strongly correlated many-body gases and for quantum information processing, as well as for dipolar quantum gases and spin systems with long-range interactions. Consequently, these molecules have received considerable attention in recent years. In this paper, we review the recent theoretical and experimental investigations of ultra-cold long-range Rydberg-ground molecules, including the scattering interaction between the Rydberg electron and ground-state atom and the resulting adiabatic potential curves, experimental observations of photo-associated Rydberg-ground molecules spectra, as well as the measurements of permanent electric dipole moment. Ultra-cold long-range Rydberg-ground molecules are prepared by photoassociation in a high-density cold atom sample. Therefore, the Rydberg electron can bind several ground-state atoms to form a polyatomic Rydberg-ground molecule. The permanent molecular electric-dipole moments are revealed by spectral line broadening in the electric fields. The latest research pointed out that the permanent electric dipole moments of the Cs nDJ -type Rydberg-ground molecules are negative, which is different from the previous reports (the electric dipole moments are positive). The negative sign reflects a deficiency of Rydberg-electron density near the ground-state perturber, which is caused by electronic configuration mixing.
Rydberg molecule, formed by one or more Rydberg atoms, exhibits remarkable properties, including an exceptionally large spatial extent, rich rovibrational level structures, permanent electric dipole moments, and a pronounced sensitivity to external fields. Based on the underlying binding mechanisms, Rydberg molecules can be divided into three categories, the ground-Rydberg molecule that is bound via a low-energy electron-atom scattering interaction between ground atom and Rydberg electron, the Rydberg-Rydberg molecule that is bound via a long-range electrostatic interaction between Rydberg atoms, and the ion-Rydberg molecule that is bound via single- or multi-polar interactions between Rydberg atom and ion. This review focuses on recent theoretical and experimental advances in diatomic Rydberg molecules, covering their formation and binding mechanisms, potential energy curves, experimental observations, and spectroscopic properties, with the aim of providing a comprehensive overview of the current state and future prospects of this rapidly developing field.
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 (such as long lifetimes and large sizes) but they also 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 the previous work (S T Rittenhouse and H R Sadeghpour 2010 Phys. Rev. Lett. 104 243002). 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.
We predict that ultralong-range Rydberg bimolecules form in collisions between polar molecules in cold and ultracold settings. The interaction of Λ-doublet nitric oxide (NO) with long-lived Rydberg NO(nf, ng) molecules forms ultralong-range Rydberg bimolecules with GHz energies and kilo-Debye permanent electric dipole moments. The Hamiltonian includes both the anisotropic charge-molecular dipole interaction and the electron-NO scattering. The rotational constant for the Rydberg bimolecules is in the MHz range, allowing for microwave spectroscopy of rotational transitions in Rydberg bimolecules. Considerable orientation of NO dipole can be achieved. The Rydberg molecules described here hold promise for studies of a special class of long-range bimolecular interactions.
A generalized class of ultralong-range Rydberg molecules is predicted which consist of a multichannel Rydberg atom whose outermost electron creates a chemical bond with a distant ground state atom. Such multichannel Rydberg molecules exhibit favorable properties for laser excitation, because states exist where the quantum defect varies strongly with the principal quantum number. The resulting occurrence of near degeneracies with states of high orbital angular momentum promotes the admixture of low l into the high l deeply bound "trilobite" molecule states, thereby circumventing the usual difficulty posed by electric dipole selection rules. Such states also can exhibit multiscale binding possibilities that could present novel options for quantum manipulation.