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arXiv:1201.1971 · Physical Review A

Electric field control in ultralong-range triatomic polar Rydberg molecules

Michael Mayle, Seth T. Rittenhouse, Peter Schmelcher, H. R. Sadeghpour

Published May 24, 2012• 23 citations
arXivHTMLPDF

Abstract

We theoretically explore the external electric field control of a species of ultralong-range molecules that emerge from the interaction of a ground-state polar molecule with a Rydberg atom. The external field mixes the Rydberg electronic states and, therefore, strongly alters the electric field seen by the polar diatomic molecule due to the Rydberg electron. As a consequence, the adiabatic potential energy curves responsible for the molecular binding can be tuned in such a way that an intersection with neighboring curves occurs. The latter leads to admixture of $s$-wave character in the Rydberg wave function and will substantially facilitate the experimental preparation and realization of this particular class of Rydberg molecule species.

DOI
10.1103/physreva.85.052511

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We theoretically explore the external electric field control of a species of ultralong-range molecules that emerge from the interaction of a ground-state polar molecule with a Rydberg atom. The external field mixes the Rydberg electronic states and, therefore, strongly alters the electric field seen by the polar diatomic molecule due to the Rydberg electron. As a consequence, the adiabatic potential energy curves responsible for the molecular binding can be tuned in such a way that an intersection with neighboring curves occurs. The latter leads to admixture of sss-wave character in the Rydberg wave function and will substantially facilitate the experimental preparation and realization of this particular class of Rydberg molecule species.
We investigate the impact of an electric field on the structure of ultra-long-range polar diatomic rubidium Rydberg molecules. Both the sss-wave and ppp-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 shifting of the corresponding potential wells in such a manner that the importance of the ppp-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 nonpolar 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.
Abstract We investigate the electronic structure of a triatomic Rydberg molecule formed by a Rydberg atom and two neutral ground-state atoms. Taking into account the s -wave and p -wave interactions, we perform electronic structure calculations and analyze the adiabatic electronic potentials evolving from the Rb ( n = 35 , l ≥ 3 ) Rydberg degenerate manifold. We hereby focus on three different classes of geometries of the Rydberg molecules, including symmetric, asymmetric and planar configurations. The metamorphosis of these potential energy surfaces in the presence of an external electric field is explored.
We investigate the impact of combined electric and magnetic fields on the structure of ultralong-range polar Rydberg molecules. Our focus is hereby on the parallel as well as the crossed field configuration, taking into account both the s -wave and p -wave interactions of the Rydberg electron and the neutral ground state atom. We show the strong impact of the p -wave interaction on the ultralong-range molecular states for a pure B -field configuration. In the presence of external fields, the angular degrees of freedom acquire vibrational character, and we encounter two- and three-dimensional oscillatory adiabatic potential energy surfaces for the parallel and crossed field configuration, respectively. The equilibrium configurations of local potential wells can be controlled via the external field parameters for both field configurations depending on the specific degree of electronic excitation. This allows us to tune the molecular alignment and orientation. The resulting electric dipole moment is in the order of several kDebye, and the rovibrational level spacings are in the range of 2– . Both properties are analyzed with varying field strengths.
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.
We explore the electronic structure and rovibrational properties of an ultralong-range triatomic Rydberg molecule formed by a Rydberg atom and a ground state heteronuclear diatomic molecule. We focus here on the interaction of a Rb( ) Rydberg atom with a KRb( N = 0) diatomic polar molecule. There is significant electronic hybridization with the Rb( n = 24, ) degenerate manifold. The polar diatomic molecule is allowed to rotate in the electric fields generated by the Rydberg electron and core as well as an external field. We investigate the metamorphosis of the Born–Oppenheimer potential curves, essential for the binding of the molecule, with varying electric field and analyze the resulting properties such as the vibrational structure and the alignment and orientation of the polar diatomic molecule.
We consider an ultralong-range polytonic Rydberg molecule formed by a Rydberg atom and two heteronuclear diatomic molecules. We focus here on the interaction of a Rb( n = 24, l ≥ 3) Rydberg atom with two KRb diatomic polar molecules in their rotational ground state. The polar diatomic molecules are allowed to rotate in the electric fields generated by the Rydberg electron and core. We investigate the electronic structure of this ultralong-range polytomic Rydberg molecule, and rovibrational properties of the two polar dimers as an additional external field is applied.