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arXiv:1305.0391 · Physical Review A

Electrically dressed ultra-long-range polar Rydberg molecules

Markus Kurz, Peter Schmelcher

Published Aug 1, 2013• 31 citations
arXivHTMLPDF

Abstract

We investigate the impact of an electric field on the structure of ultra-long-range polar diatomic rubidium Rydberg molecules. Both the $s$-wave and $p$-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 $p$-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.

DOI
10.1103/physreva.88.022501

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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.
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 predict the existence of a ubiquitous class of long-range molecular Rydberg states, whose Born-Oppenheimer potential curves are oscillatory in nature. These oscillations reflect the nodal structure of the atomic Rydberg state wave functions. The temperature and density of atoms in a Bose-Einstein condensate are particularly favorable for the laser excitation of ultra-long-range vibrational bound states localized at internuclear distances in the range 10(3)- 10(5) a.u. A surprising trilobitelike class of polar homonuclear diatomics should exhibit electric dipole moments in the kilodebye range.
We investigate the quantum dynamics of ultra-long-range trilobite molecules exposed to homogeneous electric fields. A trilobite molecule consists of a Rydberg atom and a ground-state atom, which is trapped at large internuclear distances in an oscillatory potential due to scattering of the Rydberg electron off the ground-state atom. Within the Born-Oppenheimer approximation, we derive an analytic expression for the two-dimensional adiabatic electronic potential energy surface in weak electric fields valid up to 500 V/m. This is used to unravel the molecular quantum dynamics employing the multiconfigurational time-dependent Hartree method. Quenches of the electric field are performed to trigger the wave-packet dynamics including the case of field inversion. Depending on the initial wave packet, we observe radial intrawell and interwell oscillations as well as angular oscillations and rotations of the respective one-body probability densities. Opportunities to control the molecular configuration are identified, a specific example being the possibility to superimpose different molecular bond lengths by a series of periodic quenches of the electric field.
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 an external magnetic field on ultra-long-range and ultracold Rydberg molecules. The Born–Oppenheimer potential surfaces are analysed and discussed for different values of the magnetic field strength. The magnetic field provides an angular confinement turning a rotational degree of freedom into a vibrational one. We explore the vibrational dynamics and observe a pronounced transition in the level spacing from a linear splitting via an irregular regime to a 2D harmonic oscillator-like behaviour. Scaling arguments for the dependence of the potential energy surfaces on the field strengths are provided. The occurrence of a monotonic lowering of the magnitude of the electric dipole moment with increasing magnetic field strength is shown.