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arXiv:1405.0429 · Journal of Physics B Atomic Molecular and Optical Physics

Ultralong-range Rydberg molecules in combined electric and magnetic fields

Markus Kurz, Peter Schmelcher

Published Aug 6, 2014• 21 citations
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Abstract

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.

DOI
10.1088/0953-4075/47/16/165101

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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 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 fine and spin structure of ultralong-range Rydberg molecules exposed to a homogeneous magnetic field. Each molecule consists of a 87Rb^{87}\mathrm{Rb}87Rb Rydberg atom the outer electron of which interacts via spin-dependent sss- and ppp-wave scattering with a polarizable 87Rb^{87}\mathrm{Rb}87Rb ground-state atom. Our model includes also the hyperfine structure of the ground-state atom as well as spin-orbit couplings of the Rydberg and ground-state atom. We focus on ddd-Rydberg states and principal quantum numbers nnn in the vicinity of 40. The electronic structure and vibrational states are determined in the framework of the Born-Oppenheimer approximation for varying field strengths ranging from a few up to hundred Gauss. The results show that the interplay between the scattering interactions and the spin couplings gives rise to a large variety of molecular states in different spin configurations as well as in different spatial arrangements that can be tuned by the magnetic field. This includes relatively regularly shaped energy surfaces in a regime where the Zeeman splitting is large compared to the scattering interaction but small compared to the Rydberg fine structure, as well as more complex structures for both weaker and stronger fields. We quantify the impact of spin couplings by comparing the extended theory to a spin-independent model.
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 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 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.