Abstract We propose a scheme to realize a heavy Rydberg system (HRS), a bound pair of oppositely charged ions, from a gas of ultracold atoms. The intermediate step to achieve large internuclear separations is the creation of a unique class of ultra-long-range Rydberg molecules bound in a stairwell potential energy curve. Here, a ground-state atom is bound to a Rydberg atom in an oscillatory potential emerging due to attractive singlet p-wave electron scattering. The utility of our approach originates in the large electronic dipole transition element between the Rydberg and the ionic molecule, while the nuclear configuration of the ultracold gas is preserved. The Rabi coupling between the Rydberg molecule and the heavy Rydberg system is typically in the MHz range and the permanent electric dipole moments of the HRS can be as large as one kilo-Debye. We identify specific transitions which place the creation of the heavy Rydberg system within immediate reach of experimental realization.
Abstract We propose a scheme to realize a heavy Rydberg system (HRS), a bound pair of oppositely charged ions, from a gas of ultracold atoms. The intermediate step to achieve large internuclear separations is the creation of a unique class of ultra-long-range Rydberg molecules bound in a stairwell potential energy curve. Here, a ground-state atom is bound to a Rydberg atom in an oscillatory potential emerging due to attractive singlet p-wave electron scattering. The utility of our approach originates in the large electronic dipole transition element between the Rydberg and the ionic molecule, while the nuclear configuration of the ultracold gas is preserved. The Rabi coupling between the Rydberg molecule and the heavy Rydberg system is typically in the MHz range and the permanent electric dipole moments of the HRS can be as large as one kilo-Debye. We identify specific transitions which place the creation of the heavy Rydberg system within immediate reach of experimental realization.
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.
We propose a realizable and efficient approach for exciting long-range ion-pair molecules, known as heavy Rydberg states, in an ultracold 85Rb gas via Feshbach resonances. Heavy Rydberg states, the molecular analogs of electronic Rydberg states, with the electron replaced by an atomic anion, offer opportunities for novel physics, including the formation of ultracold anions and strongly coupled plasmas. We map the positions, lifetimes, and Franck-Condon factors of heavy Rydberg resonances across a wide range of excitation energies, and we calculate the rates of formation for the most promising transitions through long-lived intermediate interferometric resonances.
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.
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 report the creation of ultra-long-range Sr2 molecules comprising one ground-state 5s21S0 atom and one atom in a 5sns3S1 Rydberg state for n ranging from 29 to 36. Molecules are created in a trapped ultracold atomic gas using two-photon excitation near resonant with the 5s5p3P1 intermediate state, and their formation is detected through ground-state atom loss from the trap. The observed molecular binding energies are reproduced with the aid of first-order perturbation theory that utilizes a Fermi pseudopotential with effective s-wave and p-wave scattering lengths to describe the interaction between an excited Rydberg electron and a ground-state Sr atom.
Molecular bonds can be divided into four primary types: ionic, covalent, van der Waals and hydrogen bonds. At ultralow temperatures a novel binding type emerges paving the way for novel molecules and ultracold chemistry [1,2]. The underlying mechanism for this new type of chemical bond is low-energy electron scattering of Rydberg electrons from polarisable ground state atoms [3]. This quantum scattering process can generate an attractive potential that is able to bind the ground state atom to the Rydberg atom at a well localized position within the Rydberg electron wave function. The resulting giant molecules can have an internuclear separation of several thousand Bohr radii, which places them among the largest known molecules to date. Their binding energies are much smaller than the Kepler frequencies of the Rydberg electrons i.e. the atomic Rydberg electron state is essentially unchanged by the bound ground state atom. Ultracold and dense samples of atoms enable the creation of these molecules via Rydberg excitation. In this paper we present spectroscopic evidence for the vibrational ground and first excited state of a Rubidium dimer Rb(5S)-Rb(nS). We apply a Born-Oppenheimer model to explain the measured binding energies for principal quantum numbers n between 34 and 40 and extract the s-wave scattering length for electron-Rb(5S) scattering in the relevant low energy regime Ekin < 100 meV. We also determine the lifetimes and the polarisabilities of these molecules. P-wave bound states [2], Trimer states [4] as well as bound states for large angular momentum of the Rydberg electron - socalled trilobite molecules [1] - are within reach in the near future and will further refine our conceptual understanding of the chemical bond.