Sr 2 Rydberg molecules are created through two-photon excitation in an ultracold strontium gas contained in an optical dipole trap and are detected through atom loss from the trap. First order perturbation theory employing the Fermi pseudopotential and effective s-wave and p-wave scattering lengths is used to evaluate the binding energies of the molecular levels.
Sr 2 Rydberg molecules are created through two-photon excitation in an ultracold strontium gas contained in an optical dipole trap and are detected through atom loss from the trap. First order perturbation theory employing the Fermi pseudopotential and effective s-wave and p-wave scattering lengths is used to evaluate the binding energies of the molecular levels.
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.
Dipole-dipole interactions, the strongest, longest-range interactions possible between two neutral atoms, cannot be better manifested anywhere else than in a Rydberg atomic system. Rydberg atoms, having high principal quantum numbers n>>1 and dipole moments that scale as n^2, provide a powerful tool to examine dipole-dipole interactions. Therefore, we have studied the production and production rates of strontium Rydberg atoms created using two-photon excitation and have explored their properties in two distinct experiments. In the first experiment, very-high-n (n~300) Rydberg atoms are produced in a tightly collimated atomic beam allowing spectroscopic studies of their energy levels and their Stark effects. Simulations using a two-active-electron model, developed by our theoretical collaborators, allow detailed analysis of the results and are in remarkable agreement with the experimental results. The high density of Rydberg atoms achieved ~ 5*10^5 cm^(-3), in this experiment will allow studies of strongly interacting Rydberg-Rydberg systems. The second experiment, in which a cold strontium Rydberg gas is excited in a magneto-optic trap, features an imaging technique offering both spatial and temporal resolution. We use this technique to observe and study the evolution of an ultra-cold strontium Rydberg gas which reveals the importance of Rydberg-Rydberg interactions in the early stages of this evolution. Strongly interacting Rydberg gas provides an opportunity to realize a very strongly-correlated ultra-cold plasma.
Summary form only given. The discovery of ultracold and dilute ensembles of atoms and molecules in magneto-optical traps (MOT) and in atomic Bose-Einstein condensates (BECs) has ushered in a new era of precision atomic and molecular spectroscopy. Since the atoms in such cold environments predominantly interact via long-range forces, the creation of BECs and dilute atomic samples has made the study of very long-range molecular states possible. In this work (Greene et al, Phys. Rev. Lett. vol. 85, p. 2458, 2000), we discuss a particular interatomic arrangement that should be favored in modern-day MOT and BEC setups and should result in the production of molecular Rydberg states whose vibrational wave functions are localized at internuclear distances of order n/sup 2/ Bohr radii, where n is the principal quantum number. The vibrational binding energies of these molecules for n=20-50 fall in the MHz and GHz range, for molecules excited from /sup 87/Rb ultracold atomic gas. We predict two distinct classes of molecular Rydberg states. The nonpolar class of Rydberg molecules form from the interaction between a Rb(nl/sub j/) Rydberg atom with low orbital angular momentum l/sub j//spl les/2 and a distant Rb ground state atom. Rydberg molecules of the second class form from the interaction between an excited Rb atom in high (l/sub j/>2) orbital angular momentum states with a ground state Rb atom.
In this work the existence of a novel type of molecule is shown whose binding is based solely on electron-atom scattering. These molecules are composed of a Rydberg atom and a ground state atom - here Rb(ns) and Rb(5s) - where the binding arises from scattering of the Rydberg electron from the ground state atom. The ground state atom is bound to the Rydberg wavefunction, which has radii on the order of 100nm, and thus these molecules are of long-range. Although the theoretical description of this interaction goes back to the famous work of Fermi in the year 1934 which was expanded in the following decades by Omont and Greene, the experimental proof of their existence was still missing. Up to now, experimental evidence for the ultralong-range Rydberg molecules was found only in spectral line broadenings. The present experiments have demonstrated the direct photoassociation of these ultralong-range Rydberg molecules for Rb(ns)-Rb(5s) triplet states from a cold and dense sample of rubidium 87 atoms for a range of principal quantum numbers, n, between 34 and 40. The high-resolution photoassociation spectra allowed for the observation of several vibrational states separated by only a few Megahertz. Based on the model by Greene the vibrational ground states v=0 are assigned and the dependence of their binding energy on the principal quantum number, n, is used to extract the triplet s-wave scattering length for electron-Rb(5s) collisions from the data. The remarkably good agreement between experiment and theory for the vibrational ground state v=0 over a range of principal quantum numbers attests to the accuracy of Fermi's original pseudopotential approach in describing interactions in excited multi-atom systems. Aside from this good agreement for the state v=0, the measurements also show that contributions from p-wave scattering cannot be neglected, as a number of excited vibrational states is observed in the experiment that are not predicted from the theory assuming only s-wave scattering. Calculations of Li, Pohl and coworkers have shown that a full solution of the electron-atom scattering is necessary for the assignment of all vibrational states. This work finds the molecular bound states to be very sensitive to both s-wave as well as p-wave electron-atom scattering and the Rydberg molecules turn out to be an accurate experimental platform to study electron-atom collisions in a previously inaccessible ultralow-energy regime. In general, the ultralong-range Rydberg molecules investigated here for rubidium are expected for all species with negative scattering length for electron-atom interaction, e. g. the other alkali atoms. Rydberg atom and ground state atom do not even have to be of the same chemical element, the only requirement is a negative scattering length of the ground state atom for electron scattering. Moreover, the binding force of the Rydberg electron is not restricted to a single ground state atom and molecules with more than one ground state atom can be created. The fact that these exotic molecules have huge bond lengths but nevertheless a vibrational spectrum with several states make a new type of ultracold Rydberg chemistry feasible. In the future, larger polymers or even heteronuclear molecules can be realized, where the number of atoms, the constituent atomic elements and the addressed Rydberg state allow to precisely select the properties of the long-range molecule.
We observe the formation of long-range Cs2 Rydberg molecules consisting of a Rydberg and a ground-state atom by photoassociation spectroscopy in an ultracold Cs gas near 6s1/2(F=3,4)→np3/2 resonances (n=26-34). The spectra reveal two types of molecular states recently predicted by D. A. Anderson, S. A. Miller, and G. Raithel [Phys. Rev. A 90, 062518 (2014)]: states bound purely by triplet s-wave scattering with binding energies ranging from 400 MHz at n=26 to 80 MHz at n=34, and states bound by mixed singlet-triplet s-wave scattering with smaller and F-dependent binding energies. The experimental observations are accounted for by an effective Hamiltonian including s-wave scattering pseudopotentials, the hyperfine interaction of the ground-state atom, and the spin-orbit interaction of the Rydberg atom. The analysis enables the characterization of the role of singlet scattering in the formation of long-range Rydberg molecules and the determination of an effective singlet s-wave scattering length for low-energy-electron-Cs collisions.
We report on the atom loss spectroscopy of strontium Rydberg atoms in a magnetooptical trap, using a two-photon excitation scheme through the intermediate state 5s5p3P1. Energies of the 5sns3S1 and 5snd3D1,2 Rydberg series of 88Sr in the range $13\ensuremath{\le}n\ensuremath{\le}50$ are determined with an absolute accuracy of 10 MHz, including the perturbed region where the 5snd3D2 series couples to the 5snd1D2 series. This represents an improvement by more than two orders of magnitude compared to previously published data. The quantum defects for each series are determined using the extended Rydberg-Ritz formula in the range where there is no strong perturbation. A value of 1377012721(10)MHz for the first ionization limit of 88Sr is extracted.