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arXiv:2007.03371 · Physical Review A

Photodissociation of long-range Rydberg molecules

Michael Peper, Johannes Deiglmayr

Published Dec 22, 2020• 9 citations
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Abstract

We present photodissociation of ultracold long-range Rydberg molecules as a tool to characterize their electronic properties. We photoassociate $^{39}\mathrm{K}_{2} 37\phantom{\rule{0.16em}{0ex}}^{2}P$ molecules with highly entangled electronic and nuclear spins of the two bound atoms and quantify the entanglement by projection of the molecular state onto noninteracting atoms using radio-frequency photodissociation. By comparison of experimental photodissociation rates with theoretical predictions, we further characterize the electronic and nuclear wave function of the photoassociated molecules. Based on the complete characterization of the formed long-range Rydberg molecules, we demonstrate a full hyperfine-spin flip of a free ground-state atom through the interaction with a Rydberg atom.

DOI
10.1103/physreva.102.062819

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We present photodissociation of ultracold long-range Rydberg molecules as a tool to characterize their electronic properties. We photoassociate 39K2372P^{39}\mathrm{K}_{2} 37\phantom{\rule{0.16em}{0ex}}^{2}P39K2​372P molecules with highly entangled electronic and nuclear spins of the two bound atoms and quantify the entanglement by projection of the molecular state onto noninteracting atoms using radio-frequency photodissociation. By comparison of experimental photodissociation rates with theoretical predictions, we further characterize the electronic and nuclear wave function of the photoassociated molecules. Based on the complete characterization of the formed long-range Rydberg molecules, we demonstrate a full hyperfine-spin flip of a free ground-state atom through the interaction with a Rydberg atom.
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 have performed high resolution photoassociation spectroscopy of rubidium ultralong-range Rydberg molecules in the vicinity of the 25P state. Because of the hyperfine interaction in the ground state perturber atom, the emerging mixed singlet-triplet potentials contain contributions from both hyperfine states. We show that this can be used to induce remote spin flips in the perturber atom upon excitation of a Rydberg molecule. Furthermore, when the spin-orbit splitting of the Rydberg state is comparable to the hyperfine splitting in the ground state, the orbital angular momentum of the Rydberg electron is entangled with the nuclear spin of the perturber atom. Our results open new possibilities for the implementation of spin-dependent interactions for ultracold atoms in bulk systems and in optical lattices.
We report on the observation of long-range Cs 2 Rydberg molecules consisting of a p-state Rydberg atom and a ground-state atom. Two types of molecular states are visible in the photoassociation spectra: states bound purely by triplet s -wave scattering and states bound by mixed singlet-triplet s -wave scattering. 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 reproduces the experimental observations. The detailed analysis reveals the important role of singlet scattering in long-range Rydberg molecules and yields an effective singlet s-wave scattering length for low-energy e − -Cs collisions.
We discuss the rotational structure of ultra-long range Rydberg molecules and their angular nuclear wave function. Expressing the complete molecular wave function in a laboratory fixed frame, we derive the transition matrix elements for the photoassociation of free ground state atoms. The coupling strength depends on the angular momentum coupling in the Rydberg molecule, which differs for the various types of Rydberg molecules. This work explains the different steps to calculate the wave functions and the transition matrix elements in a way, that they can be transferred to other Rydberg molecules involving different atomic species or molecular coupling cases.
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 long-range homonuclear diatomic nD Rydberg molecules photoassociated out of an ultracold gas of Rb87 atoms for 34≤n≤40. The measured ground-state binding energies of Rb87(nD+5S1/2) molecular states are larger than those of their Rb87(nS+5S1/2) counterparts, which shows the dependence of the molecular bond on the angular momentum of the Rydberg atom. We exhibit the transition of Rb87(nD+5S1/2) molecules from a molecular-binding-dominant regime at low n to a fine-structure-dominant regime at high n [akin to Hund's cases (a) and (c), respectively]. In the analysis, the fine structure of the nD Rydberg atom and the hyperfine structure of the 5S1/2 atom are included.