We study the possibility to use interaction between a polar molecule in the ground electronic and vibrational state and a Rydberg atom to construct two-qubit gates between molecular qubits and to coherently control molecular states. A polar molecule within the electron orbit in a Rydberg atom can either shift the Rydberg state, or form a Rydberg molecule. Both the atomic shift and the Rydberg m...

A fascinating aspect of Rydberg atoms is their ability to form huge but very weakly bound molecules with a ground state atom, only held together by a scattering process between the latter and the Rydberg electron. Beyond the usual way of creating such molecules by laser excitation from two ground state atoms with a distance of less than the Rydberg radius, we demonstrate that Rydberg molecules ...

The quadricyclane-norbornadiene system is an important model for the isomerization dynamics between highly strained molecules. In a breakthrough observation for a polyatomic molecular system of that complexity, we follow the photoionization from Rydberg states in the time-domain to derive a measure for the time-dependent structural dynamics and the time-evolving structural dispersion even while...

A fascinating aspect of Rydberg atoms is their ability to form huge but very weakly bound molecules with a ground-state atom, only held together by a scattering process between the latter and the Rydberg electron. Beyond the usual way of creating such molecules by laser excitation from two ground-state atoms with a distance of less than the Rydberg radius, we demonstrate that Rydberg molecules ...

In Rydberg atoms, at least one electron is excited to a state with a high principal quantum number. In an ultracold environment, this low-energy electron can scatter off a ground state atom allowing for the formation of a Rydberg molecule consisting of one Rydberg atom and several ground state atoms. Here we investigate those Rydberg molecules created by photoassociation for the spherically sym...

Within a dense environment (ρ ≈ 10 atoms=cm) at ultracold temperatures (T < 1 μK), a single atom excited to a Rydberg state acts as a reaction center for surrounding neutral atoms. At these temperatures, almost all neutral atoms within the Rydberg orbit are bound to the Rydberg core and interact with the Rydberg atom. We have studied the reaction rate and products for nS Rb Rydberg states, and ...

Ab initio electronic structure methods are used to estimate the cross sections for electron transfer from donor anions having electron binding energies ranging from 0.001 to 0.6 eV to each of three sites in a model disulfide-linked molecular cation. The three sites are (1) the S-S sigma(*) orbital to which electron attachment is rendered exothermic by Coulomb stabilization from the nearby posit...

Mapping the strong interaction between Rydberg excitations in ultra-cold atomic ensembles onto single photons enables the realization of optical nonlinearities which can modify light on the level of individual photons. This novel approach forms the basis of a growing Rydberg quantum optics toolbox, which already contains photonic logic building-blocks such as single-photon sources, switches, tr...

A basic theory is presented for the photoexcitation of a core state of a Rydberg atom in any type of static field; in this situation, the core state is excited by the photon while the Rydberg electron is essentially a spectator. This simple picture is made interesting through the interaction of the Rydberg electron with the core which can cause a change in the Rydberg electron’s state and can c...

We have observed and characterized two new double Rydberg anions N6H19- and N7H22- through their anion photoelectron spectra. The vertical detachment energies of these anions were found to be 0.443 and 0.438 eV, respectively. In addition, for three of the seven double Rydberg anions now known, we measured photodetachment transitions not only to the ground electronic states of their correspondin...