In a combined experimental and theoretical effort we report on two novel types of ultracold long-range Rydberg molecules. First, we demonstrate the creation of triatomic molecules of one Rydberg atom and two ground-state atoms in a single-step photoassociation. Second, we assign a series of excited dimer states that are bound by a so far unexplored mechanism based on internal quantum reflection at a steep potential drop. The properties of the Rydberg molecules identified in this work qualify them as prototypes for a new type of chemistry at ultracold temperatures.

Permanent electric dipole moments in molecules require a breaking of parity symmetry. Conventionally, this symmetry breaking relies on the presence of heteronuclear constituents. We report the observation of a permanent electric dipole moment in a homonuclear molecule in which the binding is based on asymmetric electronic excitation between the atoms. These exotic molecules consist of a ground-state rubidium (Rb) atom bound inside a second Rb atom electronically excited to a high-lying Rydberg state. Detailed calculations predict appreciable dipole moments on the order of 1 Debye, in excellent agreement with the observations.

We introduce a scheme to entangle Rydberg ions in a linear ion crystal, using the high electric polarizability of the Rydberg electronic states in combination with mutual Coulomb coupling of ions that establishes common modes of motion. After laser-initialization of ions to a superposition of ground-and Rydberg-state, the entanglement operation is driven purely by applying a voltage pulse that shuttles the ion crystal back and forth. This operation can achieve entanglement on a sub-µs timescale, more than two orders of magnitude faster than typical gate operations driven by continuous-wave lasers. Our analysis shows that the fidelity achieved with this protocol can exceed 99.9% with experimentally achievable parameters.

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