Rydberg atoms have an electron in a state with a very high principal quantum number, and as a result can exhibit unusually long-range interactions. One example is the bonding of two such atoms by multipole forces to form Rydberg-Rydberg molecules with very large internuclear distances. Notably, bonding interactions can also arise from the low-energy scattering of a Rydberg electron with negative scattering length from a ground-state atom. In this case, the scattering-induced attractive interaction binds the ground-state atom to the Rydberg atom at a well-localized position within the Rydberg electron wavefunction and thereby yields giant molecules that can have internuclear separations of several thousand Bohr radii. Here we report the spectroscopic characterization of such exotic molecular states formed by rubidium Rydberg atoms that are in the spherically symmetric s state and have principal quantum numbers, n, between 34 and 40. We find that the spectra of the vibrational ground state and of the first excited state of the Rydberg molecule, the rubidium dimer Rb(5s)-Rb(ns), agree well with simple model predictions. The data allow us to extract the s-wave scattering length for scattering between the Rydberg electron and the ground-state atom, Rb(5s), in the low-energy regime (kinetic energy, <100 meV), and to determine the lifetimes and the polarizabilities of the Rydberg molecules. Given our successful characterization of s-wave bound Rydberg states, we anticipate that p-wave bound states, trimer states and bound states involving a Rydberg electron with large angular momentum-so-called trilobite molecules-will also be realized and directly probed in the near future.

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We report on strong van der Waals blockade in two-photon Rydberg excitation of ultracold magnetically trapped 87Rb atoms. The excitation dynamics was investigated for a large range of densities and laser intensities and shows a full saturation and a strong suppression with respect to single-atom behavior. The observed scaling of the initial increase with density and laser intensity provides evidence for coherent collective excitation. This coherent collective behavior, that was observed for up to several thousand atoms per blockade volume, is generic for all mesoscopic systems which are able to carry only one single quantum of excitation.

We review experimental and theoretical tools to excite, study and understand strongly interacting Rydberg gases. The focus lies on the excitation of dense ultracold atomic samples close to, or within quantum degeneracy, to high lying Rydberg states. The major part is dedicated to highly excited S-states of Rubidium, which feature an isotropic van-der-Waals potential. Nevertheless are the setup and the methods presented also applicable to other atomic species used in the field of laser cooling and atom trapping.

We study the appearance of correlated many-body phenomena in an ensemble of atoms driven resonantly into a strongly interacting Rydberg state. The ground state of the Hamiltonian describing the driven system exhibits a second order quantum phase transition. We derive the critical theory for the quantum phase transition and show that it describes the properties of the driven Rydberg system in the saturated regime. We find that the suppression of Rydberg excitations known as blockade phenomena exhibits an algebraic scaling law with a universal exponent.