Van der Waals–stabilized Rydberg aggregates

Abstract

Assemblies of Rydberg atoms subject to resonant dipole-dipole interactions form Frenkel excitons. We show that van-der-Waals shifts can significantly modify the exciton wave function, whenever atoms approach each other closely. As a result, attractive excitons and repulsive van-der-Waals interactions can be combined to form stable one-dimensional atom chains, akin to bound aggregates. Here the van-der-Waals shifts ensure a stronger homogeneous delocalisation of a single excitation over the whole chain, enabling it to bind up to six atoms. When brought into unstable configurations, such Rydberg aggregates allow the direct monitoring of their dissociation dynamics.