Intercombination Effects in Resonant Energy Transfer

Abstract

We investigate the effect of intercombination transitions in excitation hopping processes such as those found in Förster resonance energy transfer. Taking strontium Rydberg states as our model system, the breakdown of $LS$-coupling leads to weakly allowed transitions between Rydberg states of different spin quantum number. We show that the long-range interactions between two Rydberg atoms can be affected by these weakly allowed spin transitions, and the effect is greatest when there is a near-degeneracy between the initial state and a state with a different spin quantum number. We also consider a case of four atoms in a spin chain, and show that a spin impurity can resonantly hop along the chain. By engineering the many-body energy levels of the spin-chain, the breakdown of $LS$ coupling due to inter-electronic effects in individual atoms can be mapped onto a spatial separation of the total spin and the total orbital angular momentum along the spin chain.