Long-range anisotropic interactions in Rydberg atoms and molecules

Matthew T. Eiles, H. Lee, Jesús Pérez‐Ríos +1 more

Ultralong-range "butterfly" Rydberg molecules possess large dipole moments which lead to long-range anisotropic interactions between molecules. Their properties are studied using a Hamiltonian that fully includes the electronic and nuclear spin degrees of freedom. Using this more accurate and complete theoretical description, we investigate the intermolecular interaction when the molecules are prepared in pendular states. The anisotropy of this interaction manifests itself strongly in the density of created molecules.

Donald W. Booth, Jonathan Tallant, Arne Schwettmann +1 more

Jovica Stanojevic, Robin C ot 'e

Seth T. Rittenhouse, H. R. Sadeghpour

We predict the existence of a class of ultracold giant molecules formed from trapped ultracold Rydberg atoms and polar molecules. The interaction which leads to the formation of such molecules is the anisotropic, long-range charge-dipole interaction. We show that prominent candidate molecules such as deuterated hydroxyl (OD) and KRb should bind to Rydberg rubidium atoms, with energies E(b)≃5-25 GHz at distances R≃0.1-1 μm. These molecules form in double wells, mimicking chiral molecules, with each well containing a particular dipole orientation. We prepare a set of correlated dressed electron-dipole eigenstates which are used in an on-resonance Raman scheme to coherently control the molecular dipole orientation.

Jovica Stanojevic, Robin Côté, D. Tong +3 more

Matthew T. Eiles, Hyun‐Woo Lee, Jesús Pérez‐Ríos +1 more

We propose an experiment to demonstrate a blockade mechanism caused by long-range anisotropic interactions in an ultracold dipolar gas composed of the recently observed ``butterfly'' Rydberg molecules. At the blockade radius, the strong intermolecular interaction between two adjacent molecules shifts their molecular states out of resonance with the photoassociation laser, preventing their simultaneous excitation. When the molecules are prepared in a quasi-one-dimensional (Q1D) trap, the interaction's strength can be tuned via a weak external field. The molecular density thus depends strongly on the angle between the trap axis and the field. The available Rydberg and internal molecular states provide a wide range of tunability.