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Journal of Physics Conference Series

Anisotropic blockade using pendular long-range Rydberg molecules

Matthew T. Eiles, H. Lee, Jesús Pérez‐Ríos, Chris H. Greene

Published Jul 1, 2017• 0 citations
Publisher

Abstract

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.

DOI
10.1088/1742-6596/875/9/082005

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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.
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.
The interaction between a Rydberg electron and a neutral atom situated inside its extended orbit is described via contact interactions for each atom-electron scattering channel. In ultracold environments, these interactions lead to long-range molecules with binding energies typically ranging from 10 to $1\ifmmode\times\else\texttimes\fi{}{10}^{4}$ MHz. These energies are comparable to the relativistic and hyperfine structure of the separate atomic components. Studies of molecular formation aiming to reproduce observations with spectroscopic accuracy must therefore include the hyperfine splitting of the neutral atom and the spin-orbit splittings of both the Rydberg atom and the electron-atom interaction. Adiabatic potential energy curves and permanent electric dipole moments are presented for Rb2{\mathrm{Rb}}_{2}Rb2​ and Cs2{\mathrm{Cs}}_{2}Cs2​. The influence of spin degrees of freedom on the potential energy curves and multipole moments probed in recent experimental work is elucidated, and the observed dipole moments of butterfly molecules are explained by the generalized 3PJ^{3}P_{J}3PJ​ pseudopotential derived here.
Cold and ultracold Rydberg atoms are in considerable vogue for their ability to creating strong interactions, stemming from their exaggerated and readily tunable properties. Ultralong-range Rydberg molecules have been predicted to form from the interaction of ultracold Rydberg atoms with ground-state atoms and polar molecules. In this work, we discuss and demonstrate how such molecules, which are homonuclear, form substantially large permanent electric dipole moments. A corollary benefit of such strong hybridisation is the realisation of high angular momentum degenerate Rydberg molecules (so-called trilobite molecules) with standard photoassociation techniques.
We predict that ultralong-range Rydberg bimolecules form in collisions between polar molecules in cold and ultracold settings. The interaction of Λ-doublet nitric oxide (NO) with long-lived Rydberg NO(nf, ng) molecules forms ultralong-range Rydberg bimolecules with GHz energies and kilo-Debye permanent electric dipole moments. The Hamiltonian includes both the anisotropic charge-molecular dipole interaction and the electron-NO scattering. The rotational constant for the Rydberg bimolecules is in the MHz range, allowing for microwave spectroscopy of rotational transitions in Rydberg bimolecules. Considerable orientation of NO dipole can be achieved. The Rydberg molecules described here hold promise for studies of a special class of long-range bimolecular interactions.
Rydberg molecule, formed by one or more Rydberg atoms, exhibits remarkable properties, including an exceptionally large spatial extent, rich rovibrational level structures, permanent electric dipole moments, and a pronounced sensitivity to external fields. Based on the underlying binding mechanisms, Rydberg molecules can be divided into three categories, the ground-Rydberg molecule that is bound via a low-energy electron-atom scattering interaction between ground atom and Rydberg electron, the Rydberg-Rydberg molecule that is bound via a long-range electrostatic interaction between Rydberg atoms, and the ion-Rydberg molecule that is bound via single- or multi-polar interactions between Rydberg atom and ion. This review focuses on recent theoretical and experimental advances in diatomic Rydberg molecules, covering their formation and binding mechanisms, potential energy curves, experimental observations, and spectroscopic properties, with the aim of providing a comprehensive overview of the current state and future prospects of this rapidly developing field.
Engineering molecules with a tunable bond length and defined quantum states lies at the heart of quantum chemistry. The unconventional binding mechanism of Rydberg molecules makes them a promising candidate to implement such tunable molecules. A very peculiar type of Rydberg molecules are the so-called butterfly molecules, which are bound by a shape resonance in the electron-perturber scattering. Here we report the observation of these exotic molecules and employ their exceptional properties to engineer their bond length, vibrational state, angular momentum and orientation in a small electric field. Combining the variable bond length with their giant dipole moment of several hundred Debye, we observe counter-intuitive molecules which locate the average electron position beyond the internuclear distance.