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arXiv:2004.14585 · Physical Review A

Heteronuclear Rydberg molecules

J. D. Whalen, S. K. Kanungo, Y. Lu, S. Yoshida, Joachim Burgdörfer, F. B. Dunning, T. C. Killian

Published Jun 24, 2020• 17 citations
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Abstract

In this work, the authors report on the observation of heteronuclear ultralong-range Rydberg molecules, together with a detailed theoretical analysis of the experimental data. Such heteronuclear Rydberg molecules are expected to present many new opportunities for studying quantum systems, such as probing interparticle and interspecies pair correlation functions in multicomponent many-body systems, exploring the sensitivity of the isotope shift to the mass polarization energy for Rydberg trimers or larger molecules, or studying new types of Rydberg impurities in quantum gases.

DOI
10.1103/physreva.101.060701

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Ultra-long-range Rydberg molecules (ULRMs) have attracted significant interest due to their unique electronic properties and potential applications in quantum technologies. We theoretically investigate the formation and characteristics of heteronuclear ULRMs, focusing on Rb-Cs systems. We explore the vibrational energy levels of heteronuclear nD ULRMs and compare them with homonuclear counterparts. We also predict the formation of polyatomic heteronuclear ULRMs, discussing how the binding energy and spectral features evolve as the number of ground-state atoms increases. Our theoretical predictions are presented in terms of molecular spectra and provide insight into the formation dynamics of these systems. The study further explores the potential applications of heteronuclear ULRMs in quantum information processing, quantum simulation, and precision measurements, offering new avenues for future research in many-body physics and quantum technologies.
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Ultralong-range Rydberg molecules, composed of an excited Rydberg atom and a ground-state atom, are characterized by large bond lengths, dipole moments, sensitivity to external fields, and an unusual binding mechanism based on low-energy elastic electron scattering. Although Rydberg molecules formed between alkali atoms have received the most attention, the additional complexity found in atoms with more than a single valence electron poses new theoretical challenges as well as new possibilities for control and design of the molecular structure. In this paper, we extend the theory of Rydberg molecules to include the additional spin coupling of the Rydberg states of a multivalent atom. We employ this theory to describe the properties of Rydberg molecules composed of mercury atoms. We calculate the potential energy curves of both heteronuclear (Hg∗Rb{\mathrm{Hg}}^{*}\mathrm{Rb}Hg∗Rb) and homonuclear (Hg∗Hg{\mathrm{Hg}}^{*}\mathrm{Hg}Hg∗Hg) molecules. In the former case, we propose the realization of long-range spin entanglement and remote spin flip. In the latter, we show how long-lived metastable molecular states of Hg∗Hg{\mathrm{Hg}}^{*}\mathrm{Hg}Hg∗Hg exist as resonances above the dissociation threshold.
We present a comprehensive study of the diverse properties of heteronuclear Rydberg molecules, placing a special emphasis on those composed of the light alkali-metal atoms, Li, Na, and K. Electron-atom scattering phase shifts, which determine the strength of the molecular bond, are calculated at very low energy and then used in a spin-dependent theoretical model to calculate accurate Rydberg molecule potential-energy curves. The wide parameter range accessible by combining the various properties of different alkali-metal atoms often leads to hybridized electronic states accessible via one or two photon excitation schemes. This analysis of heteronuclear molecules leads to a prediction that the relative densities and spatial distributions of atoms in an ultracold mixture can be probed at controllable length scales via spectroscopic detection of these molecules.
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.