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arXiv:2208.07776 · Physical Review Letters

Observation of Vibrational Dynamics of Orientated Rydberg-Atom-Ion Molecules

Yiquan Zou, Moritz Berngruber, Viraatt S. V. Anasuri, Nicolas Zuber, Florian Meinert, Robert Löw, Tilman Pfau

Published Jan 12, 2023• 28 citations
arXivHTMLPDF

Abstract

Vibrational dynamics in conventional molecules usually takes place on a timescale of picoseconds or shorter. A striking exception are ultralong-range Rydberg molecules, for which dynamics is dramatically slowed down as a consequence of the huge bond length of up to several micrometers. Here, we report on the direct observation of vibrational dynamics of a recently observed Rydberg-atom-ion molecule. By applying a weak external electric field of a few millivolts per centimeter, we are able to control the orientation of the photoassociated ultralong-range Rydberg molecules and induce vibrational dynamics by quenching the electric field. A high resolution ion microscope allows us to detect the molecule's orientation and its temporal vibrational dynamics in real space. Our study opens the door to the control of molecular dynamics in Rydberg molecules.

DOI
10.1103/physrevlett.130.023002

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Vibrational dynamics in conventional molecules usually takes place on a timescale of picoseconds or shorter. A striking exception are ultralong-range Rydberg molecules, for which dynamics is dramatically slowed down as a consequence of the huge bond length of up to several micrometers. Here, we report on the direct observation of vibrational dynamics of a recently observed Rydberg-atom-ion molecule. By applying a weak external electric field of a few millivolts per centimeter, we are able to control the orientation of the photoassociated ultralong-range Rydberg molecules and induce vibrational dynamics by quenching the electric field. A high resolution ion microscope allows us to detect the molecule's orientation and its temporal vibrational dynamics in real space. Our study opens the door to the control of molecular dynamics in Rydberg molecules.
Controlling molecular binding at the level of single atoms is one of the holy grails of quantum chemistry. Rydberg macrodimers─bound states between highly excited Rydberg atoms─provide a novel perspective in this direction. Resulting from binding potentials formed by the strong, long-range interactions of Rydberg states, Rydberg macrodimers feature bond lengths in the micrometer regime, exceeding those of conventional molecules by orders of magnitude. Using single-atom control in quantum gas microscopes, the unique properties of these exotic states can be studied with unprecedented control, including the response to magnetic fields or the polarization of light in their photoassociation. The high accuracy achieved in spectroscopic studies of macrodimers makes them an ideal testbed to benchmark Rydberg interactions, with direct relevance to quantum computing and information protocols where these are employed. This review provides a historic overview and summarizes the recent findings in the field of Rydberg macrodimers. Furthermore, it presents new data on interactions between macrodimers, leading to a phenomenon analogous to Rydberg blockade at the level of molecules, opening the path toward studying many-body systems of ultralong-range Rydberg molecules.
We theoretically explore the external electric field control of a species of ultralong-range molecules that emerge from the interaction of a ground-state polar molecule with a Rydberg atom. The external field mixes the Rydberg electronic states and, therefore, strongly alters the electric field seen by the polar diatomic molecule due to the Rydberg electron. As a consequence, the adiabatic potential energy curves responsible for the molecular binding can be tuned in such a way that an intersection with neighboring curves occurs. The latter leads to admixture of sss-wave character in the Rydberg wave function and will substantially facilitate the experimental preparation and realization of this particular class of Rydberg molecule species.
We present a novel binding mechanism where a neutral Rydberg atom and an atomic ion form a molecular bound state at a large internuclear distance. The binding mechanism is based on Stark shifts and level crossings that are induced in the Rydberg atom due to the electric field of the ion. At particular internuclear distances between the Rydberg atom and the ion, potential wells occur that can hold atom–ion molecular bound states. Apart from the binding mechanism, we describe important properties of the long-range atom–ion Rydberg molecule, such as its lifetime and decay paths, its vibrational and rotational structure, and its large dipole moment. Furthermore, we discuss methods of how to produce and detect it. The unusual properties of the long-range atom–ion Rydberg molecule give rise to interesting prospects for studies of wave packet dynamics in engineered potential energy landscapes.
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.
We explore the electronic structure and rovibrational properties of an ultralong-range triatomic Rydberg molecule formed by a Rydberg atom and a ground state heteronuclear diatomic molecule. We focus here on the interaction of a Rb( ) Rydberg atom with a KRb( N = 0) diatomic polar molecule. There is significant electronic hybridization with the Rb( n = 24, ) degenerate manifold. The polar diatomic molecule is allowed to rotate in the electric fields generated by the Rydberg electron and core as well as an external field. We investigate the metamorphosis of the Born–Oppenheimer potential curves, essential for the binding of the molecule, with varying electric field and analyze the resulting properties such as the vibrational structure and the alignment and orientation of the polar diatomic molecule.
The subnanoscale size of typical diatomic molecules hinders direct optical access to their constituents. Rydberg macrodimers-bound states of two highly excited Rydberg atoms-feature interatomic distances easily exceeding optical wavelengths. We report the direct microscopic observation and detailed characterization of such molecules in a gas of ultracold rubidium atoms in an optical lattice. The bond length of about 0.7 micrometers, comparable to the size of small bacteria, matches the diagonal distance of the lattice. By exciting pairs in the initial two-dimensional atom array, we resolved more than 50 vibrational resonances. Using our spatially resolved detection, we observed the macrodimers by correlated atom loss and demonstrated control of the molecular alignment by the choice of the vibrational state. Our results allow for rigorous testing of Rydberg interaction potentials and highlight the potential of quantum gas microscopy for molecular physics.