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arXiv:1602.08400 · Nature Communications

Observation of pendular butterfly Rydberg molecules

Thomas Niederprüm, Oliver Thomas, Tanita Eichert, Carsten Lippe, Jesús Pérez‐Ríos, Chris H. Greene, Herwig Ott

Published Oct 5, 2016• 104 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1038/ncomms12820

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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.
The detection and characterization of two classes of ultralong-range Rydberg molecules known as "trilobite" and "butterfly" molecules is presented. These molecules are a subset of a class of Rydberg molecules which asymptotically consist of a Rydberg atom and a ground state atom. The trilobite and butterfly molecules have giant, body-fixed permanent dipole moments on the order of 1000 Debye. The two classes of molecules are distinguished by the relative dominance of the s-wave and p-wave electron scattering. Spectra for (nS_1/2 + 6S_1/2) ^3 Sigma molecules, where n = 37, 39 and 40 and measurements of the Stark broadenings of selected trilobite states in Cs due to the application of a constant external electric field are presented. Additionally, measurements of spectra and Stark splittings for p-wave dominated (nS_1/2 + 6S_1/2) ^3 Pi molecules, where n = 31 and 32 are presented. Computational work on Rydberg pair interactions is also discussed.
We review ultralong-range Rydberg molecules (ULRMs), which are bound states between a Rydberg atom and one or more ground-state atoms with bond lengths on the order of thousands of Bohr radii. The binding originates from multiple electron-atom scattering and leads to exotic oscillatory potential energy surfaces that reflect the probability density of the Rydberg electron. This unconventional binding mechanism opens fascinating possibilities to tune molecular properties via weak external fields, to study spin-resolved low-energy electron-atom scattering as well as to control and to probe interatomic forces in few- and many-body systems. Here, we provide an overview on recent theoretical and experimental progress in the field with an emphasis on polyatomic ULRMs, field control and spin interactions.
We review ultralong-range Rydberg molecules (ULRMs), which are bound states between a Rydberg atom and one or more ground-state atoms with bond lengths on the order of thousands of Bohr radii. The binding originates from multiple electron-atom scattering and leads to exotic oscillatory potential energy surfaces that reflect the probability density of the Rydberg electron. This unconventional binding mechanism opens fascinating possibilities to tune molecular properties via weak external fields, to study spin-resolved low-energy electron-atom scattering as well as to control and to probe interatomic forces in few- and many-body systems. Here, we provide an overview on recent theoretical and experimental progress in the field with an emphasis on polyatomic ULRMs, field control and spin 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.
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 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.