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arXiv:1806.02963 · Physical Review Letters

Theoretical Prediction of the Creation and Observation of a Ghost Trilobite Chemical Bond

Matthew T. Eiles, Zhengjia Tong, Chris H. Greene

Published Sep 12, 2018• 6 citations
arXivHTMLPDF

Abstract

The "trilobite"-type of molecule, predicted in 2000 and observed experimentally in 2015, arises when a Rydberg electron exerts a weak attractive force on a neutral ground state atom. Such molecules have bond lengths exceeding 100 nm. The ultralong-range chemical bond between the two atoms is a nonperturbative linear combination of the many degenerate electronic states associated with high principal quantum numbers, and the resulting electron probability distribution closely resembles a fossil trilobite from antiquity. We show how to coherently engineer this same long-range orbital through a sequence of electric and magnetic field pulses even when the ground-state atom is not present and propose several methods to observe the resulting orbital. The existence of such a ghost chemical bond in which an electron reaches out from one atom to a nonexistent second atom is a consequence of the high level degeneracy.

DOI
10.1103/physrevlett.121.113203

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The "trilobite"-type of molecule, predicted in 2000 and observed experimentally in 2015, arises when a Rydberg electron exerts a weak attractive force on a neutral ground state atom. Such molecules have bond lengths exceeding 100 nm. The ultralong-range chemical bond between the two atoms is a nonperturbative linear combination of the many degenerate electronic states associated with high principal quantum numbers, and the resulting electron probability distribution closely resembles a fossil trilobite from antiquity. We show how to coherently engineer this same long-range orbital through a sequence of electric and magnetic field pulses even when the ground-state atom is not present and propose several methods to observe the resulting orbital. The existence of such a ghost chemical bond in which an electron reaches out from one atom to a nonexistent second atom is a consequence of the high level degeneracy.
Abstract This PhD tutorial discusses ultra-long-range Rydberg molecules, the exotic bound states of a Rydberg atom and one or more ground state atoms immersed in the Rydberg electron’s wave function. This novel chemical bond is distinct from an ionic or covalent bond, and is accomplished by a very different mechanism: the Rydberg electron, elastically scattering off of the ground state atoms, exerts a weak attractive force sufficient to form the molecule in long-range oscillatory potential wells. In the last decade this topic has burgeoned into a vibrant and mature subfield of atomic and molecular physics following the rapidly developing capability of experiment to observe and manipulate these molecules. This tutorial focuses on three areas where this experimental progress has demanded more sophisticated theoretical descriptions: the structure of polyatomic molecules, the influence of electronic and nuclear spin, and the behavior of these molecules in external fields. The main results are a collection of potential energy curves and electronic wave functions which together describe the physics of Rydberg molecules. Additionally, to facilitate future progress in this field, this tutorial provides a general overview of the current state of experiment and theory.
A generalized class of ultralong-range Rydberg molecules is predicted which consist of a multichannel Rydberg atom whose outermost electron creates a chemical bond with a distant ground state atom. Such multichannel Rydberg molecules exhibit favorable properties for laser excitation, because states exist where the quantum defect varies strongly with the principal quantum number. The resulting occurrence of near degeneracies with states of high orbital angular momentum promotes the admixture of low l into the high l deeply bound trilobite molecule states, thereby circumventing the usual difficulty posed by electric dipole selection rules. Such states also can exhibit multiscale binding possibilities that could present novel options for quantum manipulation.
A generalized class of ultralong-range Rydberg molecules is predicted which consist of a multichannel Rydberg atom whose outermost electron creates a chemical bond with a distant ground state atom. Such multichannel Rydberg molecules exhibit favorable properties for laser excitation, because states exist where the quantum defect varies strongly with the principal quantum number. The resulting occurrence of near degeneracies with states of high orbital angular momentum promotes the admixture of low l into the high l deeply bound "trilobite" molecule states, thereby circumventing the usual difficulty posed by electric dipole selection rules. Such states also can exhibit multiscale binding possibilities that could present novel options for quantum manipulation.
Permanent electric dipole moments are important for understanding symmetry breaking in molecular physics, control of chemical reactions, and realization of strongly correlated many-body quantum systems. However, large molecular permanent electric dipole moments are challenging to realize experimentally. We report the observation of ultralong-range Rydberg molecules with bond lengths of ~100 nanometers and kilo-Debye permanent electric dipole moments that form when an ultracold ground-state cesium (Cs) atom becomes bound within the electronic cloud of an extended Cs electronic orbit. The electronic character of this hybrid class of "trilobite" molecules is dominated by degenerate Rydberg manifolds, making them difficult to produce by conventional photoassociation. We used detailed coupled-channel calculations to reproduce their properties quantitatively. Our findings may lead to progress in ultracold chemistry and strongly correlated many-body physics.
Rydberg atom is one with a highly excited electron, and this electron can interact with a second atom in its ground state to form a weakly bound Rydberg molecule.One example of such a bound state is a "trilobite Rydberg molecule," so-called because the electron's probability distribution resembles the long-extinct sea creature.Markus Exner at the Technical University of Kaiserslautern, Germany, and colleagues have now obtained high-resolution measurements of the vibrational spectra of trilobite Rydberg molecules formed from pairs of rubidium atoms [1].The results offer a rigorous test of theoretical models.
We investigate triatomic molecules that consist of two ground-state atoms and a highly excited Rydberg atom, bound at large internuclear distances of thousands of angstroms. In the molecular state the Rydberg electron is in a superposition of high angular momentum states whose probability densities resemble the form of trilobite fossils. The associated potential-energy landscape has an oscillatory shape and supports a rich variety of stable geometries with different bond angles and bond lengths. Based on an electronic structure investigation we analyze the molecular geometry systematically and develop a simple building principle that predicts the triatomic equilibrium configurations. As a representative example we focus on 87Rb^{87}\mathrm{Rb}87Rb trimers correlated to the n=30n=30n=30 Rydberg state. Using an exact diagonalization scheme we determine and characterize localized vibrational states in these potential minima with energy spacings on the order of 100 $\mathrm{MHz}\ifmmode\times\else\texttimes\fi{}h$.