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arXiv:1603.02990 · Journal of Physics B Atomic Molecular and Optical Physics

Mapping trilobite state signatures in atomic hydrogen

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

Published Jun 20, 2016• 21 citations
arXivHTMLPDF

Abstract

Abstract A few-body approach relying on static line broadening theory is developed to treat the spectroscopy of a single Rydberg excitation to a trilobite-like state immersed in a high density ultracold medium. The present theoretical framework implements the recently developed compact treatment of polyatomic Rydberg molecules, allowing for an accurate treatment of a large number of perturbers within the Rydberg orbit. This system exhibits two unique spectral signatures: its lineshape depends on the Rydberg quantum number n but, strikingly, is independent of the density of the medium, and it is characterized by sharply peaked features reflecting the oscillatory structure of the potential energy landscape.

DOI
10.1088/0953-4075/49/14/14lt01

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Abstract A few-body approach relying on static line broadening theory is developed to treat the spectroscopy of a single Rydberg excitation to a trilobite-like state immersed in a high density ultracold medium. The present theoretical framework implements the recently developed compact treatment of polyatomic Rydberg molecules, allowing for an accurate treatment of a large number of perturbers within the Rydberg orbit. This system exhibits two unique spectral signatures: its lineshape depends on the Rydberg quantum number n but, strikingly, is independent of the density of the medium, and it is characterized by sharply peaked features reflecting the oscillatory structure of the potential energy landscape.
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 $\mathrm{MHz}\ifmmode\times\else\texttimes\fi{}h$.
We present spectroscopy of a single Rydberg atom excited within a Bose-Einstein condensate. We not only observe the density shift as discovered by Amaldi and Segrè in 1934, but a line shape that changes with the principal quantum number n. The line broadening depends precisely on the interaction potential energy curves of the Rydberg electron with the neutral atom perturbers. In particular, we show the relevance of the triplet p-wave shape resonance in the e^{-}-Rb(5S) scattering, which significantly modifies the interaction potential. With a peak density of 5.5×10^{14} cm^{-3}, and therefore an interparticle spacing of 1300 a_{0} within a Bose-Einstein condensate, the potential energy curves can be probed at these Rydberg ion-neutral atom separations. We present a simple microscopic model for the spectroscopic line shape by treating the atoms overlapped with the Rydberg orbit as zero-velocity, uncorrelated, pointlike particles, with binding energies associated with their ion-neutral separation, and good agreement is found.
Abstract Sufficiently high densities in Bose–Einstein condensates provide favorable conditions for the production of ultralong-range polyatomic molecules consisting of one Rydberg atom and a number of neutral ground state atoms. The chemical binding properties and electronic wave functions of these exotic molecules are investigated analytically via hybridized diatomic states. The effects of the molecular geometry on the system’s properties are studied through comparisons of the adiabatic potential curves and electronic structures for both symmetric and randomly configured molecular geometries. General properties of these molecules with increasing numbers of constituent atoms and in different geometries are presented. These polyatomic states have spectral signatures that lead to non-Lorentzian line-profiles.
This work presents a theoretical approach for lineshapes of Rydberg excitations in high-density media. In particular, we introduce the quasi-static lineshape theory, leading to a methodic and general approach, and its validity is studied. Next, using 84Sr as a prototypical scenario, we discuss the role of the thermal atoms and core–perturber interactions, generally disregarded in Rydberg physics. Finally, we present a characterization of the role of Rydberg–core perturber interactions based on the density and principal quantum number that, beyond affecting the lineshape, could potentially apply to chemi-ionization reactions responsible for the decay of Rydberg atoms in high-density media.
We perform three-photon photoassociation to obtain high resolution spectra of ^{87}Rb trilobite dimers for the principal quantum numbers n=22, 24, 25, 26, and 27. The large binding energy of the molecules in combination with a relative spectroscopic resolution of 10^{-4} provides a rigorous benchmark for existing theoretical models. A recently developed Green's function framework, which circumvents the convergence issues that afflicted previous studies, is employed to theoretically reproduce the vibrational spectrum of the molecule with high accuracy. The relatively large molecular binding energy is primarily determined by the low-energy S-wave electron-atom scattering length, thereby allowing us to extract the ^{3}S_{1} scattering phase shift with unprecedented accuracy, at low-energy regimes inaccessible to free electrons.
Trilobites are exotic giant dimers with enormous dipole moments. They consist of a Rydberg atom and a distant ground-state atom bound together by short-range electron-neutral attraction. We show that highly polar, polyatomic trilobite states unexpectedly persist and thrive in a dense ultracold gas of randomly positioned atoms. This is caused by perturbation-induced quantum scarring and the localization of electron density on randomly occurring atom clusters. At certain densities these states also mix with an s state, overcoming selection rules that hinder the photoassociation of ordinary trilobites.