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Physica Scripta

Correlation effects in double Rydberg atoms

Pierre Camus

Published Jan 1, 1994• 8 citations
Publisher

Abstract

The present review is devoted to the recent advances performed in alkaline-earth atoms by the selective laser preparation of autoionizing asymmetrical double Rydberg states which have, so far, not been observed in natural environments. Because the great amount of flexibility achieved by the sequential laser electron excitations, a wide choice of two-electron situations have been investigated and analyzed which exhibit spectral features due to long-range effects of the Coulomb electron-electron repulsion. To overcome the autoionization broadening of the lines, double Rydberg states with a non-core penetrating high-ℓ outer electron were produced by combining temporal laser excitation technique with the electric-field switching method. The study of the spectral correlation signatures in Nsn ℓ double Rydberg states versus ℓ allow to understand their evolution from simple spectra (ℓ ⩾ 10) due to long-range dipole interaction to more complex data (ℓ ⩽ 7) induced by short-range multipole effects when two electrons start to influence more each other.

DOI
10.1088/0031-8949/1994/t51/003

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•Dec 2, 2016•0 citations
The present review is devoted to the recent advances performed in alkaline-earth atoms by the selective laser preparation of autoionizing asymmetrical double Rydberg states which have, so far, not been observed in natural environments. Because the great amount of flexibility achieved by the sequential laser electron excitations, a wide choice of two-electron situations have been investigated and analyzed which exhibit spectral features due to long-range effects of the Coulomb electron-electron repulsion. To overcome the autoionization broadening of the lines, double Rydberg states with a non-core penetrating high-ℓ outer electron were produced by combining temporal laser excitation technique with the electric-field switching method. The study of the spectral correlation signatures in Nsn ℓ double Rydberg states versus ℓ allow to understand their evolution from simple spectra (ℓ ⩾ 10) due to long-range dipole interaction to more complex data (ℓ ⩽ 7) induced by short-range multipole effects when two electrons start to influence more each other.
Abstract In this brief review, the opportunities that the alkaline-earth elements offer for studying new aspects of Rydberg physics are discussed. For example, the bosonic alkaline-earth isotopes have zero nuclear spin which eliminates many of the complexities present in alkali Rydberg atoms, permitting simpler and more direct comparison between theory and experiment. The presence of two valence electrons allows the production of singlet and triplet Rydberg states that can exhibit a variety of attractive or repulsive interactions. The availability of weak intercombination lines is advantageous for laser cooling and for applications such as Rydberg dressing. Excitation of one electron to a Rydberg state leaves behind an optically active core ion allowing, for high- L states, the optical imaging of Rydberg atoms and their (spatial) manipulation using light scattering. The second valence electron offers the possibility of engineering long-lived doubly excited states such as planetary atoms. Recent advances in both theory and experiment are highlighted together with a number of possible directions for the future.
Using five-laser resonance excitation in combination with a method of sequential ionization by a pulsed and a constant electric field, we have observed the nearly pure spectra (the ion resonance background was greatly suppressed) for the highly excited double Rydberg states NLn'l (N\ensuremath{\gtrsim}40, N/n'\ensuremath{\gtrsim}0.5 and L,l4) of ytterbium in which the mutual penetration of the two excited wave functions is remarkable. Analysis of the spectra (relative cross section for different L states) has revealed the importance of the ``hybridization'' in the excited electron orbits which arises from the correlation of the two electrons in such highly excited states.
This paper is devoted to the autoionization process of large-angular-momentum Rydberg states. After a brief account of autoionization formalism in nonrelativistic theory and single-configuration approximation, we apply it to atomic states with one electron of large angular momentum. The dominant contribution is the direct one and the exchange contribution is ignored. In this framework, the autoionization width varies with the principal quantum number as ${n}^{\mathrm{\ensuremath{-}}3}$ and exponentially with the angular momentum. When two excited electrons interact with a spherically symmetric core, it is demonstrated that the interaction between the Rydberg electron and the core polarized by the valence electron is proportional to the interaction between the two active electrons. Using newly derived radial matrix elements, we obtain a generally good agreement between our results and experiments on barium and strontium. Large-l Rydberg states are shown to be stable versus autoionization as soon as l is about 7. Possible refinements of our method are reviewed.
The authors have studied double ionization of Ba 6snl Rydberg states through resonant two-photon excitation of 8snl double-Rydberg states with n=13 and 14 and different l. The laser intensity dependence of Ba 2+ yield measured for l>or=8, when the electrons suffer long-range dipole interaction, shows a decrease from four-photon for l=8 to less than three for l=11. The four-photon dependence is due to autoionization decay populating the Ba + (7p) levels which gives an indirect signature to the Ba 2+ production. By increasing l this decay vanishes and the data show evidence of a direct double-ionization process via planetary-electron states for l>or=10. Additional intensity measurements performed for low l=6 states strongly mixed with 5fn'l' ones by short-range multipole interaction, reveal indirect Ba 2+ production and an individual case of partial stabilization due to destructive interference leading to direct double ionization.
Cold gases of Rydberg atoms are an ideal system in which to study the novel effects of strong interatomic interactions. This thesis describes the design and construction of the world's first experiment to study Rydberg states in a cold gas of an alkaline earth metal, in this particular case strontium. We have studied a wide range of Rydberg states, and have developed a sensitive ``step-scan" spectroscopic technique that detects the spontaneous ionization of the Rydberg gas. The step-scan method is used to acquire Stark maps, and these measurements verify a single-electron model for calculating dipole matrix-elements. From the matrix-elements, interaction strengths between strontium Rydberg atoms have been calculated for the first time. The presence of two valence electrons in an alkaline earth metal, such as strontium, offers a new angle on the study of Rydberg atoms. We create doubly excited ``autoionizing" states, the first such study in a cold gas. Autoionization is used as a high yield probe of Rydberg states, and enables a study of excitation dynamics with nanosecond time-resolution. We show that autoionization can quantitatively identify and elucidate state mixing in the Rydberg gas, and probe population transfer at the very onset of ultra-cold plasma formation.
Highly excited Rydberg states, neutral atomic states with one or more electrons promoted to states of large principal quantum number n are now commonly used for producing quantum entanglement. This is facilitated through the "Rydberg Blockade" effect where the presence of a single Rydberg atom blocks excitation of further atoms in a surrounding mesoscopic volume due to strong atom-atom interactions induced by the large dipole moments associated with Rydberg atoms. In this work, we report the first observation of this phenomenon in a hot atomic beam using very high n, n ~300 - 500, strontium nF Rydberg states. Inside the blockaded volume (size around 0.1mm), the Rydberg number distribution is sub-Poissonian. However, as predicted by theoretical calculations, due to the anisotropic nature of the atom-atom interactions, the blockade is incomplete. However, the blockade effect is sufficiently strong to enable detailed study of few-body atom-atom interactions and of entanglement. Doubly-excited Rydberg states having a pair of electrons excited to high lying energy levels are typically difficult to create and are short lived because of "autoionization" resulting from electron-electron scattering. Strontium Rydberg atoms are used to study this scattering and we demonstrate an efficient mechanism to eliminate "autoionization" pointing to the production of long-lived strongly correlated two-electron-excited atomic states.