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Physical Review A

Observation of strong electronic correlation for highly excited double Rydberg states of ytterbium

Wenbo Huang, Xiang-Yuan Xu, C. B. Xu, M. Xue, L. Q. Li, D. Y. Chen

Published Feb 1, 1994• 14 citations
Publisher

Abstract

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.

DOI
10.1103/physreva.49.r653

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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.
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.
The atomic triply excited double Rydberg states (TEDRS) of La have been studied both experimentally and theoretically. It is revealed that in such an asymmetric four-body system where three electrons have very different orbital energies, the electronic correlations can be understood by means of decomposing into different dielectronic correlations that play different roles time-dependently. The correlations depend strongly on the relative excited orbital energies of three valence electrons. Our theoretical approach based on a semiclassical model is able to interpret the two observed patterns of La+{\mathrm{La}}^{+}La+ ion distributions among high Rydberg states resulted from the decay of TEDRS.
The autoionization distribution of the triply excited double Rydberg states (TEDRS) 5 d 5/2 N Lnl ( N ⩽ 22; n ⩽ 50; L, l < 4) of La has been investigated by using five-laser resonance excitation in combination with a method of sequential ionization by a pulsed electric field and a constant electric field. The experimental results exhibit that the La atoms in TEDRS predominantly single-autoionize to the ionic Rydberg states located in a few Rydberg manifolds. Furthermore, a difference of autoionization mechanisms between TEDRS above and those below the double ionization threshold is found.