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Physical Review A

Atomic triply excited double Rydberg states of lanthanum investigated by selective laser excitation

Weidong Sun, Panpan Xue, Xiu-Ping Xie, Wenbo Huang, C. B. Xu, Z. P. Zhong, Xiang-Yuan Xu

Published Aug 13, 2001• 2 citations
Publisher

Abstract

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 ${\mathrm{La}}^{+}$ ion distributions among high Rydberg states resulted from the decay of TEDRS.

DOI
10.1103/physreva.64.031402

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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.
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.
Double Rydberg states were populated by triple electron capture in collisions of highly charged ions with atoms. The highest stabilization of states produced by triple capture at $v\ensuremath{\cong}0.2\mathrm{a}.\mathrm{u}.$ was found for binding energies of the projectile electrons near the limits of the $({2,n,n}^{\ensuremath{'}})$ and $({3,n,n}^{\ensuremath{'}})$ series. Population of triply excited double Rydberg states was confirmed by the emission of Rydberg transitions. Results are interpreted by two successive autotransfer into Rydberg states for $({3,n,n}^{\ensuremath{'}})$ states and of one-step two-electron autotransfer for $({2,n,n}^{\ensuremath{'}})$ 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.
We show that the recently observed class of long-range ion-Rydberg molecules can be divided into two families of states, which are characterized by their unique electronic structures resulting from the ion-induced admixture of quantum defect-split Rydberg nPnPnP states with different low-field-seeking high-lll states. We predict that in both cases, these diatomic molecular states can bind additional ground-state atoms lying within the orbit of the Rydberg electron, thereby forming charged ultralong-range Rydberg molecules (ULRMs) with binding energies similar to that of conventional nonpolar ULRMs. To demonstrate this, we consider a Rydberg atom interacting with a single ground-state atom and an ion. The additional atom breaks the system's cylindrical symmetry, which leads to mixing between states that would otherwise be decoupled. The electronic structure is obtained using exact diagonalization over a finite basis and the vibrational structure is determined using the multiconfiguration time-dependent Hartree method. Due to the lobelike structure of the electronic density, bound trimers with both linear and nonlinear geometrical configurations of the three nuclei are possible. The predicted trimer binding energies and excitation series are distinct enough from those of the ion-Rydberg dimer to be observed using current experimental techniques.