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Journal of Physics B Atomic and Molecular Physics

Resonance interaction and self-broadening of alkali resonance lines. I. Adiabatic potential curves

Mladen Movre, Goran Pichler

Published Sep 11, 1977• 168 citations
Publisher

Abstract

Adiabatic potential curves were calculated using perturbation theory for the long-range electrostatic interaction between two alkali atoms of the same species, one being in the ground state, the other in the resonance-excited state. Comparison with recent experiments showed that the observed satellites and asymmetries in the self-broadened quasi-state wings of the alkali resonance lines are the consequence of extrema in certain potential curves between the fine-structure levels.

DOI
10.1088/0022-3700/10/13/016

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Recent theoretical studies with alkali atoms A* excited to high Rydberg states predicted the existence of ultra-long-range molecular bound states. Such excited dimers have large electric dipole moments which, in combination with their long radiative lifetimes, make them excellent candidates for manipulation in applications. This Letter reports on experimental investigations of the self-broadening of Rb principal series lines, which revealed multiple satellites in the line wings. The positions of the satellites agree quantitatively with theoretically predicted minima in the excited long-range Rydberg states of Rb2.

arXiv:physics/0609220•Physical Review Letters•Dec 8, 2006•41 citations
Adiabatic potential curves were calculated using perturbation theory for the long-range electrostatic interaction between two alkali atoms of the same species, one being in the ground state, the other in the resonance-excited state. Comparison with recent experiments showed that the observed satellites and asymmetries in the self-broadened quasi-state wings of the alkali resonance lines are the consequence of extrema in certain potential curves between the fine-structure levels.
Recent absorption measurements of the self-broadening of Rb principal series lines [C. H. Greene, E. L. Hamilton, H. Crowell, C. Vadla, and K. Niemax, Phys. Rev. Lett. 97, 233002 (2006)] verified the existence of minima in highly excited long-range potentials of Rb2{\text{Rb}}_{2}Rb2​ which were predicted theoretically as bound Rydberg molecule [C. H. Greene, A. S. Dickinson, and H. R. Sadeghpour, Phys. Rev. Lett. 85, 2458 (2000)]. The present paper reports on the extension of these experimental studies to principal series lines of K broadened by K as well as Cs broadened by Cs. In addition, the broadening of some lower members of the K, Rb, and Cs principal line series due to heteroatomic interactions was investigated. The analysis of the measured satellite structures in the quasistatic line wings and their comparison to the previously published analogous data for ${\text{Rb}}^{\ensuremath{\ast}}+\text{Rb}$ system lead to the conclusion that one can expect existence of potential minima in homo- and heteroatomic alkali-metal ${A}^{\ensuremath{\ast}}+B$ systems in a wide range of principal quantum numbers, starting with K, Rb, and Cs excited to the third resonance states. The positions and strengths of the satellite structures indicate that the potential minima are due to scattering of the valence electron by ground-state perturbers.
In addition to previous absorption measurements of Cs resonance lines, new investigations on Na, K and Rb also showed definitely that beyond symmetrical Lorentzian central parts of the lines, the stronger components of the resonance lines have blue and the weaker components red asymmetry. This behaviour can be explained by a quasistatic treatment of the self-broadening mechanism taking interatomic interaction potentials into account. But with additional data it is now possible to give a different interpretation of the origin of observed asymmetries than suggested in the previous paper on Cs resonance lines (see abstr. A5740 of 1975). The asymmetries are shown to arise from the mutual repulsion of two potential curves of the same species.
The authors outline an asymptotic calculation of adiabatic potential curves for diatomic quasimolecular systems that happens to be quite accurate in the domain of long-range forces, even for atoms with complex electronic configurations. A formula for the molecular oscillator strength expressed via the oscillator strengths of the constituent atoms and the eigenfunctions of the effective Hamiltonian is presented. Quite general theoretical results on the electrostatic interaction within these quasimolecular systems are then applied to a calculation of the dipole-dipole interaction for the quasimolecule Eu-Sr, leading to the adiabatic potentials in the region of interatomic distances larger than approximately 1.0 nm. These results are checked by comparing the quasistatic absorption coefficient for the blue quasistatic wing of the Eu resonance line broadened by the influence of Sr atoms to the experimentally derived profile [K. Niemax, Phys. Rev. Lett. 55. 56 (1985)]. Excellent agreement is obtained. A great influence of the molecular oscillator strengths on the shape of the quasistatic profile is found, so that, in general, the character of the interaction potential could not be judged from log-log plots of the absorption coefficient alone.
The purpose of this work is the evaluation of the linewidth w and lineshift d of the sodium resonance line 3p − → 3s when the excited atoms are evolving in their parent gas. Assuming the Baranger impact approximation, these two quantities are given in terms of the phase shifts of the ground Na(3s) + Na(3s) and the excited Na(3p)+Na(3s) states. The quantal calculations and the semi-classical method, developed by Mott and Massey and Landau and Lifshitz, show that the cross sections σ and λ vary with the energy like E−1/2, the width w and the shift d do not depend on the temperature, the long-range interactions have a big influence on w and d, and the rate coefficients depend on the dispersion coefficients like w/n ≈ +7.298 × 10−8C3(Σ) and d/n ≈ +8.893 × 10−9C3(Σ). The study also shows that the sodium results can be extended to the other alkali-metal atoms (Li, K, Rb, Cs, and Fr) by a simple scaling. Keywords: potential energy curve, broadening cross section, rate coefficient, linewidth, lineshift, dispersion coefficient
Experiments have revealed that pressures of noble gases cause bands to appear in both the red and violet wings of the alkali doublet lines. The present paper is devoted to the explanation of these bands and to the shift and shape of the doublet lines which they accompany. In order to examine various qualitative proposals previously put forth to this end, we first ascertain the validity of the statistical theory as applied to the magnetic substates of the alkali resonance lines and develop a criterion for adiabaticity. This criterion indicates that the earlier theories are inadequate. Shift and broadening of the two components of the alkali doublet lines are then calculated as functions of noble gas density by considering the van der Waals energy perturbation due to n simultaneously acting perturbers. The conclusion, which is in agreement with experiments, is that the P322 resonance line is shifted and broadened more than the 2P½ resonance line at moderate pressures. A phenomenological approach is used to construct a more reasonable theory of the ``satellite'' bands. In the absence of reliable knowledge concerning the repulsive portions of the interaction curves, only a semiquantitative understanding of the data is achieved.
Recent theoretical studies with alkali atoms A* excited to high Rydberg states predicted the existence of ultra-long-range molecular bound states. Such excited dimers have large electric dipole moments which, in combination with their long radiative lifetimes, make them excellent candidates for manipulation in applications. This Letter reports on experimental investigations of the self-broadening of Rb principal series lines, which revealed multiple satellites in the line wings. The positions of the satellites agree quantitatively with theoretically predicted minima in the excited long-range Rydberg states of Rb2.