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Journal of Physics B Atomic Molecular and Optical Physics

Theory of collisionally induced nlJ to nlJ' transitions in Rydberg states of alkalis

Leszek Sirko, K. Rosiński

Published Feb 14, 1991• 5 citations
Publisher

Abstract

The authors have presented a theoretical description of nlJ to nlJ' transitions in alkali metal atoms colliding with noble gas atoms and N 2 . The theory is based on application of the Fermi pseudopotential and first-order perturbation theory. The theory provides good agreement with experimental results for J-mixing in D states of Cs.

DOI
10.1088/0953-4075/24/3/007

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Journal of Physics B Atomic Molecular and Optical Physics•Jan 10, 2002•7 citations
The authors have presented a theoretical description of nlJ to nlJ' transitions in alkali metal atoms colliding with noble gas atoms and N 2 . The theory is based on application of the Fermi pseudopotential and first-order perturbation theory. The theory provides good agreement with experimental results for J-mixing in D states of Cs.
It is shown for the first time that the theoretical model for the collisional l mixing in atomic intermediate Rydberg states proposed by de Prunele and Pascale (1979) can also be applied to J mixing in the intermediate Rydberg states with higher quantum defect delta l values and not only to collisions with noble gas atoms and N 2 but also with ground-state alkali atoms. The model is applied to the calculation of J-mixing cross sections of nD Rydberg states of Rb (n=7-10) and Cs (n=9-23) perturbed by noble gas atoms and N 2 . J mixing in Cs(nD)-Cs(6S 1 2/)(n=11-23) collisions is also considered. The agreement with the available results is rather good.
Collisional broadening of nS Rydberg states by K, Rb, and Cs atoms is studied using the adiabatic approach for the $^{3}\mathrm{\ensuremath{\Sigma}}$ quasimolecular state and impulse approximation for all other contributions to the collisional width. The calculations are based on the use of the low-energy phase shifts for electron scattering by alkali metals obtained from ab initio close-coupling calculations and their extrapolation according to the modified effective range theory. We obtain a good agreement for the magnitude of the width with experimental data and satisfactory agreement for the oscillatory part of the width as a function of the principal quantum number. We find that the theory overestimates the amplitude of the oscillations. In the case of Cs as a perturber, the agreement with experimental data is good if we assume the existence of the low-energy 3^{3}3P resonance of ${\mathrm{Cs}}^{\mathrm{\ensuremath{-}}}$. However, recent ab initio bound-state and scattering calculations indicate the existence of the Cs (3{(}^{3}(3P) bound state rather than the resonance.
We have presented a theoretical description of J-mixing (the transfer of excitation between fine structure) cross sections of a Rydberg Cs atom induced by thermal collisions with noble-gas atoms. The theory is based on the application of impulse approximation theory and a kind of model-potential wave function. The results agree well with available recent experimental values for He, Ne, and Ar atoms. But for the heavier noble-gas atoms Kr and Xe, the theoretical cross sections are larger than the experimental ones.
The J-mixing process of alkali-metal atoms in thermal collisions with noble-gas atoms has been a nemesis due to the fact that the process is a complicated three-body collision process. Since current theoretical methods treat the collision process as a two-body one by ignoring the interaction between the perturber noble-gas atom and the alkali-metal atomic core, their results do not agree with experiments, especially in lower-n states and for heavier noble-gas atoms. Within the framework of an eikonal approximation in this paper, we have presented a theoretical description of the J-mixing process of alkali-metal atoms. Our present work shows that the direct contribution to the process from the interaction between the perturber atom and the alkali-metal atomic core is negligible, but the interaction makes its effect felt within a higher-order term which depends on the perturber-core total cross section ${\mathrm{\ensuremath{\sigma}}}_{\mathrm{tot}}^{\mathit{A}+\mathrm{\ensuremath{-}}}$B and the matrix element 〈${\mathit{r}}^{\mathrm{\ensuremath{-}}2}$〉nl{\mathrm{〉}}_{\mathit{n}\mathit{l}}〉nl​. The theoretical cross sections obtained for Cs and Rb atoms' J-mixing processes exhibit a similar dependence on the principal quantum number n as the experimental results, expecially in the lower-n states and for the heavier noble-gas atoms.
In this paper we present the results and discuss the applicability of an impact theory of lineshapes, developed by Henry and Herman for the pressure-induced broadening and shifting of transitions from the ground state to various Rydberg states of alkalis, to the situation in which the perturbing atoms are ground-state rare gas atoms. This theory, which has successfully described the collisional broadening of Rydberg states by alkali atoms, can without major alterations predict the widths and shifts of Doppler-free two-photon transitions to n S and n D states of Rb and Na, 6⩽ n ⩽30, perturbed by He, Ne, Ar, Kr and Xe. The results in all cases show reasonable agreement with experiment, with the transitions to Na**( n D) states being somewhat less satisfactory than the others.