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Journal of Physics B Atomic Molecular and Optical Physics

Nonadiabatic mechanism of the quenching of the alkali atoms Rydberg states in collisions with atoms of the same type

V. M. Borodin, Andrey K. Kazansky

Published Aug 14, 1989• 0 citations
Publisher

Abstract

The nonadiabatic mechanism of the quenching of the alkali atoms' Rydberg states in collisions with atoms of the same type, is described. The diabatic energy curves depend on the internuclear distance due to internuclear axis rotation and transitions are produced by the polarisation interaction of the atom with the Rydberg electron. It is shown that the cross sections of the processes may be large enough: sigma approximately 103-104 au and the principal role of classically forbidden nuclear configurations is exposed. The results are shown to be dependent on the type of Rydberg atom.

DOI
10.1088/0953-4075/22/15/002

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•Jan 1, 1995•0 citations
The nonadiabatic mechanism of the quenching of the alkali atoms' Rydberg states in collisions with atoms of the same type, is described. The diabatic energy curves depend on the internuclear distance due to internuclear axis rotation and transitions are produced by the polarisation interaction of the atom with the Rydberg electron. It is shown that the cross sections of the processes may be large enough: sigma approximately 103-104 au and the principal role of classically forbidden nuclear configurations is exposed. The results are shown to be dependent on the type of Rydberg atom.
The adiabatical mechanism of the oscillations of the broadened cross sections produced by collisions of Rydberg alkali atoms with ground-state atoms of an ambient alkali gas is presented. The dependence of the oscillations of the cross sections on the principal quantum number n arises due to the oscillations of the mixing parameter for the pseudocrossing between the 3 P ion state energy curve of the ambient gas atom and the Rydberg state dependent on n. The latter oscillations are generated by the oscillations of the Rydberg electron wavefunction in the coordinate space. The numerical results obtained are in good agreement with the experimental data for different colliding pairs. The matching of the adiabatical picture and the conventional impulse approximation is discussed.
We report the results of comparative studies of ion-pair formation and quenching processes in collisions of Rydberg Li( nl ) and Cs( nl ) atoms with Ca(4s 2 ), Sr(5s 2 ) and Ba(6s 2 ) atoms possessing small electron affinities. Our consideration includes both the cases of selectively excited Rydberg nl -states with small orbital angular momentum ( l ≪ n ) and nearly circular states with l ∼ n − 1. Calculations of the electron-transfer processes are based on the semiclassical theory of nonadiabatic transitions and exact expression for the Rydberg-covalent–ionic coupling terms. Calculations of nonresonant quenching processes are carried out within the framework of the available theory of inelastic and quasielastic transitions between Rydberg-covalent states. The ion-pair formation and resonant quenching cross sections are shown to be significantly dependent not only on the principal quantum number n but also on the orbital angular momentum l and the binding energy of the alkaline-earth anion. For each system under study we find the regions of n in which either the resonant quenching or the ion-pair formation processes are predominant. The relative role of the resonant and nonresonant mechanisms of depopulation of Rydberg states is investigated.
The results of theoretical investigations of the excitation, quenching, ionization and broadening of the Rydberg atomic levels in inelastic collisions with ground‐state atoms of buffer or parent gases are presented. The different physical mechanisms of these processes due to the scattering of the perturbing neutral particle on the quasifree electron and on the core of the Rydberg atom are considered. In particular the role of the potential and resonance scattering of the slow electron on the perturbing atoms in the quenching and broadening processes is discussed. The effects of the nonadiabatic transfer of the Rydberg electron energy to the kinetic energy of the colliding atoms and to the energy of the electronic shell of the quasimolecular ion are also considered. The results of calculations of the cross sections and the rate constants of the quenching, boradening and ionziation processes for some physcial systems are presented and are compared with available experimental data.
We use the adiabatic theory in the complex plane of internuclear distance to calculate the Rydberg-state broadening cross sections in the ambient alkali-metal gases. We have found that the imaginary parts of the branch points between the relevant energy curves have an oscillatory structure that is projected into a similar structure in the broadening cross section. The results of the distorted-wave diabatic perturbation theory and the present theory are in excellent agreement for the principal quantum numbers of the Rydberg atoms n30. Unlike the diabatic perturbation theory, the adiabatic approach does not merge with the impulse approximation and fails for higher n.
Abstract The results of theoretical studies of the resonant quenching and ion-pair formation processes induced by collisions of Rydberg atoms with highly polar molecules possessing small electron affinities are reported. We elaborate an approach for describing collisional dynamics of both processes and demonstrate the predominant role of resonant quenching channel of reaction for the destruction of Rydberg states by electron-attaching molecules. The approach is based on the solution of the coupled differential equations for the transition amplitudes between the ionic and Rydberg covalent terms of a quasimolecule formed during a collision of particles. It takes into account the possibility of the dipole-bound anion decay in the Coulomb field of the positive ionic core and generalizes previous models of charge-transfer processes involving Rydberg atoms to the cases, when the multistate Landau–Zener approaches become inapplicable. Our calculations for Rb ( nl ) atom perturbed by C 2 H 4 SO 3 , CH 2 CHCN , CH 3 NO 2 , CH 3 CN , C 3 H 2 O 3 , and C 3 H 4 O 3 molecules show that the curves representing the dependence of the resonant quenching cross sections on the principal quantum number n are bell-shaped with the positions of maxima being shifted towards lower values of n and the peak values, σ max ( q ) , several times higher than those for the ion-pair formation, σ max
This dissertation deals with thermal collisions of highly excited (Rydberg) atoms with atoms in the ground state. The inelastic processes in these collisions manifest themselves mainly in broadening of Rydberg spectral lines. Advancements in tunable laser techniques allowed observation of the ion-pair formation in such collisions as well. Theoretical treatments of these collisions can be separated in two groups according to the principal quantum number n of the Rydberg atom: impulse approximation (n≥30),(n\ge30),(n≥30), and adiabatic approximation (n≤20).(n\le20).(n≤20). Both approaches are presented in application to spectral line broadening. The off-shell modification of the impulse approximation is developed. The pseudopotentials for singlet and triplet electron scattering from Rb and Cs are re-constructed from the phase shift data. These potentials are used to calculate the off-shell amplitudes, which are employed to obtain broadening cross sections. The taking into account of the off-shell effects is shown to improve the agreement with the experiment in the intermediate region of principal quantum number 20<n<30.20 < n < 30.20<n<30. The adiabatic approximation in the framework of Borodin-Kazansky theory is improved to include the exact Coulomb Green's function and the final radius of the ground state atom. The adiabatic theory explains the oscillations with n in the experimental broadening cross sections. The adiabatic theory is developed for the ion-pair formation. The zero-range-potential-Coulomb-field model is employed to generate realistic energy curves. The model allows exact numerical solution, which is used to verify the analytical theory that is set forth to describe the non-adiabatic transitions at large internuclear distances. Adiabatic calculations rely on the complex plane technique that requires the analytical continuation of the energy curves in the complex plane of parameters. Development of the algorithms for the continuation of Mathieu and Whittaker's functions, used in these calculations, constitutes an important methodological achievement of this work. Although all applications of the theories are worked out for alkali-metal atoms, the results can be applied to other atomic species as well.