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Journal of Physics B Atomic and Molecular Physics

Theoretical model for the collision of high Rydberg atoms with neutral atoms or molecules

E. de Prunelé, J. Pascale

Published Aug 14, 1979• 77 citations
Publisher

Abstract

A theoretical model for the collision of atoms in high Rydberg states (nl) with neutral atoms or molecules is proposed, based on the assumption that the electron-perturber interaction is of very short range compared with the mean radius of the Rydberg atom. A semiclassical method is used to derive a compact expression for the collision probability. The calculations need total cross sections for the scattering of a free and low-energy electron by the perturber. The model is applied to the calculation of a free and low-energy electron by the perturber. The model is applied to the calculation of cross sections for the quenching of n 2 D or n 2 F Rydberg states of Na and Rb by rare-gas atoms of N 2 . On the whole the calculated cross sections are in reasonable agreement with experimental data for n>10 approximately. The model and the results of the calculations are discussed and compared with other theoretical works.

DOI
10.1088/0022-3700/12/15/013

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A theoretical model for the collision of atoms in high Rydberg states (nl) with neutral atoms or molecules is proposed, based on the assumption that the electron-perturber interaction is of very short range compared with the mean radius of the Rydberg atom. A semiclassical method is used to derive a compact expression for the collision probability. The calculations need total cross sections for the scattering of a free and low-energy electron by the perturber. The model is applied to the calculation of a free and low-energy electron by the perturber. The model is applied to the calculation of cross sections for the quenching of n 2 D or n 2 F Rydberg states of Na and Rb by rare-gas atoms of N 2 . On the whole the calculated cross sections are in reasonable agreement with experimental data for n>10 approximately. The model and the results of the calculations are discussed and compared with other theoretical works.
A theory of inelastic n,l-changing and quasielastic l-mixing collisions of Rydberg atoms with the heavy rare-gas atoms is developed. It is based on the semiclassical impact-parameter approach combined with the normalized perturbation theory. Semiclassical formulas for scaled transition probabilities and cross sections as functions of the inelasticity parameter and the collision strength are analyzed. This approach gives a general description of collisional nl\ensuremath{\rightarrow}${\mathit{n}}^{\ensuremath{'}}$ transitions independently of the specific values of the principal quantum number, the relative velocity, and the type of colliding atoms. The energy and angular dependence of the electron-atom scattering amplitude is included in the theory by incorporating the impulse-approximation results in the weak-coupling limit. The Ramsauer-Townsend effect affects significantly the values of the cross sections, especially for the inelastic transitions with large energy transfer. The results obtained are used in calculations of the quenching cross sections for the Rb(nS,nD,nF) atoms in collisions with Ar, Kr, and Xe. Comparison of theory and experiment is made in a wide range of the principal quantum numbers and transition energy defects. \textcopyright{} 1996 The American Physical Society.
Simple analytical expressions for the cross sections of nl to n'l' transitions from Rydberg-neutral inelastic collisions are obtained on the basis of the free electron model for electron-perturber scattering. The dependences of the electron-perturber scattering amplitude on the electron momentum and scattering angle are allowed for. The analytical results agree well with available numerical calculations. The analysis of the equations obtained yields a conclusion that the cross sections at l<or=l' depend weakly on l and l' for degenerate states and are proportional to the statistical weights of the final states for transitions with large energy defects.
The author obtains simple analytical expressions for the cross sections of the state-changing and ionisation collisions of Rydberg atoms with neutral atomic particles due to the Rydberg-electron-perturber interaction. The theoretical investigation is based on the impulse approximation and binary encounter approach for the form factor. The earlier results of Alekseev and Sobel'man (1965) and Omont (1977) turn out to be the limiting cases of the author's expressions. The calculated quenching cross sections for the Rydberg states agree well with experimental results and numerical calculations.
Semiclassical calculations of the quasi-elastic l-mixing and inelastic n,l-changing processes in thermal collisions of a Rydberg sodium atom with rare-gas atoms (Ne, Ar, Kr and Xe) as well as and atoms with Ne are presented in a wide range of principal quantum numbers. The main emphasis is put on the study of the effects in the Rydberg-atom - rare-gas-atom collisions associated with both the short- and long-range (polarization) parts of the electron - perturber interaction. It is shown that the polarization interaction between the highly excited electron and the Ne atom provides the major contribution to the cross section of the l-mixing and n, l -changing transitions. We show that the Ramsauer - Townsend effect in slow electron scattering by the heavy rare-gas atoms significantly affects the values of the cross sections, particularly for the inelastic transitions with large energy transfer. A quantitative explanation of these phenomena is given using the recently developed semiclassical normalized perturbation theory for the Rydberg-atom - neutral collisions combined with the modified effective range theory for scattering of slow electrons by the rare-gas atoms.
A classical model for l mixing of Rydberg states in atomic collisions is described. The primary assumption of the model is that l changing occurs in a single hard-sphere collision between the Rydberg electron and the perturbing atom which is represented by the zero-energy scattering length L. Predictions of the model, which are in the form of cross sections as functions of principal quantum number n, are compared with data for l mixing of Na(nd) and Rb(nf) by rare-gas atoms. Agreement is, in most cases, quite good, comparable with that of other, more sophisticated, models. It is shown that, because the calculation must be carried out in the reference frame of the ion core, the energy deficit between low angular momentum states and the nearest hydrogenic manifold can be made up in a single collision between the Rydberg electron and the perturbing atom, an effect that is analogous to the gravitational slingshot effect used to alter the orbits of a spacecraft under the influence of the Sun's gravitational field. Comparison of data for l mixing by ground-state Rb atoms with model calculations in which L is treated as a free parameter leads to an estimate of 10 a.u. for the zero-energy scattering length of Rb.
Atoms in highly excited Rydberg states possess physical characteristics quite unlike those associated with atoms in the ground or low-lying excited states. In particular, they are physically very large and are only very weakly bound. In consequence, collisions can lead to a wide variety of reaction processes many of which are unique to Rydberg species and have very large collision cross sections. In collisions with neutral targets, Rydberg atoms behave not as an atom but rather as a pair of well-separated independent scatterers, namely the core ion and the excited Rydberg electron. In the present article we discuss many of the different reactions that can occur when Rydberg atoms collide with neutral targets, focusing principally on reactions that are dominated by (binary) Rydberg electron-target interactions and include collisions with molecules that attach free low-energy electrons and with polar targets. In certain situations, however, interactions involving the Rydberg core ion are important. This is illustrated using as an example the destruction of ultralong-range Rydberg molecules excited in a cold dense gas.