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Physical Review A

Semiclassical approach to Rydberg-atom intercombination transitions in collisions with electrons

M. I. Syrkin

Published Sep 1, 1994• 8 citations
Publisher

Abstract

The intercombination transitions between l-resolved Rydberg levels due to collisions with fast electrons are studied within the Ochkur approximation for principal quantum numbers n\ensuremath{\le}20, where l is the angular momentum. The use of the Heisenberg correspondence principle for radial integrals enables one to obtain analytic expressions for any term in the multipole expansion of the cross section for collisions with an arbitrary n and l change. For transitions involving angular momenta that are small compared to the principal quantum numbers, the semiclassical and the exact results are found to be fairly close, within the accuracy consistent with the Born approximation. As a result, the semiclassical approach furnishes a ready estimate for cross sections, and its validity range proves broad enough to cover the region of large momenta transferred to the atom. The numerical results also confirm that dipole transitions have no dominance over the collisions with other \ensuremath{\Delta}l values, in accord with the general model of intercombination scattering.

DOI
10.1103/physreva.50.2284

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The intercombination transitions between l-resolved Rydberg levels due to collisions with fast electrons are studied within the Ochkur approximation for principal quantum numbers n\ensuremath{\le}20, where l is the angular momentum. The use of the Heisenberg correspondence principle for radial integrals enables one to obtain analytic expressions for any term in the multipole expansion of the cross section for collisions with an arbitrary n and l change. For transitions involving angular momenta that are small compared to the principal quantum numbers, the semiclassical and the exact results are found to be fairly close, within the accuracy consistent with the Born approximation. As a result, the semiclassical approach furnishes a ready estimate for cross sections, and its validity range proves broad enough to cover the region of large momenta transferred to the atom. The numerical results also confirm that dipole transitions have no dominance over the collisions with other \ensuremath{\Delta}l values, in accord with the general model of intercombination scattering.
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.
The analytical formulae for the cross-sections with arbitrary change {triangle}n=n{prime}-n and {triangle}1=1{prime}-1 has been obtained in the Born limit. No spin exchange {triangle}S=0: although the total cross-sections n->n are dominated by dipole transitions, the non-dipole transitions {triangle}1>1 can contribute up to 30-50%ER for large {triangle}n>>1. Intercombination transitions {triangle}S=1: the large transfer transitions {triangle}1>>1 are of major importance, as opposed to the previous case.
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.
The title process with simultaneous rotational deexcitation of molecules was investigated theoretically by using the semiquantal approximation. The dipole Born and dipole Glauber differential cross sections were employed for the electron-molecule rotational deexcitation process. Numerical applications were made to the following systems: Xe+CO, HCl, HF, and LiF. A comparative study of the two approximations was carried out concerning the dependences of the cross sections on the following various quantities: n (principal quantum number), J (initial rotational quantum number), \ensuremath{\Delta}J (rotational quantum number change), D (dipole moment), V (relative collision velocity). As the molecular dipole moment becomes larger, there appears a prominent difference in the n dependence of the cross section. The Glauber approximation brings about a decrease in the cross section and yields a sawlike n dependence in contrast to a steplike n dependence in the case of the Born approximation. In the collisions involving lowly excited Rydberg atoms, ionization with simultaneous dipole-forbidden transition of a molecule becomes dominant compared to the ionization with simultaneous dipole-allowed transition. The cross section was found to be inversely proportional to the relative collision velocity; thus the ionization rate becomes independent of temperature. A comparison was also made between the experiment for the ionization rate at 300 K for Xe(27f)+HF and Xe(31f)+HCl.
In collisions of Rydberg atoms with charged projectiles at velocities approximately matching the speed of the Rydberg electron vn{v}_{n}vn​ (matching velocity), nnn being the principal quantum number of the Rydberg level, the dipole-forbidden transitions with large angular-momentum transfer $\ensuremath{\Delta}l\ensuremath{\gg}1$ substantially dominate over dipole-allowed transitions $\ensuremath{\Delta}l=1$, although both are induced by the dipole interaction. Here it is shown that as the projectile velocity decreases the adiabatic character of the depopulation depends on the energy distribution of states in the vicinity of the initial level. If the spectrum is close to degeneracy (as for high-lll levels) the dipole-forbidden depopulation prevails practically over the entire low-velocity region, down to velocities $\ensuremath{\sim}{n}^{3}[\frac{\ensuremath{\Delta}E}{\mathrm{Ry}}]{v}_{n}$, where $\ensuremath{\Delta}E$ is the energy spacing adjoining to the level due to either a quantum defect or the relevant level width or splitting, whichever is greater. If the energy gaps are substantial (as for strongly nonhydrogenic sss and ppp levels in alkali-metal atoms), then the fraction of dipole transitions in the total depopulation reaches a flat minimum just below the matching velocity and then grows again, making the progressively increasing contribution to the low-velocity depopulation. The analytic models based on the first-order Born amplitudes (rather than the two-level adiabatic approximation) furnish reasonable estimates of the fractional dipole-allowed and dipole-forbidden depopulations.
Collisions of Rydberg atoms with other atoms may induce changes in the electronic orbital angular momentum of the Rydberg state. A theory is presented that expresses the cross section for this process in terms of the sss-wave amplitude for low-energy-electron scattering from the other atom. In its most accurate form, the theory requires a convolution of the electron-scattering amplitude and the initial momentum-space wave function of the Rydberg state. However, an approximate analytic solution is derived in which the lll-mixing cross section at a particular nnn is written as the electron-scattering cross section at the mean electronic kinetic energy of the Rydberg state, multiplied by a scaling function that depends only on nnn. The analytic solution clearly exhibits the asymptotic scaling behavior of the cross sections. Collisions of Na(nd)+He\mathrm{Na}(\mathrm{nd})+\mathrm{He}Na(nd)+He, Ne, and Ar are treated as specific examples.