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Physical Review A

Excitation and deexcitation processes in slow collisions of Rydberg atoms with ground-state parent atoms

R.K. Janev, A. A. Mihajlov

Published Nov 1, 1979• 44 citations
Publisher

Abstract

The excitation and deexcitation processes in slow collisions of highly excited (Rydberg) atoms with ground-state parent atoms are considered. A mechanism, based on the quasiresonant energy transfer within the electronic part of the colliding system, is proposed for these processes. Both direct and exchange reaction channels are included into the treatment. Expressions for the $n\ensuremath{\rightarrow}{n}^{\ensuremath{'}}$ transition probabilities are obtained in closed form. Probability and cross section calculations for some transitions and level decays in the ${\mathrm{H}}^{*}(n)$-H system are presented.

DOI
10.1103/physreva.20.1890

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Total cross sections for quenching of low-n Rydberg states of Li $(n<10,$ $l=0)$ in collision with the ground state He have been calculated in the low-energy region $(v<~0.1\mathrm{a}.\mathrm{u}.)$ by employing the molecular orbital approximation. Results for the total depopulation of the parent states, along with those for excitation and de-excitation mechanisms have been presented. Present cross sections exhibit the low-energy Stueckelberg oscillations. Using a model two-state calculation we present a detailed comparative study between the quantum-mechanical and semiclassical findings. Except at very low energies, the semiclassical cross sections agree nicely with their quantum counterparts. The reaction rates at thermal energies are also reported.

Physical Review A•Feb 11, 2000•2 citations
The excitation and deexcitation processes in slow collisions of highly excited (Rydberg) atoms with ground-state parent atoms are considered. A mechanism, based on the quasiresonant energy transfer within the electronic part of the colliding system, is proposed for these processes. Both direct and exchange reaction channels are included into the treatment. Expressions for the n\ensuremath→n\ensuremath′n\ensuremath{\rightarrow}{n}^{\ensuremath{'}}n\ensuremath→n\ensuremath′ transition probabilities are obtained in closed form. Probability and cross section calculations for some transitions and level decays in the H∗(n){\mathrm{H}}^{*}(n)H∗(n)-H system are presented.
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.
The process of ionization in slow-atom-Rydberg-atom collisions is investigated. A resonant energy exchange mechanism is considered responsible for the electron transition into the continuum. Both symmetrical and asymmetrical systems are considered. The ionization probabilities and cross sections for a number of Rydberg states in the colliding systems H∗(n)+H{\mathrm{H}}^{*}(n)+\mathrm{H}H∗(n)+H, Li∗(n)+Li{\mathrm{Li}}^{*}(n)+\mathrm{Li}Li∗(n)+Li, H∗(n)+Li{\mathrm{H}}^{*}(n)+\mathrm{Li}H∗(n)+Li are calculated.
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.
First Major Highlight: Collisional Stark Mixing at ultralow energies in Rydberg Plasmas. Atoms in high (n,l) states formed in cold Rydberg plasmas decay to the ground state in a succession of radiative transitions populating intermediate excited states. Which states are populated during cascading and with what probability can be obtained from known transition probabilities. Classical models simplify the calculation considerably, revealing the "trajectory" in nt space followed during the cascade, scaling rules and other aspects hidden within the quantal approach. Conserved Quantity (quantal analogue obscure): Quantal-Classical correspondence in radiative recombination and decay is directly demonstrated. Classical transition probabilities and radiative, recombination cross-section are in excellent agreement with quantal results. Cross section for three body collisional capture is formulated for arbitrary electron-energy distributions.
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.
Total cross sections for quenching of low-n Rydberg states of Li (n<10,(n<10,(n<10, l=0)l=0)l=0) in collision with the ground state He have been calculated in the low-energy region (v< 0.1a.u.)(v<~0.1\mathrm{a}.\mathrm{u}.)(v< 0.1a.u.) by employing the molecular orbital approximation. Results for the total depopulation of the parent states, along with those for excitation and de-excitation mechanisms have been presented. Present cross sections exhibit the low-energy Stueckelberg oscillations. Using a model two-state calculation we present a detailed comparative study between the quantum-mechanical and semiclassical findings. Except at very low energies, the semiclassical cross sections agree nicely with their quantum counterparts. The reaction rates at thermal energies are also reported.