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The Journal of Chemical Physics

Electronic mechanisms of Penning ionization involving excited alkali atoms

M. T. Djerad, F. Gounand, Anil Kumar, M. Chéret

Published Dec 1, 1992• 7 citations
Publisher

Abstract

Penning ionization (PI) occurring during the collision of a Rydberg atom Rb(nl) with a resonant state K(4P) or Rb(5P) is analyzed theoretically. By using a semiclassical approach, we calculate the rate coefficients corresponding to both the direct and exchange decay channels. We implement the method by deriving various approximations for the exchange and direct decay widths. The radiative mechanism is found to dominate the thermal-energy quenching of alkali atoms by PI, the exchange being negligible. The calculated values are in reasonable agreement with the available experimental results.

DOI
10.1063/1.463403

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Penning ionization (PI) occurring during the collision of a Rydberg atom Rb(nl) with a resonant state K(4P) or Rb(5P) is analyzed theoretically. By using a semiclassical approach, we calculate the rate coefficients corresponding to both the direct and exchange decay channels. We implement the method by deriving various approximations for the exchange and direct decay widths. The radiative mechanism is found to dominate the thermal-energy quenching of alkali atoms by PI, the exchange being negligible. The calculated values are in reasonable agreement with the available experimental results.
Associative and Penning ionisation cross sections, rho AI and rho PI are calculated for collisions of two excited atoms Rb(nl)+Rb(5p 2 P 3 2/) in the classical impact parameter formulation for nl=5d to 9d and 7s. It is shown that the very large Penning ionisation rate constants, measured by the authors and presented earlier, can be well explained by such a model in terms of direct and exchange autoionisation widths, as well as the associative ionisation contributions which have been observed to be quite different for ns and nd cases.
The authors measure rate coefficients for Penning ionisation occurring in a vapour mixture of rubidium and potassium at thermal energy. The experimental technique uses the mass spectrometry analysis of collisional currents resulting from continuous laser excitation of the atoms. They report the first experimental evidence concerning the non-occurrence of an exchange-type mechanism. Although a second exchange-type reaction cannot be discarded by their experimental results, it seems that Penning ionisation, involving low-lying excited alkali atoms, most probably proceeds via the direct mechanism.
Abstract Penning ionisation (PI) processes involving pairs of Rydberg alkali-metal atoms, excited to different quantum states and experiencing dipole–dipole interactions, have a wide range of important properties in atomic physics. Within the framework of the semiclassical approximation, we have used both numerical and analytical approaches to examine the Penning autoionisation width dependence on the state quantum numbers in a quasi-molecule formed by the interacting partner atoms. We described the characteristics of optimal quantum numbers that lead to enhanced PI widths for the interacting Rydberg atom pairs of all alkali-metal atoms. The excited states of atoms in these pairs are asymmetric, resulting in a large atomic shell size difference: inspired by Efimov et al (2016 J. Phys. B: At. Mol. Opt. Phys. 49 125302), we call such a pair ‘Tom’ and ‘Jerry’ (for ‘big’ and ‘small’). Compared to symmetric pairs, the optimal asymmetric pairs display a significant (by several orders of magnitude) increase in the PI rate. This property makes PI a relevant source for producing charged particles in cold Rydberg systems that spontaneously evolve into cold plasma. Contrary to hydrogen atoms examined in (Efimov et al 2016 J. Phys. B: At. Mol. Opt. Phys. 49 125302), the difference in quantum defects in alkali-metal atoms results in a strong Penning width dependence on the orbital quantum numbers l of the quasi-molecule. In particular, alkali-metal atoms exhibit two PI channels associated with bound–bound optical transitions showing Δ l = ±1—individual and closely spaced (doublet-like) configurations of optimal pairs. Furthermore, we demonstrate that the presence of Förster resonances can lead to a notable (up to five times) increase in the PI efficiency.
The combined relativistic energy approach and relativistic many-body perturbation theory with the zeroth Dirac-Fock potential approximation are used for computing the thermal Blackbody radiation ionization characteristics of the alkali Rydberg atoms, in particular, the rubidium and caesium in Rydberg states with principal quantum number n = 20-100. Preliminary application of theory to computing ionization rate for the Rydberg sodium atom in the have demonstrated physically reasonable agreement between the theoretical and experimental data. The accuracy of the theoretical data is provided by a correctness of the corresponding relativistic wave functions and accounting for the exchange-correlation effects.
Abstract Features of Penning ionization in cold gaseous media of Rydberg alkali-metal atoms have been investigated. In contrast to the hydrogen atom, the corresponding autoionization widths exhibit a strong (by orders of magnitude) dependence on the orbital quantum numbers of the atoms involved in the long-range dipole–dipole interaction. An important feature of Penning ionization is the nontrivial dependence of its efficiency on the Rydberg particle size. For all types of alkali-metal atoms, the optimal highly nonsymmetric configurations of Rydberg pairs have been found that lead to the explosive (by several orders of magnitude) intensification of the free electron formation by means of the Penning ionization processes. This property makes Penning ionization an important means of forming primary charged particles during the cold Rydberg plasma formation. The numerical data for pairs of potassium atoms are reported that demonstrate a significant effect of the Förster resonance on the values of the Penning ionization rate constants.