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Atoms

Dynamic Instability of Rydberg Atomic Complexes

M. S. Dimitrijević, Vladimir A. Srécković, Alaa Abo Zalam, Nikolai N. Bezuglov, Andrey N. Klyucharev

Published Feb 8, 2019• 5 citations
Publisher

Abstract

Atoms and molecules in highly excited (Rydberg) states have a number of unique characteristics due to the strong dependence of their properties on the values of principal quantum numbers. The paper discusses the results of an investigation of collisional Rydberg complexes specific features, resulting in the development of dynamic chaos and the accompanying diffusion autoionization processes. It is shown (experiment and theory) that, in subthermal low energies, the global chaotic regime that evolved in quasimolecular systems leads to significant changes in the Rydberg gases radiation/ionization kinetics. The effect of Förster resonance on the width of the fluorescence spectra and stochastic ionization processes in Rydberg systems is also discussed.

DOI
10.3390/atoms7010022

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Atoms and molecules in highly excited (Rydberg) states have a number of unique characteristics due to the strong dependence of their properties on the values of principal quantum numbers. The paper discusses the results of an investigation of collisional Rydberg complexes specific features, resulting in the development of dynamic chaos and the accompanying diffusion autoionization processes. It is shown (experiment and theory) that, in subthermal low energies, the global chaotic regime that evolved in quasimolecular systems leads to significant changes in the Rydberg gases radiation/ionization kinetics. The effect of Förster resonance on the width of the fluorescence spectra and stochastic ionization processes in Rydberg systems is also discussed.
Contemporary views on the formation of dynamic nonlinear resonances in isolated intermediate Rydberg quasi-molecular complexes formed by a single elementary act upon the slow collision highly excited atoms are discussed. A relation between the emergence of dynamic resonance and the quasi-intersection of atomic terms is revealed in the quasi-classical approximation. Relationships between the widths of dynamic resonances and the dipole matrix element leading to the corresponding quasi-intersections are determined. The physical reasons for the dynamic chaos regime are formulated. A quasi-classical statistical description is given of the diffusion ionization of an atomic complex with a dense network of quasi-intersections of terms. Development of the stochastic instability of the Rydberg electron trajectories due charge exchange inside the collision complex is considered. The effect the narrowing region of stochastic motion has when passing through the Coulomb convergence of the levels with a simultaneous drop in the ionization rate of quasi-molecular systems is predicted for external statistical magnetic and electric fields under conditions of Förster resonance.
Rydberg atoms are increasingly being used as a means of introducing long-range, tunable interactions into atomic systems through their strong dipole-dipole interactions. When creating such interactions, however, there are a variety of potential effects that can occur, such as state (n and/or L) changing or Penning ionization, which can complicate the dynamics of the system. In the following work, such interactions are investigated for Rydberg-Rydberg collisions using very high-n, n ~300, strontium Rydberg atoms in an atomic beam configuration. By exploiting Rydberg blockade and the inherent distribution of atomic velocities present in an atomic beam, it is possible to create a 1D array of moving Rydberg atoms which will naturally overtake each other over time. Measurements of both Penning ionization and state changing for such collisions are made and compared with classical trajectory Monte-Carlo (CTMC) simulations, with both indicating large collisional cross sections on the order of 1 x 10-6 cm2 for Penning ionization and nearly 8 x 10-5 cm2 for state changing interactions. In a second series of experiments, previous work involving doubly-excited Rydberg states is expanded upon by investigating autoionization with high-n, L > 3, Rydberg states. Past research involving autoionization has shown that the effect is strongly L-dependent, with high-L states having significantly smaller autoionizing rates. To create well-defined, L > 3 states, the use of microwave fields to drive various high-n, n ~ 150, n1F3 → (n+1)1G4, (n+2)1H5 transitions is investigated, with spectroscopic measurements of these transitions providing quantum defect values for n1G4 and n1H5 states. These measurements provide a basis for future studies into the L-dependence of high-n, n ~ 300, autoionizing Rydberg atoms, with the eventual goal of creating a long-lived, doubly-excited “planetary” Rydberg state.
We have considered two types of interactions between particles resulting in autoionization of the intermediate Rydberg collisional complex.The first type is caused by the charge exchange processes inside the ionic core of the complex and is responsible for the formation of the final associative ionization channel due to the departure of a Rydberg electron (RE) of the complex to the energy continuum.We have investigated the evolution of the orbital momentum L of RE and discovered a non-trivial time dependence of L, demonstrating a contrasting oscillatory structure in both direction orientation and its absolute value.The second type of interaction, dipole-dipole interaction, dominates in cold highly excited gaseous media and leads to Penning ionization of various pairs of Rydberg atoms.We have found the optimal quantum configurations of atomic pairs, which intensify the PI rates by several orders of magnitude, and become important suppliers of charged particles upon the evolution of Rydberg gas into cold plasma.
The problem of impact ionization of two Rb atoms, one of which belongs to the Rydberg P series and the other of which is in the ground state, is studied and solved with the use of the methods of stochastic dynamics for description of the path instability of a Rydberg electron in a collision diatomic complex. The actual potential of the atomic framework was taken into account in terms of the single-channel quantum-defect method, whose accuracy was demonstrated on the example of determination of the photoionization cross sections in the quasi-classical approximation. A representation of the effective average lifetime of an external electron in the bound state that takes into account both the diffusion migration within the Coulomb crowding of the potential energy curves for the quasi-molecular complex and the direct quantum autoionization is obtained in analytical form. It is shown that the rate constants of diffusion collisional ionization calculated by us are in good agreement with the experimental data.
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.
It was only recently established that the ubiquitous black-body radiation plays an important role in the spectroscopy of Rydberg atoms even at room temperature. 1.2 Black-body radiation causes shifts in the energy of atomic levels,2 induces transitions between atomic states,2 causes photoionization of Rydberg atoms,3 and affects the population of highly excited states in the recombination of ions.4•5 We will show that black-body radiation also causes diffusive ionization of Rydberg atoms and ions. Under certain conditions, the principal condition among which is the collision-induced mixing of levels in I, the diffusion process resulting from black-body radiation is the basic mechanism for the ionization of Rydberg atoms.