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arXiv:1507.03357 · Journal of Physics B Atomic Molecular and Optical Physics

Quantum mechanical calculation of Rydberg–Rydberg autoionization rates

Martin Kiffner, Davide Ceresoli, Wenhui Li, Dieter Jaksch

Published Oct 6, 2016• 14 citations
arXivHTMLPDF

Abstract

Abstract We present quantum mechanical calculations of autoionization rates for two rubidium Rydberg atoms with weakly overlapping electron clouds. We neglect exchange effects and consider tensor products of independent atom states forming an approximate basis of the two-electron state space. We consider large sets of two-atom states with randomly chosen quantum numbers and find that the charge overlap between the two Rydberg electrons allows one to characterise the magnitude of the autoionization rates. If the electron clouds overlap by more than one percent, the autoionization rates increase approximately exponentially with the charge overlap. This finding is independent of the energy of the initial state.

DOI
10.1088/0953-4075/49/20/204004

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Abstract We present quantum mechanical calculations of autoionization rates for two rubidium Rydberg atoms with weakly overlapping electron clouds. We neglect exchange effects and consider tensor products of independent atom states forming an approximate basis of the two-electron state space. We consider large sets of two-atom states with randomly chosen quantum numbers and find that the charge overlap between the two Rydberg electrons allows one to characterise the magnitude of the autoionization rates. If the electron clouds overlap by more than one percent, the autoionization rates increase approximately exponentially with the charge overlap. This finding is independent of the energy of the initial state.
This paper is devoted to the autoionization process of large-angular-momentum Rydberg states. After a brief account of autoionization formalism in nonrelativistic theory and single-configuration approximation, we apply it to atomic states with one electron of large angular momentum. The dominant contribution is the direct one and the exchange contribution is ignored. In this framework, the autoionization width varies with the principal quantum number as ${n}^{\mathrm{\ensuremath{-}}3}$ and exponentially with the angular momentum. When two excited electrons interact with a spherically symmetric core, it is demonstrated that the interaction between the Rydberg electron and the core polarized by the valence electron is proportional to the interaction between the two active electrons. Using newly derived radial matrix elements, we obtain a generally good agreement between our results and experiments on barium and strontium. Large-l Rydberg states are shown to be stable versus autoionization as soon as l is about 7. Possible refinements of our method are reviewed.
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.
Abstract We consider Penning ionization of Rydberg atom pairs as an Auger-type process induced by the dipole–dipole interaction and employ semiclassical formulae for dipole transitions to calculate the autoionization width as a function of the principal quantum numbers, n d , n i , of both atoms. While for symmetric atom pairs with n d = n i = n 0 the well-known increase of the autoionization width with increasing n 0 is obtained, the result for asymmetric pairs is counterintuitive—for a fixed n i of the ionizing atom of the pair, the autoionization width strongly increases with decreasing n d of the de-excited atom. For H Rydberg atoms this increase reaches two orders of magnitude at the maximum of the n d dependence, and the same type of counterintuitive behavior is exhibited also by Na, Rb and Cs atoms. This is a purely quantum-mechanical effect, which points towards existence of optimal (we call them ‘Tom’ and ‘Jerry’ for ‘big’ and ‘small’) pairs of Rydberg atoms with respect to autoionization efficiency. Building on the model of population redistribution in cold Rydberg gases proposed in [1], we demonstrate that population evolution following the initial laser excitation of Rydberg atoms in state n 0 would eventually lead to the formation of such Tom–Jerry pairs with n i > n 0 > n d which feature autoionization widths that are enhanced by several orders of magnitude compared to that of two atoms in the initial laser-excited state n 0 . We also show that in the high-density regime of cold Rydberg gas experiments the ionization rate of Tom–Jerry pairs can be substantially larger than the blackbody radiation-induced photoionization rate.
The autoionization mechanisms of dense n P 3/2 ( n = 20–97) Rydberg gases of 87 Rb atoms in the spontaneous evolution were investigated for the first time. By observing the characteristic time of the electrons generated through autoionization process, the dependence of autoionization mechanisms (black‐body radiation, electron–Rydberg collision, and Penning ionization) on the principal quantum number n of initial n P states was demonstrated. The dependence on the number n in n P Rydberg atoms is similar to those in n D Rydberg atoms.
Laser-induced autoionization, a form of forced autoionization, is discussed. Highly excited atomic Rydberg states generally have a small cross section for photoionization due to their small overlap with the nucleus. The cross section for photoionization can be strongly enhanced if the Rydberg series is perturbed by an atomic state with a relatively large cross section for photoionization. The photoionization dynamics of such a perturbed Rydberg system shows strong similarities to that of an autoionizing Rydberg series. For intense laser pulses, which strongly couple the perturber to the continuum, the photoionization rate is limited by the coupling between the Rydberg states and the perturber or, in other words, the autoionization rate. The model describing this ionization dynamics is applied to the barium 6snd(1,3{(}^{1,3}(1,3D2{\mathit{D}}_{2}D2​) state which is perturbed by the 5d7d(1{(}^{1}(1D2{\mathit{D}}_{2}D2​) state. The calculations show good agreement with experimental results of photoionization of barium Rydberg states with subpicosecond laser pulses of light of 620 nm in wavelength.