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Journal of Physics B Atomic Molecular and Optical Physics

Ionization due to the interaction between two Rydberg atoms

F. Robicheaux

Published Jan 6, 2005• 67 citations
Publisher

Abstract

Using a classical trajectory Monte Carlo method, we have computed the ionization resulting from the interaction between two cold Rydberg atoms. We focus on the products resulting from close interaction between two highly excited atoms. We give information on the distribution of ejected electron energies, the distribution of internal atom energies and the velocity distribution of the atoms and ions after the ionization. If the potential for the atom is not purely Coulombic, the average interaction between two atoms can change from attractive to repulsive giving a Van de Graaff-like mechanism for accelerating atoms. In a small fraction of ionization cases, we find that the ionization leads to a positive molecular ion where all of the distances are larger than 1000 Bohr radii.

DOI
10.1088/0953-4075/38/2/024

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Journal of Physics B Atomic Molecular and Optical Physics•May 26, 2005•34 citations
Using a classical trajectory Monte Carlo method, we have computed the ionization resulting from the interaction between two cold Rydberg atoms. We focus on the products resulting from close interaction between two highly excited atoms. We give information on the distribution of ejected electron energies, the distribution of internal atom energies and the velocity distribution of the atoms and ions after the ionization. If the potential for the atom is not purely Coulombic, the average interaction between two atoms can change from attractive to repulsive giving a Van de Graaff-like mechanism for accelerating atoms. In a small fraction of ionization cases, we find that the ionization leads to a positive molecular ion where all of the distances are larger than 1000 Bohr radii.
In a recent work [Phys. Rev. Lett. 98, 023004 (2007)], we investigated the influence of the attractive van der Waals interaction on the pair distribution and Penning ionization dynamics of ultracold Rydberg gases. Here we extend this description to atoms initially prepared in Rydberg states exhibiting repulsive interaction. We present calculations based on a Monte Carlo algorithm to simulate the dynamics of many atoms under the influence of both repulsive and attractive long-range interatomic forces. Redistribution to nearby states induced by blackbody radiation is taken into account, changing the effective interaction potentials. The model agrees with experimental observations, where the ionization rate is found to increase when the excitation laser is blue detuned from the atomic resonance.
We have observed the ionization of a cold gas of Rb Rydberg atoms which occurs when nsnsnsnsnsns van der Waals pairs of nsnsns atoms of $n\ensuremath{\approx}$ 40 on a weakly repulsive potential are transferred to an attractive dipole-dipole nsnpnsnpnsnp potential by a microwave transition. Comparing the measurements to a simple model shows that the initial 300-$\ensuremath{\mu}$K thermal velocity of the atoms plays an important role. Excitation to a repulsive dipole-dipole potential does not lead to more ionization on a 15-$\ensuremath{\mu}$s time scale than leaving the atoms in the weakly repulsive nsnsnsnsnsns state. This observation is slightly surprising since a radiative transition must occur to allow ionization in the latter case. Finally, by power broadening of the microwave transition, to allow transitions from the initial nsnsnsnsnsns state to the nsnpnsnpnsnp state over a broad range of internuclear spacings, it is possible to accelerate markedly the evolution to a plasma.
The emission of fast ions in Penning ionization of cold Rydberg atoms is experimentally observed, and the underlying ion acceleration mechanisms are identified. In the experiment, the Rydberg atoms in nS/nP/nD (n = 20-50) states were prepared by laser excitation of cold atoms in a magneto-optical trap, and the Penning ions were measured using velocity-map imaging technology. The influence of Penning process on the lifetime of Rydberg gas and the ion velocity distribution was investigated. The ion originating from conventional Penning ionization gains a velocity significantly higher than the thermal velocity of cold atom. It is accelerated by Coulomb repulsion from the nearby de-excited Rydberg atom. In addition, a small fraction of ions with velocities exceeding 40 m/s has been observed. These ions are interpreted as arising from double-ionization process of Rydberg atom-pair. The strong Coulomb repulsion between two ions within a close distance gives them considerable acceleration, resulting in a large velocity of the ions.
The results of a theoretical investigation of prompt many-body ionization are reported. Our calculations address an experiment that reported ionization in Rydberg gases for densities two orders of magnitude less than expected from ionization between pairs of atoms. The authors argued that the results were due to the simultaneous interaction between many atoms. We performed classical calculations for many interacting Rydberg atoms with the ions fixed in space and have found that the many-atom interaction does allow ionization at lower densities than estimates from two-atom interactions. However, we found that the density fluctuations in a gas play a larger role. These two effects are an order of magnitude too small to account for the experimental results suggesting at least one other mechanism strongly affects ionization.
Heavy-Rydberg ion-pair states, molecular quantum systems that are bound by their long-range pure Coulomb attraction, are formed through Rydberg atom collisions with molecules that attach low energy electrons. Collisions of potassium Rydberg atoms K(np) with the attaching species CCl4 and SF6 lead, respectively, to dissociative and non-dissociative electron attachment with subsequent formation of bound ion-pair states K+..Cl- and K+..SF6-.\nThe experimental apparatus used to produce and detect heavy-Rydberg ion-pair states consists of a reaction region and a separate analysis region. It separates a fraction of the product ion pairs from the parent Rydberg atoms, eliminating spurious background signals associated with blackbody-induced and electric-field ionization of Rydberg atoms. A position sensitive detector in the analysis region is employed to measure their velocity, angular, and binding energy distribution and lifetimes. Measurements of the spatial distribution of ion pairs provide information on their velocity and angular distributions, and their binding energy distribution is measured using electric field-induced dissociation. The lifetime of the ion-pair states is influenced by multiple processes including internal-to-translational energy transfer, autodetachment of the electron, and neutralization through charge transfer.\nThe experimental results are compared with the results of a Monte Carlo collision code that models both the initial Rydberg electron attachment and the subsequent evolution and molecular dynamics of the ion pairs. This model highlights the factors such as the kinematics of the Rydberg atom and the attaching particle and energy released in dissociation (in the case of dissociative attachment) that are important in governing ion pair formation. The model calculations are in good agreement with the experimental data.
A stochastic model of associative ionization in collisions of Rydberg atoms with ground-state atoms is presented. The conventional Duman–Shmatov–Mihajlov–Janev (DSMJ) model treats the ionization as excitation of Rydberg electron to the continuum by the electric-dipole field generated by exchange interaction within the quasi-molecular ion. The stochastic model essentially extends this treatment by taking into account redistribution of population over a range of Rydberg states prior to ionization, which is caused by non-adiabatic processes in overlapping multiple level crossings of quasi-molecular Rydberg states. The redistribution is modelled as diffusion of electrons in the Rydberg energy spectrum using a Fokker–Planck-type equation. The process of l -mixing of Rydberg states at large internuclear distances and twisting of the collision trajectories on attractive potentials are taken into account. The choice of the collision velocity distribution is also shown to be important. Associative ionization rates have been calculated for Na**( nl ) + Na collisions with n = 5–25 and l = 0, 1, 2, and compared with the available experimental data and the calculations performed using the nonlinear DSMJ model. At relatively low n the stochastic model yields a substantially better agreement with the experimental data than the DSMJ model, while the results of both models converge at large n .