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The Journal of Chemical Physics

Associative formation of Rydberg state clusters from collisions between a Rydberg state species and a ground state neutral atom

Xianzhao Peng, James E. Abbott, Wei Kong

Published Aug 22, 2000• 10 citations
Publisher

Abstract

Using a mass analyzed threshold ionization (MATI) spectrometer, the spectra of the monomer, dimer, and trimer of sodium were measured. Intense dimer signals both at the ionization threshold and at Rydberg resonances of the monomer were observed. Below the adiabatic threshold of the dimer, a trimer spectrum which showed vibrational progressions similar to those of the dimer was also recorded. In both cases, the high energy edge of the heavier cluster was shifted to a lower energy compared with that of the lighter cluster. The monomer time-of-flight spectrum at the Rydberg resonances was diffuse, while the time-of-flight spectrum of the dimer was sharp and intense. Based on the continuity of oscillator strength and further energetic analysis, we conclude that the dimer signal at the Rydberg resonances of the monomer originated from collisional association between a Rydberg state atom and a ground state atom. Similarly, the trimer signal was from the combination between a Rydberg state dimer and a ground state atom. The combined product from collision was in a Rydberg state that can be field ionized during MATI detection. This work offers direct experimental evidence for the formation of high Rydberg state species through collisional recombination.

DOI
10.1063/1.1287280

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Using a mass analyzed threshold ionization (MATI) spectrometer, the spectra of the monomer, dimer, and trimer of sodium were measured. Intense dimer signals both at the ionization threshold and at Rydberg resonances of the monomer were observed. Below the adiabatic threshold of the dimer, a trimer spectrum which showed vibrational progressions similar to those of the dimer was also recorded. In both cases, the high energy edge of the heavier cluster was shifted to a lower energy compared with that of the lighter cluster. The monomer time-of-flight spectrum at the Rydberg resonances was diffuse, while the time-of-flight spectrum of the dimer was sharp and intense. Based on the continuity of oscillator strength and further energetic analysis, we conclude that the dimer signal at the Rydberg resonances of the monomer originated from collisional association between a Rydberg state atom and a ground state atom. Similarly, the trimer signal was from the combination between a Rydberg state dimer and a ground state atom. The combined product from collision was in a Rydberg state that can be field ionized during MATI detection. This work offers direct experimental evidence for the formation of high Rydberg state species through collisional recombination.
Highly excited (Rydberg) atoms are produced and can exist for significant periods of time in various plasma environments. It is necessary to know cross sections for the various collision processes involving these atoms if a complete understanding of the physics of these environments is to be attained.\nThe experimental investigation of collisional phenomena between high Rydberg sodium atoms and electrons is described in this thesis. A fraction of the atoms in a ground state sodium beam is optically excited (using lasers) to well-defined, high Rydberg states (principal quantum numbers chosen around 40). Subsequent to their production the Rydberg atoms are allowed to interact with 25 eV electrons for a specified time interval following which the collision products are detected. The electrons are produced in a beam which is crossed at right angles with the sodium beam. Important collision processes are (1) electron impact ionization of the Rydberg atom, and (2) electron-Rydberg atom interactions in which the quantum state of the atom is changed (state changing collisions).\nResults are presented for an observed state changing process which is identified as angular momentum state changing only (no change in the value of the principal quantum number). Cross sections for this process are measured to be 10('-10) to 10('-9) cm('2). Problems encountered during the work which prevented the measurement of electron impact ionization cross sections are discussed. In the course of the work two other topics required study: (1) the process of electric field ionization of Rydberg atoms (used to detect the atoms), and (2) the effects of background (300 K) radiation (from the chamber walls, for example) on Rydberg atoms. Results of these studies are also presented.
Collisional and thermal ionization of sodium n S and n D Rydberg atoms with n = 8–20 has been studied. The experiments were performed using a two-step pulsed laser excitation in an effusive atomic beam at atom density of about 2 × 10 10 cm −3 . Molecular and atomic ions from associative, Penning and thermal ionization processes were detected. It was found that the atomic ions were created mainly due to photoionization of Rydberg atoms by photons of blackbody radiation at the ambient temperature of 300 K. Blackbody ionization rates and effective lifetimes of Rydberg states of interest were determined. The molecular ions were found to be from associative ionization in Na( nL ) + Na(3S) collisions. Rate constants of associative ionization have been measured using an original method based on relative measurements of Na + 2 and Na + ion signals.
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 .
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.
Long-lived, excited neutral particles, arising from the interaction of monochromatic synchrotron radiation with ground state He atoms, have been observed at photon energies close to the (N = 1,2,3 and 4) ionization thresholds. The measurements have been made using an unconventional experimental arrangement in which charged particles, responsible for the dominant signal in conventional photon impact studies, are prevented from reaching the detector. For , it appears that the formation, via photoexcitation, of relatively long-lived, doubly excited Rydberg states is a necessary step in the production of the observed signal. Four processes that might account for the production of the excited neutral particles are considered. The simplest, that atoms in the initial doubly excited Rydberg states are themselves directly observable, is considered unlikely. However, the lifetimes of the photoexcited double Rydberg states may be increased through the effects of electric fields present in the apparatus. Transitions from these double Rydberg states, occurring either as a result of collisions or by fluorescence, could result in metastable, singly excited neutral particles. The presence of signal related to the existence of long-lived doubly excited states could be significant in the interpretation of other photon impact measurements.