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.
Ion formation in sodium vapor (\ensuremath{\sim}
1011 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}3}$) containing Rydberg atoms (18\ensuremath{\le}n\ensuremath{\le}35) was investigated. Both atomic ions and diatomic molecular ions resulting from collisions between highly excited sodium,
Na∗∗, and Na(3s) were observed. However, the predominant production mechanism was found to be photoionization of
Na∗∗ by blackbody radiation, the rate of which was measured at 500 K and found to be \ensuremath{\simeq}5.7\ifmmode\times\else\texttimes\fi{}
103 ${\mathrm{sec}}^{\mathrm{\ensuremath{-}}1}$ for n=18, in good agreement with theory. The
Na+ signal from blackbody photoionization is observed to be independent of n, which we interpret as implying rapid and nearly complete self-l-mixing, mixing by collisions with Na(3s) atoms, for both s and d states. It is probable, however, that the s states are mixed to the adjacent, n-1, manifold of l states. It was also found that the heavy-body collision cross sections for
Na+ and
Na2+ formation, while roughly three orders of magnitude lower than our estimate of the self-l-mixing cross section, are appreciable, of order 100 A
˚2.
The ionization of low-Rydberg-state He atoms in the n
1P state (n=14) in collisions with the polar molecules
NH3,
SO2, and acetone (
C3H6O) is carried out in a crossed-beam experiment at thermal kinetic energies. The dependence of the experimental ionization cross sections ${\ensuremath{\sigma}}_{i}^{\mathrm{expt}}$ on the relative velocity of the reactants is obtained by a time-of-flight method. We observe that it varies mainly as 1/
vr2 in a large part of the studied velocity range, while a 1/
vr velocity dependence is predicted by the free-electron model for the higher Rydberg levels.
In the present work very-high-n Rydberg-atoms
(nsim100−nsim400) are used to probe electron-molecule collisions at ultra-low electron energies. Based on the essentially-free-electron model, for sufficiently high n, Rydberg atom-molecule collisions can be described in terms of a binary interaction between the target molecule and the essentially-free Rydberg electron. Since the average kinetic energy of the Rydberg electron is ultra-low
rm(sim85mueV−sim1.4meV), analysis of the very-high-n Rydberg-atom collision data can provide information on electron-molecule scattering at electron energies corresponding to electron temperatures of only $\\sim
1\\sp\\circ$K, which are far below those accessible using any alternate approach.\nRate constants for destruction of very-high-n Rydberg atoms in collisions with various target molecules have been measured. This study focuses on Rydberg electron transfer to an electron-attaching molecule which results in negative ion formation via the reactions
rmK(itnp/)+XYtoKsp++(XY)sp−∗ortoKsp++Xsp−+Yeqno(1)and on rotational energy transfer from polar molecules which leads to Rydberg atom ionization
rmK(itnp/)+XY(itJ/)toKsp++itesp−+XY(itJ/−1)eqno(2)\nThe n dependence of the rate constants for Rydberg-atom destruction depends on the reactions involved. In reaction (1) the rate constant is independent of n whereas in reaction (2) it increases nearly linearly with n. When both reactions are possible, the measured n dependence can be explained in terms of contributions from each process.\nThe essentially-free-electron model suggests that the n dependence of the rate constants for Rydberg-atom destruction reflects the energy dependence of the cross sections of the corresponding free electron-molecule collision processes which are $$\\eqalignno{&e\\sp- + \\rm XY \\to (XY)\\sp{-*}\\ or\\ \\to X\\sp- + Y&(1\\sp\\prime)\\cr &e\\sp- + \\rm XY({\\it J\\/}) \\to {\\it e}\\sp- + XY({\\it J\\/}-1)&(2\\sp\\prime)\\cr}$$Analysis of the data therefore provides the behavior of cross sections for these processes at ultra-low electron energies.
An experimental study of the depopulation and final-state distribution of Na 36s and 30p Rydberg states under Na + bombardment in the presence of electric fields up to 50 V cm -1 has been carried out. Incident energies E from 171 to 967 eV span the range from 0.6 to. 1.4 times the mean orbital speed of the excited electron in the initial state. Absolute depopulation cross sections of order 10 -8 cm 2 , believed accurate within 25%, are reported as functions of field and energy. sigma 36s is proportional to E -1 , but sigma 30p is nearly independent of energy. The distribution of final states was measured by selective field ionization. At weak fields for which the initial state is well separated from the nearest Stark manifold, final states are broadly distributed across the nearest manifolds. But for stronger fields that shift the initial state close to a Stark manifold the final states are strongly concentrated among the energetically closest manifold sublevels.
The results of the first measurements of the velocity dependence of the total ionization ${\ensuremath{\sigma}}_{I}$ and the total destruction ${\ensuremath{\sigma}}_{d}$ (ionization+excitation+deexcitation) cross sections for fast Rydberg-atom-neutral-molecule collisions are presented. The observed resonant structure in and the absolute magnitudes of ${\ensuremath{\sigma}}_{I}$ and ${\ensuremath{\sigma}}_{d}$ unambiguously confirm the prediction that the Rydberg electron bound to a fast atom scatters quasifreely. The data also strongly hint that the ionic core does the same.