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.
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.
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 .
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.
Results of theoretical calculations of ionization rates of Rb and Na Rydberg atoms by blackbody radiation (BBR) are presented. Calculations have been performed for
nS,
nP, and
nD states of Na and Rb, which are commonly used in a variety of experiments, at principal quantum numbers
n=8−−65 and at three ambient temperatures of 77, 300, and
600K. A peculiarity of our calculations is that we take into account the contributions of BBR-induced redistribution of population between Rydberg states prior to photoionization and field ionization by extraction electric field pulses. The obtained results show that these phenomena affect both the magnitude of measured ionization rates and shapes of their dependences on
n. The calculated ionization rates are compared with the results of our earlier measurements of BBR-induced ionization rates of Na
nS and
nD Rydberg states with
n=8−−20 at
300K. A good agreement for all states except
nS with
n>15 is observed. We also present the useful analytical formulas for the quick estimation of BBR ionization rates of Rydberg atoms.