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Journal of Physics B Atomic Molecular and Optical Physics

Collisions of Na+ions with Na Rydberg atoms in electric fields: depopulation cross sections and final-state distributions from 36s and 30p initial states

R G Rolfes, L. G. Gray, Keith B. MacAdam

Published May 28, 1992• 10 citations
Publisher

Abstract

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.

DOI
10.1088/0953-4075/25/10/013

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Ion formation in sodium vapor (\ensuremath{\sim}${10}^{11}$ ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}3}$) 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, ${\mathrm{Na}}^{\mathrm{*}\mathrm{*}}$, and Na(3s) were observed. However, the predominant production mechanism was found to be photoionization of ${\mathrm{Na}}^{\mathrm{*}\mathrm{*}}$ 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{}${10}^{3}$ ${\mathrm{sec}}^{\mathrm{\ensuremath{-}}1}$ for n=18, in good agreement with theory. The ${\mathrm{Na}}^{+}$ 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 ${\mathrm{Na}}^{+}$ and ${\mathrm{Na}}_{2}$${\mathrm{}}^{+}$ formation, while roughly three orders of magnitude lower than our estimate of the self-l-mixing cross section, are appreciable, of order 100 A${\r{}}^{2}$.

Physical Review A•Jul 1, 1986•28 citations
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.
Ar+{\mathrm{Ar}}^{+}Ar+ and Na+{\mathrm{Na}}^{+}Na+ ion beams bombarding Na ns and np Rydberg-state targets at impact velocities near the Bohr-orbital velocity of the target atoms (i.e., v\ifmmode \tilde{}\else \~{}\fi{}\ensuremath{\approxeq}1) induce transitions to (n-1)l states (l\ensuremath{\ge}2) with larger-than-geometric cross sections. Depopulation of ns states proceeds directly into the full n-1, l\ensuremath{\ge}2 manifold rather than populating the np or (n-1)p states as the first of a sequence of dipole-allowed steps. Depopulation of np states leads to a distribution of final states that is dominated by the nearer or high-l part of the n-1 manifold. n dependences of the cross section for ns depopulation are given at several energies for n=32--41 and at a single energy for np, n=26--32. The absolute cross section for Na(36s) depopulation falls gradually but steadily for reduced velocities v\ifmmode \tilde{}\else \~{}\fi{} increasing from 0.3 to 1.35. Bombardment of Na 39s and 39p states in applied fields 0--18.5 V/cm reveals that the final-state distributions become narrower as manifold states are Stark shifted close to the initial states. No theoretical results are available for direct comparison with these experiments, but the method of coupled channels seems to be the most suitable candidate.
New experimental results have been obtained in collisions of singly charged ions with Na Rydberg atoms. (a) The distribution of final n states populated by electron capture shows non-monotonic variations of width with incident energy over the range 60-2100 eV. (b) The total capture cross section for alkali ions on Rydberg targets shows peaks and dips over the same energy range, correlated with particular reduced velocities v and the polarization of the exciting laser. (c) {ell}-Changing collision of Na{sup +} on Na(nd) targets, n=26 and 28, at low v preferentially transfer multiple units {h_bar} of orbital angular momentum under single-collision conditions, despite very large impact parameters. (d) Inelastic impacts of Na{sup f+} on Na 36s and 30p states, perturbed by electric fields, populate a strongly field-dependent mixture of nearby Stark levels. A synopsis of recent progress will be given.
An experimental study of the depopulation of Na(30s) Rydberg atoms under He + ion bombardment has been undertaken to identify the range of collision velocities at which strongly coupled behaviour of the 30s and nearby levels at low velocity changes to predominantly dipole-allowed coupled at high velocity. Ion energies ranged from 700 to 3900 eV corresponding to collision velocities of 2.4 to 5.6 times the mean orbital speed of the excited 30s electron. The ratio of the cross section for the dipole-allowed transitions (30s to 30p and 30s to 29p) to the total depopulation cross section was determined for each collision velocity. (Other dipole-allowed transitions were observed to be negligible.) This ratio was found to increase from only 20% at a reduced velocity of 2.4 to 65% at a reduced velocity of 5.6. The ratio of the two dipole cross sections, sigma (30s-30p)/ sigma (30s-29p), was also determined and compared to calculations based on the dipole approximation with first-order perturbation theory.
The theory of collisions of Rydberg atoms with rare-gas atoms is generalized to include the effects of an applied static electric field. Two effects occur. First, the field causes the states to split, and the increased energy separations lead to a decrease in the inelastic cross sections. Second, there is a change in the form of the wave functions, because the various Stark states in the field have electron charge distributions that may be localized in very different regions of space. The present work focuses on this second effect. With the description of the initial and final Stark states of the Rydberg atom by the proper electronic wave functions obtained in parabolic coordinates, cross sections are obtained for a variety of specific transitions of Rydberg atoms (n=10,15,and20n=10, 15, \mathrm{and} 20n=10,15,and20) caused by collisions. The calculations are strictly valid for hydrogen, but exhibit general features that are expected to apply to other Rydberg atoms as well. The results show a dramatic effect on the cross section for particular transitions depending on the degree of overlap of the initial and final charge distributions. In addition, it is observed that transitions are favored that involve small changes in the azimuthal quantum number mmm. The origin of this tendency is discussed.
We have observed electron impact ionization of highly excited sodium Rydberg atoms in nsnsns and ndndnd states, n=35−−51n=35--51n=35−−51, below E=2  eVE=2\text{ }\text{ }\mathrm{e}\mathrm{V}E=2  eV electron kinetic energy with energy resolution 0.25 eV. Measured absolute cross sections near 0 eV range from ${\ensuremath{\sigma}}_{35d}\ensuremath{\approx}7\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}10}$ to ${\ensuremath{\sigma}}_{50d}\ensuremath{\approx}4\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}9}\text{ }\text{ }{\mathrm{c}\mathrm{m}}^{2}$. The energy dependence is consistent with that of widely used binary encounter approximation cross sections, and ${\ensuremath{\sigma}}_{n}$ follows a power law in nnn. The measured cross sections are 14 to 24 times larger than theoretically predicted values. This enhancement may signal the effect of large polarizabilities of high Rydberg states not yet accounted for in ionization theories.
Ion formation in sodium vapor (\ensuremath{\sim}1011{10}^{11}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∗∗{\mathrm{Na}}^{\mathrm{*}\mathrm{*}}Na∗∗, and Na(3s) were observed. However, the predominant production mechanism was found to be photoionization of Na∗∗{\mathrm{Na}}^{\mathrm{*}\mathrm{*}}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{10}^{3}103 ${\mathrm{sec}}^{\mathrm{\ensuremath{-}}1}$ for n=18, in good agreement with theory. The Na+{\mathrm{Na}}^{+}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+{\mathrm{Na}}^{+}Na+ and Na2{\mathrm{Na}}_{2}Na2​+{\mathrm{}}^{+}+ 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{\r{}}^{2}˚2.