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Physical Review Letters

Alignment and geometrical effects on Stueckelberg interference structure in cross sections for inelastic collisions involving Rydberg atoms

Bidhan C. Saha, Neal F. Lane

Published May 30, 1994• 12 citations
Publisher

Abstract

A theoretical study of Stueckelberg interference structure in inelastic, state-changing integrated cross sections for collisions of low-Rydberg Na (n10) atoms with ground state He atoms is reported. The dependence of the Stueckelberg interference structure on orbital geometry and alignment of the initial state is predicted. Interference oscillations are found in the cross sections for both initial ns and np states; in the latter case, the features show considerable sensitivity with respect to variations in the spatial alignment of the principal axis of the electron charge distribution at some collision velocities and near isotropy at others.

DOI
10.1103/physrevlett.72.3487

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Alignment and intracollisional interference effects in slow collisions between low-Rydberg Na and ground-state He atoms

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Semiclassical, coupled-states calculations have been performed of slow state-changing collisions between low-Rydberg (n <10) ns and np atoms and ground state He atoms. The dependence of cross sections on the initial orbital alignment of np atoms is studied. Structure in the cross sections, arising from interference between localized electron scattering (at avoided crossings), i.e., Stueckelburg oscillations, vary with the geometry (size, shape) and alignment (for non-spherical states) of the electron cloud of the initial target atom.

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Slow collisions of ions with Rydberg atoms

Keith B. MacAdam

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.

Bulletin of the American Physical Society•Dec 1, 1992•0 citations
A theoretical study of Stueckelberg interference structure in inelastic, state-changing integrated cross sections for collisions of low-Rydberg Na (n10) atoms with ground state He atoms is reported. The dependence of the Stueckelberg interference structure on orbital geometry and alignment of the initial state is predicted. Interference oscillations are found in the cross sections for both initial ns and np states; in the latter case, the features show considerable sensitivity with respect to variations in the spatial alignment of the principal axis of the electron charge distribution at some collision velocities and near isotropy at others.
Semiclassical, coupled-states calculations have been performed of slow state-changing collisions between low-Rydberg (n <10) ns and np atoms and ground state He atoms. The dependence of cross sections on the initial orbital alignment of np atoms is studied. Structure in the cross sections, arising from interference between localized electron scattering (at avoided crossings), i.e., Stueckelburg oscillations, vary with the geometry (size, shape) and alignment (for non-spherical states) of the electron cloud of the initial target atom.
Retention of orbital alignment during near-resonant energy transfer collisions of rare-gas projectiles with excited alkaline-earth-metal atoms is explored theoretically for scattering of Xe from Rydberg states of Ca. For such collisions, conventional interpretations of alignment phenomena, which are based on potential curves for a transient molecule thought to form during the collision, are not relevant. Theoretical partial magnetic sublevel cross sections for ${\mathrm{Ca}}^{**}(4s17d{}^{1}{D}_{2}\ensuremath{\rightarrow}4s18p{}^{1}{P}_{1})$ transitions confirm the existence of alignment effects, as demonstrated experimentally by Spain et al. [J. Chem. Phys. 102, 9532 (1995)], at a mean relative velocity of 914 m/s. Theory further predicts heretofore unobserved oscillatory structures in these cross sections as a function of relative velocity and that these oscillations depend strongly on the initial magnetic quantum number of the Rydberg electron.
Recent experimental and theoretical studies of near-resonant energy transfer collisions involving rare-gas atoms and alkali or alkaline earth atoms which have been initially excited to an aligned state via one or more linearly polarized rasters have yielded a wealth of insight into orbital alignment and related effects. We have extended this inquiry to initially aligned Rydberg states, examining state-to-state and alignment-selected cross sections using quantum collision theory augmented by approximations appropriate to the special characteristics of the Rydberg state (e.g., the quasi-free-electron model and the impulse approximation).
A recent quantum mechanical study [W. Isaacs and M. A. Morrison, Phys. Rev. A 57, R9 (1998)] discovered pronounced oscillations in cross sections for near-resonant energy transfer collisions of rare-gas atoms with initially aligned Rydberg atoms. We analyze such collisions for 17d(m)-->18p(m(')) transitions in the Ca-He system semiclassically and show that the oscillations arise from a phase interference process unique to Rydberg target states. In addition to explaining the origin of these structures, this analysis explains their disappearance when the relative Ca-He velocity goes to infinity and/or the energy defect vanishes and their dependence on the initial and final magnetic quantum numbers of the transition.
Alignment and orientation effects in collisions of helium with Rydberg atoms due to the presence of static electric and magnetic fields are predicted. Analytical expressions are obtained for the cross sections of the state-to-state transitions within the manifold with the same principal quantum number. For moderate field-induced inelasticity, the curves of the cross sections vs the fields intensity show modulations that are explained in terms of the phase differences accumulated by the wave functions of the states involved in the collision. Due to the presence of the magnetic field, transitions involving inversion of high magnetic quantum numbers are dramatically quenched. The possibility of observing the predicted effects is discussed. The reported analytical cross sections are expected to help in the understanding of the results.
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.