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Optics and Spectroscopy

Inelastic collisions with the participation of aligned and oriented atoms in the /sup 1/P/sub 1/ state

Alexander Z. Devdariani, Yu. N. Sebyakin

Published Feb 1, 1987• 0 citations
OpenAlex

Abstract

A formula has been obtained which describes the dependence of the overall cross section of the inelastic process in experiments with intersecting atomic and light beams on five parameters, two of which depend on the properties of the quasimolecule and the collisional energy, and three others on the degree of linear polarization of the exciting light and two angles which determine the geometry of the experiment. It was shown that measuring the overall cross section by varying the two latter parameters allows us to obtain additional information on the mechanism of the reactions. As an example, the experimentally studied process of spin transfer in Ca(4s5p/sup 1/P/sub 1/)+He and the process of Penning ionization of He(2/sup 1/P/sub 1/)+Cd(Zn) has been considered.

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Experimental studies concerning elastic and inelastic electron scattering by coherently ensembles of Ba (...6s6p (sub 1)P(sub 1)) atoms with various degrees of alignment will be described. An in-plane, linearly-polarized laser beam was utilized to prepare these target ensembles and the electron scattering signal as a function of polarization angle was measured for several laser geometries at fixed impact energies and scattering angles. From these measurements, we derived cross sections and electron-impact coherence parameters associated with the electron scattering process which is time reverse of the actual experimentally studied process. This interpretation of the experiment is based on the theory of Macek and Herte. The experimental results were also interpreted in terms of cross sections and collision parameters associated with the actual experimental processes. Results obtained so far will be presented and plans for further studies will be discussed.

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Christopher J. M. Smith, Jan P. J. Driessen, Larry Eno +1 more

In a crossed beam atomic energy transfer experiment, relative cross sections are measured between initial and final magnetic substates of atomic orbitals in a three vector correlation experiment. A pulsed laser beam prepares Ca(4s5p 1P1) in a single magnetic sublevel ‖j1mi〉 with respect to the laser polarization vector. Subsequent collision with He at a well-defined relative velocity yields Ca(4s5p 3P2). The near-resonant Ca(4s5p 3P2) is probed by a second polarized pulsed laser, revealing its magnetic sublevel ‖j2mf〉 distribution with respect to the probe laser polarization vector. The experiment is analyzed in the collision frame where the direction of the initial relative velocity vector serves as the quantization axis. In this frame, the initial and final Ca states are characterized by substates ‖j1m1〉 and ‖j2m2〉, respectively. Fourteen collision frame cross sections are needed to describe the energy transfer completely. Eight of these cross sections are real and positive (conventional type—describing population transfer) and six are complex (coherence type—containing phase information). By symmetry, only 15 unique parameters for the real and imaginary parts of the cross sections are required, nine of which are obtained here using linear polarizations and collinear laser beams. Possible cases for circularly polarized light are also tabulated; measurement of these cases would provide several more parameters. For initial parallel preparation of the 1P1 p orbital with respect to the relative velocity (m1=0), the final 3P2 state is highly aligned in the m2=±1 and m2=±2 sublevels. Initial preparation of the p orbital perpendicular to the relative velocity vector (m1=±1) produces an aligned 3P2 state with greater population in the m2=0 and m2=±1 sublevels compared to the m2=±2 sublevels. Using the coherence information and symmetry, orientation cross sections are obtained into the m2=±1 sublevels (i.e., m preserving 1→1 and m-changing 1→−1) and are nearly identical. Preparation of the Ca p orbital perpendicular to the initial relative velocity enhances the state-specific collisional transfer of 1P1→3P2 by a factor of 2.2±0.2 over initial parallel preparation.

The Journal of Chemical Physics•Jun 1, 1992•34 citations

Description of polarization-dependent associative ionization of radiatively excited atoms

Gerard Nienhuis

We analyze the dependence of the rate of associative ionization of two radiatively excited atoms on the polarization properties of the exciting light. This provides a direct relation between the observed ion-production rate as a function of the polarization and the ionization rates for various combinations of the magnetic substates. We consider an atomic beam irradiated by a single laser beam, as well as an atomic vapor. The description applies to a recent experimental observation of a strong polarization dependence of the ionization rate in an atomic beam, and at the same time we suggest alternate experimental methods of analyzing the total cross sections of any inelastic or reactive binary collision of excited atoms as a function of the magnetic quantum numbers.

Physical Review A•Dec 1, 1982•44 citations
A formula has been obtained which describes the dependence of the overall cross section of the inelastic process in experiments with intersecting atomic and light beams on five parameters, two of which depend on the properties of the quasimolecule and the collisional energy, and three others on the degree of linear polarization of the exciting light and two angles which determine the geometry of the experiment. It was shown that measuring the overall cross section by varying the two latter parameters allows us to obtain additional information on the mechanism of the reactions. As an example, the experimentally studied process of spin transfer in Ca(4s5p/sup 1/P/sub 1/)+He and the process of Penning ionization of He(2/sup 1/P/sub 1/)+Cd(Zn) has been considered.
The results of theoretical study of orientation, alignment and coherence effects in atomic collisions are presented. The conventional and coherence cross-sections that can be measured in collisional experiments with atomic beams are expressed via quantities dependent on the dynamics only and independent of geometry. The quantities introduced are the generalized Grawert parameters describing the collisional processes that occur in gas cell experiments (average cross-sections). The generalization of Grawert parameters allows us to obtian direct relationships between the average cross-sections and the conventional and coherence cross-sections.
The alignment of atomic states as the result of collisions with a beam of slow charged particles is investigated. The problem of the collisional reorientation of atomic moments is solved by numerical integration of the equations of the impact parameter method taking into account charge--quadrupole interaction. Calculations are made of the alignment of the /sup 2/P/sub 3//sub ///sub 2/ levels of alkali atoms populated by collisions with selective excitation of the /sup 2/P/sub 1//sub ///sub 2/ level. The linear polarization of light emitted by the /sup 2/P/sub 3//sub ///sub 2/ level attains some tens of percents and corresponds to the predominance of polarization in directions perpendicular to the beam. The efficiency of the resulting alignment depends on the volume density but not on the velocity of the beam of charged particles. Thus the slow drift of ions (and electrons) in a gas-discharge plasma can compete with alignment as the result of fluxes of charged particles. We shall formulate the sum rules for anisotropic collisional relaxation of atomic polarization moments. It follows from these that for the appearance of alignment in intramultiplet mixing under the action of anisotropic collisions we require a nonuniform population of multiplet levels that differs from the more » ratio of their statistical weights. « less
Experimental studies concerning elastic and inelastic electron scattering by coherently ensembles of Ba (...6s6p (sub 1)P(sub 1)) atoms with various degrees of alignment will be described. An in-plane, linearly-polarized laser beam was utilized to prepare these target ensembles and the electron scattering signal as a function of polarization angle was measured for several laser geometries at fixed impact energies and scattering angles. From these measurements, we derived cross sections and electron-impact coherence parameters associated with the electron scattering process which is time reverse of the actual experimentally studied process. This interpretation of the experiment is based on the theory of Macek and Herte. The experimental results were also interpreted in terms of cross sections and collision parameters associated with the actual experimental processes. Results obtained so far will be presented and plans for further studies will be discussed.
In a crossed beam atomic energy transfer experiment, relative cross sections are measured between initial and final magnetic substates of atomic orbitals in a three vector correlation experiment. A pulsed laser beam prepares Ca(4s5p 1P1) in a single magnetic sublevel ‖j1mi〉 with respect to the laser polarization vector. Subsequent collision with He at a well-defined relative velocity yields Ca(4s5p 3P2). The near-resonant Ca(4s5p 3P2) is probed by a second polarized pulsed laser, revealing its magnetic sublevel ‖j2mf〉 distribution with respect to the probe laser polarization vector. The experiment is analyzed in the collision frame where the direction of the initial relative velocity vector serves as the quantization axis. In this frame, the initial and final Ca states are characterized by substates ‖j1m1〉 and ‖j2m2〉, respectively. Fourteen collision frame cross sections are needed to describe the energy transfer completely. Eight of these cross sections are real and positive (conventional type—describing population transfer) and six are complex (coherence type—containing phase information). By symmetry, only 15 unique parameters for the real and imaginary parts of the cross sections are required, nine of which are obtained here using linear polarizations and collinear laser beams. Possible cases for circularly polarized light are also tabulated; measurement of these cases would provide several more parameters. For initial parallel preparation of the 1P1 p orbital with respect to the relative velocity (m1=0), the final 3P2 state is highly aligned in the m2=±1 and m2=±2 sublevels. Initial preparation of the p orbital perpendicular to the relative velocity vector (m1=±1) produces an aligned 3P2 state with greater population in the m2=0 and m2=±1 sublevels compared to the m2=±2 sublevels. Using the coherence information and symmetry, orientation cross sections are obtained into the m2=±1 sublevels (i.e., m preserving 1→1 and m-changing 1→−1) and are nearly identical. Preparation of the Ca p orbital perpendicular to the initial relative velocity enhances the state-specific collisional transfer of 1P1→3P2 by a factor of 2.2±0.2 over initial parallel preparation.
We analyze the dependence of the rate of associative ionization of two radiatively excited atoms on the polarization properties of the exciting light. This provides a direct relation between the observed ion-production rate as a function of the polarization and the ionization rates for various combinations of the magnetic substates. We consider an atomic beam irradiated by a single laser beam, as well as an atomic vapor. The description applies to a recent experimental observation of a strong polarization dependence of the ionization rate in an atomic beam, and at the same time we suggest alternate experimental methods of analyzing the total cross sections of any inelastic or reactive binary collision of excited atoms as a function of the magnetic quantum numbers.