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Physical Review A

Anisotropy of excited He+ formed in the photoionization of helium

H. R. Sadeghpour, Chris H. Greene

Published Jan 1, 1989• 13 citations
Publisher

Abstract

Semianalytic methods are developed to predict the alignment and orientation of excited helium ions produced in the photoionization of neutral helium in the low-energy limit. The ionic electron probability distribution is shown to align itself orthogonal to the direction of the incident light polarization axis in the same manner as the photoelectron angular distribution [C.H. Greene, Phys. Rev. Lett. 44, 869 (1980)]. In certain instances, propensity rules for the alignment and orientation of the ionic electron are violated. Coherent contributions from different degenerate orbital angular momenta are seen to be partially responsible for these ``unfavored'' trends. Explicit predictions of the time-unresolved fluorescence polarization are presented, including the effects of fine-structure depolarization.

DOI
10.1103/physreva.39.115

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Semianalytic methods are developed to predict the alignment and orientation of excited helium ions produced in the photoionization of neutral helium in the low-energy limit. The ionic electron probability distribution is shown to align itself orthogonal to the direction of the incident light polarization axis in the same manner as the photoelectron angular distribution [C.H. Greene, Phys. Rev. Lett. 44, 869 (1980)]. In certain instances, propensity rules for the alignment and orientation of the ionic electron are violated. Coherent contributions from different degenerate orbital angular momenta are seen to be partially responsible for these ``unfavored'' trends. Explicit predictions of the time-unresolved fluorescence polarization are presented, including the effects of fine-structure depolarization.
The alignment-orientation process is exactly treated for an alkali-like atom with purely electronic couplings. Analytic expressions for the circular polarization of the optical emission are given for specific types of anisotropic excitation in terms of the magnetic field and the spin-orbit parameter. No advanced formalism is used. It is shown how the hyperfine interaction with the electron orbital motion operates in a manner very similar to the purely electronic spin-orbit coupling, again leading to orbital orientation and to circularly polarized optical emission. Detailed computed results for alignment-orientation conversion for neutral helium are summarized, as are the results of experiments which directly exhibit circularly polarized emission due to the alignment-orientation effect in gases.
A method alternative to the density matrix formalism is applied to derive a general expression for the radiative decay probability following the photoionization of polarized atoms in two-step approximation. The graphical technique of the angular momentum theory is used for the integration over angular and spin variables. The general expression joining both steps of photoionization and fluorescence contains the possibility to investigate the polarization of all particles in the initial and final states and the angular distributions as well as angular correlations of photoelectrons and radiation. A simple way to get the expressions for special cases of the angular distribution and polarization of fluorescence radiation in the photoionization of randomly orientated and polarized atoms is given as an example of the practical application of the general formula.
Anisotropy of angular momenta: ideas and methods The fundamental idea forming the basis of early quantum theory was the quantization of the angular momentum of the atom, which, at a later stage, assumed the form of the Bohr–Sommerfeld quantization rule [360], namely ∲ pdq = n ℏ where p and q are the generalized momentum and coordinate. This concept has retained its physical meaning in modern-day quantum mechanics [371, 372]. In the course of the further development of quantum mechanical concepts it became increasingly clear that in the theory of atoms and molecules the angular momentum is a ‘dominant’ notion, the fundamental significance of which is in no small degree connected with its dimension of action, which coincides with that of Planck's constant ℏ. In the interaction between particles and a directed beam of photons the angular momentum of the system is conserved, thus forming the basis for the optical method of producing spatial anisotropy of the distribution of the angular momenta of the ensemble of particles, i.e. its optical polarization . In terms of quantum concepts, spatial anisotropy means that in an ensemble of particles a non-equilibrium population of magnetic sublevels m j of angular momenta is created. We make a distinction between the alignment of momenta, for instance in the absorption of linear polarized light, when there is no difference between the population of ± m j -sublevels, and orientation , when such a difference exists. Anisotropic distribution of angular momenta in an excited state, as produced in absorption, manifests itself directly in the polarization of fluorescence. It is rather likely that understanding of the anisotropic distribution of the angular momenta of atoms was enhanced by Hanle's [184] discovery in 1924.
The mixing of state multipoles for an atomic state with unresolved fine structure in a magnetic field is investigated in its simplest case: the conversion of alignment to orientation. The combined action of the external field and the spin-orbit coupling results in a build-up of orientation and hence in the emission of circularly polarised light although the excitation process is axially symmetric and is invariant with respect to the reversal of the symmetry axis and thus the system could only show alignment initially. The case investigated is the collisional excitation of the He 3 3 D state by He + ions. After correction of some errors in the theoretical literature the agreement between the calculated and the observed circular polarisation of the fluorescence radiation from the collisionally excited He atoms is very good. Owing to possible objections in two previous experiments this is the first unambiguous demonstration of the alignment to orientation conversion effect.
The asymmetry parameter β for fluorescence photons emitted during the radiative decay of the sp2, n +( 1 P o ), sp2, n −( 1 P o ), 2p n d( 1 P o ) and 2p n d( 3 D o ) series of helium doubly excited states, formed by the absorption of linearly polarized synchrotron radiation, has been measured. The results are compared with recent theoretical calculations (Žitnik et al 2002 Phys. Rev. A 65 032520). At high n the β parameter is shown to increase and oscillate due to the excitation of triplet states, optically accessible from the helium ground state due to spin–orbit effects.
We observe the parity-unfavored photoelectron emission in multiphoton single ionization of krypton atoms in an intense ultraviolet laser field. With systematic experiments of successively varying the light ellipticity and intensity, we identify that this parity-unfavored emission is associated with the first excited ionic state via a resonant pathway. We reveal an abnormal Coulomb asymmetry of the parity-unfavored photoelectron emission in elliptically polarized fields when the ellipticity is less than 0.3. The simulation using the time-dependent Schr\"odinger equation based on single-active-electron approximation fails to reproduce the experiment. We attribute the experimental observations to the angular momentum correlation between the resonantly excited electron and the spin-orbit excited ion. Our results demonstrate that the well-known picture of the angular momentum transfer in multiphoton ionization is broken and instead that the electron shares the spin angular momenta of photons with the ion as an effect of electron correlations.