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Physical Review Letters

Spin-Orbit Coupling and Photoelectron Polarization in Multiphoton Ionization of Atoms

P. Lambropoulos

Published Mar 5, 1973• 78 citations
Publisher

Abstract

It is shown that multiphoton ionization of unpolarized atoms with circularly polarized light can lead to the production of highly polarized electrons. The connection of this effect with the Fano effect in single-photon ionization is discussed.
DOI
10.1103/physrevlett.30.413

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The theory of multiphoton ionization for an atomic system of arbitrary complexity is developed using a density matrix formalism. An expression is obtained which determines the differential N-photon ionization cross section as a function of the polarization states of the target atom and the incident radiation. The parameters which characterize the photo-electron angular distribution are related to the general reduced matrix elements for the N-photon transition. Two-photon ionization of unpolarized atoms is treated as an illustration of the use of the theory. The dependence of the multiphoton ionization cross section on the polarization state of the incident radiation, which has been observed in two- and three-photon ionization of Cs, is accounted for by the theory. Finally, the photoelectron spin polarization produced by the multiphoton ionization of unpolarized atoms, like the analogous polarization resulting from single-photon ionization, is found to depend on the circular polarization of the incident radiation.
We propose two realistic schemes for producing electron spin-polarized alkaline-earth ions. One of the schemes is based on one-photon resonant two-photon ionization via fine structure manifolds of triplet states, while the other is based on one-photon resonant one-photon ionization. For both schemes we find that the ionization must take place from a triplet state to produce spin-polarized photoions. Photoions produced from a singlet state are always unpolarized regardless of the laser polarization and a magnetic sublevel from which ionization takes place. We carry out specific analysis for both schemes with Sr atoms, and find 85%–90% and 66% polarizations for the former and the latter schemes, respectively, if the wavelengths and polarizations of lasers are judiciously chosen. In particular, if all the produced photoions are in the ground s state, we find an exact one-to-one correspondence between the spin-polarization of photoions and ejected photoelectrons.