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Advances in atomic and molecular physics

Angular Correlation in Multiphoton Ionization of Atoms

Stephen J. Smith, Gerd Leuchs

Published Jan 1, 1988• 46 citations
Publisher
DOI
10.1016/s0065-2199(08)60231-6

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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.

Journal of Physics B Atomic and Molecular Physics•Aug 1, 1973•28 citations
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.
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.