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Physical Review Letters

Circular Dichroism in Photo-Single-Ionization of Unoriented Atoms

James M. Feagin

Published Jan 15, 2002• 5 citations
Publisher

Abstract

We predict circular dichroism in photo-single-ionization angular distributions from spherically symmetric atomic states if the ionized electron is detected using two-slit interferometry. We demonstrate that the resulting electron interference pattern captures phase information on quadrupole corrections to the photoionization amplitude lost in conventional angular distributions.

DOI
10.1103/physrevlett.88.043001

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We predict circular dichroism in photo-single-ionization angular distributions from spherically symmetric atomic states if the ionized electron is detected using two-slit interferometry. We demonstrate that the resulting electron interference pattern captures phase information on quadrupole corrections to the photoionization amplitude lost in conventional angular distributions.
In quantum mechanics the Young-type double-slit experiment can be performed with electrons either traveling through a double slit or being coherently emitted from two inversion symmetric molecular sites. In the latter one the valence photoionization cross sections of homonuclear diatomic molecules were predicted to oscillate over kinetic energy almost 50 years ago. Beyond the direct proof of the oscillatory behavior of these photoionization cross sections σ, we show that the angular distribution of the emitted electrons reveals hitherto unexplored information on the relative phase shift between the corresponding partial waves through two-center interference patterns.
Circular dichroism has been detected in the polarization of the fluorescence resulting from the decay of excited calcium ions. Synchrotron radiation was used to both ionize and excite calcium atoms from their ground state, and the photoejected electron was detected in coincidence with the polarized fluorescent photon. By introducing a degree of left, then right circularly polarized light into the incident photon beam the circular dichroism could be measured. The analysis of the results was carried out using recent developments of the statistical tensor method, and it was possible to determine the sign of the phase difference between the outgoing waves.
In multiphoton ionization of atoms, elliptical dichroism may arise in the photoelectron angular distributions due to the interference of the possible ionization pathways. We here consider the interaction of atoms with an elliptically polarized biharmonic ($\ensuremath{\omega} + 2\ensuremath{\omega}$) field which simultaneously allows one- and two-photon ionization of the atoms. The interference between these two ionization pathways introduces contributions to the elliptical dichroism in addition to the dichroism that arises from the two-photon ionization alone. We show that these additional dichroism contributions can lead to a stronger dichroism in comparison to the one arising from two-photon ionization only. We present a relativistic analysis of the corresponding photoelectron angular distributions and discuss individual contributions to the dichroic phenomena. Detailed computations have been performed for biharmonic ionization of neutral helium atoms.
The ion momentum distribution in the x-ray-induced dissociative photoionization of molecules is investigated, treating the ionization analytically under the Born-Oppenheimer approximation and simulating numerically the ion motion via the Schrödinger equation. The ion-photoelectron entanglement transfers information of the electronic interference to the ion dynamics. As a consequence, the ion momentum distributions of dissociative molecular photoionization present Young's double-slit interference when the photoelectron emission angle is fixed. We demonstrate that double-slit interference signatures persist in the ion longitudinal momentum shift even when the information of the correlated photoelectron is lost, which is the case for heteronuclear molecules when an additional photoelectron recoil momentum arises due to the different ion masses. For the case of sequential double ionization, we show that double-slit interference in the ion dynamics can be utilized for coherent control of the molecular dynamics.
The polarization dependence of the photoionization probability was analyzed in the case when a randomly oriented atom is irradiated by two crossing polarized monochromatic photon beams with the same frequency. It was found that the angular distributions of photoelectrons exhibit the effect of circular dichroism (CD), which consists of the dependence of the photoionization probability on the sign of the circular polarization degree of each beam. We demonstrate that the CD effect exists only for coherent crossing photon beams. It was shown that CD effects are strongly dependent on the phase difference between the electric field vectors of the photon beams and have a quite large magnitude. The possibilities of the experimental observation of CD effects are discussed.