Breakdown of the electric dipole approximation at Cooper minima in direct two-photon ionisation

We predict breakdown of the electric dipole approximation at nonlinear Cooper minimum in direct two-photon K-shell atomic ionisation by circularly polarised light. According to predictions based on the electric dipole approximation, we expect that tuning the incident photon energy to the Cooper minimum in two-photon ionisation results in pure depletion of one spin projection of the initially bound 1s electrons, and hence, leaves the ionised atom in a fully oriented state. We show that by inclusion of electric quadrupole interaction, dramatic drop of orientation purity is obtained. The low degree of the remaining ion orientation provides a direct access to contributions of the electron-photon interaction beyond the electric dipole approximation in the two-photon ionisation of atoms and molecules. The orientation of the photoions can be experimentally detected either directly by a Stern-Gerlach analyzer, or by means of subsequent Kα fluorescence emission, which has the information about the ion orientation imprinted in the polarisation of the emitted photons.