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Phys Rev Lett. 2006 Feb 24;96(7):073906. Epub 2006 Feb 24.

Three-step model for high-harmonic generation in many-electron systems.

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Argonne National Laboratory, Argonne, Illinois 60439, USA.


The three-step model (TSM) of high-harmonic generation (HHG) is generalized to atomic and molecular many-electron systems. Using many-body perturbation theory, corrections to the standard TSM due to exchange and electron-electron correlations are derived. It is shown that canonical Hartree-Fock orbitals represent the most appropriate set of one-electron states for calculating the HHG spectrum. To zeroth order in many-body perturbation theory, a HHG experiment allows direct access, in general, to a combination of occupied Hartree-Fock orbitals rather than to the highest occupied molecular orbital by itself.

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