Interference effects in high-order harmonic generation by homonuclear diatomic molecules

Abstract

A theory of high-order harmonic generation by diatomic molecules is introduced. Various versions (with or without the dressing of the initial and/or final molecular state) of the molecular strong-field approximation are investigated. Using examples of homonuclear diatomic molecules such as ${\mathrm{H}}_{2}$, ${\mathrm{N}}_{2}$, and ${\mathrm{O}}_{2}$, it is shown that clear two-center interference minima in the harmonic spectra as a function of the molecular orientation appear only if the final molecular state is undressed. For ${\mathrm{H}}_{2}$ the positions of these minima are in agreement with the ab initio numerical results. Physically, the returned electron wave packet recombines into a molecular orbital, which is a linear combination of the atomic orbitals having different parities. The interference minima in the harmonic spectrum are caused by the destructive interference of the corresponding partial recombination amplitudes. In accordance with this, we have derived an interference minima condition which is valid for arbitrary homonuclear diatomic molecules.