Multiorbital effects in high-order harmonic emission from CO2

We study the ellipticity of high-order harmonics emitted from CO2 molecule driven by linearly polarized laser fields using numerical simulations within the time-dependent density functional theory. We find that the overall ellipticity of the harmonics is small, which is in agreement with experimen- tal data. On the other hand, our analysis of the numerical results indicates that several valence orbitals contribute significantly to the harmonic emission and some of these contributions show a strong ellipticity of the harmonics. The small ellipticity in the total harmonics signal arises from a combination of factors, namely, the fact that harmonic emission from different orbitals is strongest at different alignment angles of the molecular axis with respect to the laser polarization direction, as well as interference effects and a strong laser coupling between several inner valence orbitals.