Uncovering multiple orbitals influence in high harmonic generation from aligned N2

Recent measurements on high-order harmonic generation (HHG) from N2 aligned perpendicular to the driving laser polarization (B K McFarland et al 2008 Science 322 1232) have shown a maximum at the rotational half-revival. This has been interpreted as the signature of the HHG contribution from the molecular orbital just below the highest occupied molecular orbital (HOMO). By using the recently developed quantitative rescattering theory combined with accurate photoionization transition dipoles, we show that the maximum at the rotational half-revival is indeed associated with the HOMO-1 contribution. Our results also show that the HOMO-1 contribution becomes increasingly more important near the HHG cutoff and therefore depends on the laser intensity. (fast track communication)