Role of molecular orbital symmetry on the alignment dependence of high-order harmonic generation with molecules

Abstract

It is shown that the alignment dependence of the yields of high-order harmonic generation (HHG) from molecules by intense lasers is governed by the orbital symmetry of the outermost electron(s). For N2, with its outermost σg electron, the HHG yield is maximal when the molecules are aligned with the laser polarization direction, in agreement with the recent experiment of Itatani [Nature 432, 867 (2004)]. For O2, with its outermost πg electron, the HHG yield peaks when the molecules are aligned at about 45° from the polarization axis. We emphasize that the alignment dependence is determined mostly by the orbital symmetry and weakly on the laser parameters or the species. © 2005 The American Physical Society.