Dependence upon the molecular and atomic ground state of higher-order harmonic generation in the few-optical-cycle regime

Abstract

High-order harmonic generation from molecules (${\mathrm{O}}_{2}$, ${\mathrm{N}}_{2}$, ${\mathrm{H}}_{2}$, and $\mathrm{C}{\mathrm{O}}_{2}$) and atoms (Xe, Ar, and Kr) has been studied in the few optical cycle domain. Two laser peak intensities; $2\ifmmode\times\else\texttimes\fi{}{10}^{14}$ and $6\ifmmode\times\else\texttimes\fi{}{10}^{14}\phantom{\rule{0.3em}{0ex}}\mathrm{W}\phantom{\rule{0.2em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}2}$, were compared. At the lower intensity spectra were approximately the same for molecules and atoms with the same ionization potential, at higher laser intensity the cutoff of ${\mathrm{O}}_{2}$ and $\mathrm{C}{\mathrm{O}}_{2}$ extends far beyond the cutoff of Xe and Kr, respectively, in contrast with ${\mathrm{N}}_{2}$ and ${\mathrm{H}}_{2}$ which exhibit cutoffs very close to that of Ar. This behavior is well explained by adopting an atomlike approximation for the molecule response in the high-field regime and employing the Lewenstein's model, properly modified in order to account for the nonlinear dipole moment of a randomly oriented molecule ensemble.