Multiphoton ionization and high-order harmonic generation of He, Ne, and Ar atoms in intense pulsed laser fields: Self-interaction-free time-dependent density-functional theoretical approach

We present a detailed study of the multiphoton ionization and high-order harmonic generation (HHG) processes of rare-gas atoms (He, Ne, and Ar) in intense pulsed laser fields by means of a self-interaction-free time-dependent density-functional theory (TDDFT) recently developed. The time-dependent exchange-correlation potential with proper short- and long-range potential is constructed by means of the time-dependent optimized effective potential (TDOEP) method and the incorporation of an explicit self-interaction-correction (SIC) term. The TDOEP-SIC equations are solved accurately and efficiently by the time-dependent generalized pseudospectral technique. In this study, all the valence electrons are treated explicitly and nonperturbatively and their partial contributions to the ionization and HHG are analyzed. The results reveal instructive and qualitatively different behavior from each subshell orbital. Moreover, we found that the HHG yields from Ne and Ar atoms are considerably larger than that of the He atom in strong fields. Three main factors are identified for accounting the observed phenomena: (a) the binding energy of the subshell valence electron, (b) the orientation of the valence electron orbital (with respect to the electric-field polarization), and (c) the effect of multiphoton resonant excitation. In particular, we found that the np(0) valence electrons (in Ne and Ar) with lowest binding energies and electron orbital orientation parallel to the electric-field direction, make the dominant contributions to both ionization and HHG processes in sufficiently strong fields.