Nonperturbative time-dependent density-functional theory of ionization and harmonic generation in OCS and CS{sub 2} molecules with ultrashort intense laser pulses: Intensity and orientational effects
- Laboratoire de Chimie Theorique, Faculte des Sciences, Universite de Sherbrooke, Quebec, J1K 2R1 (Canada)
Molecular high-order harmonic generation (MHOHG) and molecular orbital ionization rates are calculated for the nonsymmetric OCS and symmetric CS{sub 2} molecules using numerical solutions of Kohn-Sham (KS) equations of time-dependent density functional theory in the nonlinear nonperturbative regime of laser-molecule interactions for different laser-molecule orientations and intensities. It is found that the ionization of inner-shell KS molecular orbitals contributes significantly to the ionization and MHOHG processes for intensities I{>=} 3.5 x 10{sup 14} W/cm{sup 2}. Ionization rate maxima correspond to the alignment of maximum KS orbital densities with the laser pulse polarization instead of orbital ionization potentials. Furthermore, degeneracies of orbitals are removed as a function of laser-molecule angle, thus affecting ionization rates, the MHOHG spectra, and their polarizations, the latter allowing for identifying inner-orbital ionization.
- OSTI ID:
- 22072234
- Journal Information:
- Physical Review. A, Vol. 84, Issue 3; Other Information: (c) 2011 American Institute of Physics; Country of input: International Atomic Energy Agency (IAEA); ISSN 1050-2947
- Country of Publication:
- United States
- Language:
- English
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