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Title: 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

Abstract

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.

Authors:
;  [1]
  1. Laboratoire de Chimie Theorique, Faculte des Sciences, Universite de Sherbrooke, Quebec, J1K 2R1 (Canada)
Publication Date:
OSTI Identifier:
22072234
Resource Type:
Journal Article
Journal Name:
Physical Review. A
Additional Journal Information:
Journal Volume: 84; Journal Issue: 3; Other Information: (c) 2011 American Institute of Physics; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 1050-2947
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; DENSITY FUNCTIONAL METHOD; HARMONIC GENERATION; IONIZATION; IONIZATION POTENTIAL; LASERS; MOLECULAR ORBITAL METHOD; MOLECULES; NONLINEAR PROBLEMS; NUMERICAL SOLUTION; POLARIZATION; PULSES; TIME DEPENDENCE

Citation Formats

Penka Fowe, Emmanuel, and Bandrauk, Andre D. 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. United States: N. p., 2011. Web. doi:10.1103/PHYSREVA.84.035402.
Penka Fowe, Emmanuel, & Bandrauk, Andre D. 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. United States. https://doi.org/10.1103/PHYSREVA.84.035402
Penka Fowe, Emmanuel, and Bandrauk, Andre D. Thu . "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". United States. https://doi.org/10.1103/PHYSREVA.84.035402.
@article{osti_22072234,
title = {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},
author = {Penka Fowe, Emmanuel and Bandrauk, Andre D},
abstractNote = {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.},
doi = {10.1103/PHYSREVA.84.035402},
url = {https://www.osti.gov/biblio/22072234}, journal = {Physical Review. A},
issn = {1050-2947},
number = 3,
volume = 84,
place = {United States},
year = {2011},
month = {9}
}