Effects of multiple electronic shells on strong-field multiphoton ionization and high-order harmonic generation of diatomic molecules with arbitrary orientation: An all-electron time-dependent density-functional approach

Journal Article · Thu Oct 15 04:00:00 EDT 2009 · Physical Review. A

DOI:https://doi.org/10.1103/PHYSREVA.80.043412· OSTI ID:21316432

Telnov, Dmitry A ^[1]; Chu, S -I ^[2]

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1. Department of Physics, St. Petersburg State University, 198504 St. Petersburg (Russian Federation)
2. Department of Chemistry, University of Kansas, Lawrence, Kansas 66045 (United States)

We present a time-dependent density-functional theory approach with proper long-range potential for an ab initio study of the effect of correlated multielectron responses on the multiphoton ionization (MPI) and high-order harmonic generation (HHG) of diatomic molecules N{sub 2} and F{sub 2} in intense short laser pulse fields with arbitrary molecular orientation. We show that the contributions of inner molecular orbitals to the total MPI probability can be sufficiently large or even dominant over the highest-occupied molecular orbital, depending on detailed electronic structure and symmetry, laser field intensity, and orientation angle. The multielectron effects in HHG are also very important. They are responsible for enhanced HHG at some orientations of the molecular axis. Even strongly bound electrons may have a significant influence on the HHG process.

• OSTI ID: 21316432
• Journal Information: Physical Review. A, Journal Name: Physical Review. A Journal Issue: 4 Vol. 80; ISSN 1050-2947; ISSN PLRAAN
• Country of Publication: United States
• Language: English

Related Subjects

74 ATOMIC AND MOLECULAR PHYSICS
DENSITY FUNCTIONAL METHOD
ELECTRONIC STRUCTURE
ELECTRONS
FLUORINE
HARMONIC GENERATION
LASER RADIATION
LASERS
MOLECULAR ORBITAL METHOD
MOLECULAR STRUCTURE
MOLECULES
MULTI-PHOTON PROCESSES
NITROGEN
ORIENTATION
PHOTOIONIZATION
PHOTON-MOLECULE COLLISIONS
POTENTIALS
TIME DEPENDENCE