High-order-harmonic generation in homonuclear and heteronuclear diatomic molecules: Exploration of multiple orbital contributions
- Center for Quantum Science and Engineering, Department of Physics, National Taiwan University, Taipei 10617, Taiwan (China)
- Department of Physics, St. Petersburg State University, 198504 St. Petersburg (Russian Federation)
We present a time-dependent density functional theory (TDDFT) approach with proper asymptotic long-range potential for nonperturbative treatment of high-order harmonic generation (HHG) of diatomic molecules with their molecular axis parallel to the laser field polarization. A time-dependent two-center generalized pseudospectral method in prolate spheroidal coordinate system is used for accurate and efficient treatment of the TDDFT equations in space and time. The theory is applied to a detailed all-electron nonperturbative investigation of HHG processes of homonuclear (N{sub 2} and F{sub 2}) and heteronuclear (CO, BF, and HF) molecules in intense ultrashort laser pulses with the emphasis on the role of multiple molecular orbitals (MOs). The results reveal intriguing and substantially different nonlinear optical response behaviors for homonuclear and heteronuclear molecules. In particular, we found that the HHG spectrum for homonuclear molecules features a destructive interference of MO contributions while heteronuclear molecules show mostly constructive interference of orbital contributions.
- OSTI ID:
- 21544656
- Journal Information:
- Physical Review. A, Journal Name: Physical Review. A Journal Issue: 4 Vol. 83; ISSN 1050-2947; ISSN PLRAAN
- Country of Publication:
- United States
- Language:
- English
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Related Subjects
ASYMPTOTIC SOLUTIONS
CALCULATION METHODS
CARBON COMPOUNDS
CARBON MONOXIDE
CARBON OXIDES
CHALCOGENIDES
CONFIGURATION
DENSITY FUNCTIONAL METHOD
ELECTROMAGNETIC RADIATION
ELECTRONS
ELEMENTARY PARTICLES
ELEMENTS
FERMIONS
FLUORINE
FLUORINE COMPOUNDS
FREQUENCY MIXING
HALOGEN COMPOUNDS
HALOGENS
HARMONIC GENERATION
HYDROFLUORIC ACID
HYDROGEN COMPOUNDS
INORGANIC ACIDS
INORGANIC COMPOUNDS
INTERFERENCE
LASER RADIATION
LEPTONS
MATHEMATICAL SOLUTIONS
MOLECULAR ORBITAL METHOD
MOLECULES
NITROGEN
NONLINEAR PROBLEMS
NONMETALS
OXIDES
OXYGEN COMPOUNDS
POLARIZATION
POTENTIALS
PULSES
RADIATIONS
SPACE DEPENDENCE
SPECTRA
SPHERICAL CONFIGURATION
TIME DEPENDENCE
VARIATIONAL METHODS