High-order-harmonic generation in homonuclear and heteronuclear diatomic molecules: Exploration of multiple orbital contributions

Journal Article · Fri Apr 15 00:00:00 EDT 2011 · Physical Review. A

DOI:https://doi.org/10.1103/PHYSREVA.83.043414· OSTI ID:21544656

Heslar, John ^[1]; Telnov, Dmitry ^[2]; Chu, Shih-I ^[1]

---

1. Center for Quantum Science and Engineering, Department of Physics, National Taiwan University, Taipei 10617, Taiwan (China)
2. 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, Vol. 83, Issue 4; Other Information: DOI: 10.1103/PhysRevA.83.043414; (c) 2011 American Institute of Physics; ISSN 1050-2947
• Country of Publication: United States
• Language: English

Related Subjects

74 ATOMIC AND MOLECULAR PHYSICS
ASYMPTOTIC SOLUTIONS
CARBON MONOXIDE
DENSITY FUNCTIONAL METHOD
ELECTRONS
FLUORINE
HARMONIC GENERATION
HYDROFLUORIC ACID
INTERFERENCE
LASER RADIATION
MOLECULAR ORBITAL METHOD
MOLECULES
NITROGEN
NONLINEAR PROBLEMS
POLARIZATION
POTENTIALS
PULSES
SPACE DEPENDENCE
SPECTRA
SPHERICAL CONFIGURATION
TIME DEPENDENCE
CALCULATION METHODS
CARBON COMPOUNDS
CARBON OXIDES
CHALCOGENIDES
CONFIGURATION
ELECTROMAGNETIC RADIATION
ELEMENTARY PARTICLES
ELEMENTS
FERMIONS
FLUORINE COMPOUNDS
FREQUENCY MIXING
HALOGEN COMPOUNDS
HALOGENS
HYDROGEN COMPOUNDS
INORGANIC ACIDS
INORGANIC COMPOUNDS
LEPTONS
MATHEMATICAL SOLUTIONS
NONMETALS
OXIDES
OXYGEN COMPOUNDS
RADIATIONS
VARIATIONAL METHODS