High-order-harmonic generation in homonuclear and heteronuclear diatomic molecules: Exploration of multiple orbital contributions
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Issue Date
2011-04-22Author
Heslar, John
Telnov, Dmitry A.
Chu, Shih-I
Publisher
American Physical Society
Type
Article
Article Version
Scholarly/refereed, publisher version
Metadata
Show full item recordAbstract
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 (N2 and F2) 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.
Description
This is the publisher's version, also available electronically from http://journals.aps.org/pra/abstract/10.1103/PhysRevA.83.043414.
ISSN
1050-2947Collections
Citation
Heslar, John; Telnov, Dmitry A.; Chu, Shih-I. (2011). "High-order-harmonic generation in homonuclear and heteronuclear diatomic molecules: Exploration of multiple orbital contributions." Physical Review A, 83(04):043414. http://dx.doi.org/10.1103/PhysRevA.83.043414
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