期刊
PHYSICAL REVIEW A
卷 80, 期 4, 页码 -出版社
AMER PHYSICAL SOC
DOI: 10.1103/PhysRevA.80.043412
关键词
ab initio calculations; density functional theory; fluorine; harmonic generation; molecular configurations; molecular electronic states; molecular orientation; molecule-photon collisions; multiphoton processes; nitrogen; photoionisation
资金
- Division of the Office of Basic Energy Sciences
- Office of Sciences
- U. S. Department of Energy
- U. S. National Science Foundation
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-2 and F-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.
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