We present a valence orbital method of calculating high-order harmonic generation from a diatomic molecule with arbitrary orientation by using a space rotation operator. We evaluate the effects of each valence orbital...We present a valence orbital method of calculating high-order harmonic generation from a diatomic molecule with arbitrary orientation by using a space rotation operator. We evaluate the effects of each valence orbital on harmonic emissions from N2 and O2 molecules in detail separately. The calculation results confirm the different properties of harmonic yields from N2 and O2 molecules which are well consistent with available experimental data. We observe that due to the orientation dependence of ／sigma and ／pi orbitals, the bonding orbital （π2pz）^2 of N2 determines the maximum of harmonic emission when the molecular axis of N2 is aligned parallel to the laser vector, and the magnitude of the high harmonic signal gradually weakens with the orientation angle of molecular axis increasing. But for O2 molecule the antibonding orbitals （π2pz）^1 and （π2pz）^1 contribute to the maximum of harmonic yield when O2 is aligned at 45° and bonding orbitals （π2pz）^2 and （π2pz）^2 slightly influence the orientation angle of maximum of harmonic radiation not exactly at 45°.展开更多
基金supported by the National Natural Science Foundation of China (Grant Nos. 10774033, 60878018 and 10674036)the Program of Excellent Team in Harbin Institute of Technologythe Program for New Century Excellent Talents in University(NCET),China (Grant No. NCET-04-0319)
文摘We present a valence orbital method of calculating high-order harmonic generation from a diatomic molecule with arbitrary orientation by using a space rotation operator. We evaluate the effects of each valence orbital on harmonic emissions from N2 and O2 molecules in detail separately. The calculation results confirm the different properties of harmonic yields from N2 and O2 molecules which are well consistent with available experimental data. We observe that due to the orientation dependence of ／sigma and ／pi orbitals, the bonding orbital （π2pz）^2 of N2 determines the maximum of harmonic emission when the molecular axis of N2 is aligned parallel to the laser vector, and the magnitude of the high harmonic signal gradually weakens with the orientation angle of molecular axis increasing. But for O2 molecule the antibonding orbitals （π2pz）^1 and （π2pz）^1 contribute to the maximum of harmonic yield when O2 is aligned at 45° and bonding orbitals （π2pz）^2 and （π2pz）^2 slightly influence the orientation angle of maximum of harmonic radiation not exactly at 45°.
