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Opt Express. 2011 Jan 17;19(2):436-47. doi: 10.1364/OE.19.000436.

Two-center interference in high-order harmonic generation from heteronuclear diatomic molecules.

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  • 1Wuhan National Laboratory for Optoelectronics, Huazhong University of Science and Technology, Wuhan, China.


Two-center interference for heteronuclear diatomic molecules (HeDM) is investigated. The minimum in the high-order harmonic spectrum, as a consequence of the destructive interference, is shifted to lower harmonic orders compared with that in a homonuclear case. This phenomenon is explained by performing phase analysis. It is found that, for an HeDM, the high harmonic spectrum contains information not only on the internuclear separation but also on the properties of the two separate centers, which implies the potential application of estimating the asymmetry of molecules and judging the linear combination of atomic orbitals (LCAO) for the highest occupied molecular orbital (HOMO). Moreover, the possibility to monitor the evolution of HOMO itself in molecular dynamics is also promised.

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