Two-Center Interference of Heteronuclear Diatomic Molecules in High-Order Harmonic Generation

Abstract

We have investigated the phenomenon of two-center destructive interference for heteronuclear diatomic molecules (HeDM) in the high-order harmonic generation, which results in the minimum in high-order harmonic spectrum. It is found that the minimum is shifted to lower harmonic orders compared with that in a homonuclear case, which is explained by performing phase analysis. The analysis shows that for an HeDM the 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). In addition to that, the possibility to monitor the evolution of HOMO itself in molecular dynamics is also promised.