Influence of asymmetry and nodal planes on high-harmonic generation in heteronuclear molecules

Abstract

The relation between high-harmonic spectra and the geometry of the molecular orbitals in position and momentum space is investigated. In particular we choose two isoelectronic pairs of homonuclear and heteronuclear molecules, such that the highest occupied molecular orbital of the former exhibit at least one nodal plane. The imprint of such planes is a strong suppression in the harmonic spectra, for particular alignment angles. We are able to identify two distinct types of nodal planes. If the nodal planes are determined by the atomic wavefunctions only, the angle for which the yield is suppressed will remain the same for both types of molecules. In contrast, if they are determined by the linear combination of atomic orbitals at different centers in the molecule, there will be a shift in the angle at which the suppression occurs for the heteronuclear molecules, with regard to their homonuclear counterpart. This shows that, in principle, molecular imaging, which uses the homonuclear molecule as a reference and enables one to observe the wavefunction distortions in its heteronuclear counterpart, is possible.

14 pages, 7 figures. Figs. 3, 5 and 6 have been simplified in order to comply with the arXiv size requirements

References in corpus (6)

• Photoelectron angular distributions from strong-field ionization of oriented molecules
• Laser-induced alignment and orientation of quantum-state-selected large molecules
• Field-free orientation of CO molecules by femtosecond two-color laser fields
• High-harmonic generation from arbitrarily oriented diatomic molecules including nuclear motion and field-free alignment
• Inducing elliptically polarized high-order harmonics from aligned molecules with linearly polarized femtosecond pulses
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Cited by in corpus (6)

• Two-center minima in harmonic spectra from aligned polar molecules
• Holographic detection of parity in atomic and molecular orbitals
• Multielectron corrections in molecular high-order harmonic generation for different formulations of the strong-field approximation
• Excitation, two-center interference and the orbital geometry in laser-induced nonsequential double ionization of diatomic molecules
• Imprints of the molecular-orbital geometry on the high-harmonic ellipticity
• Angle-Resolved Spectra of the Direct Above-Threshold Ionization of Diatomic Molecule in IR+XUV laser field