Abstract

We investigate the connection between high-harmonic spectra and the geometry of the molecular orbitals in position and momentum space, by choosing two isoelectronic pairs of homonuclear and heteronuclear molecules. In all cases, we assume that the highest occupied molecular orbital of the former exhibit at least one nodal plane. From the high-order harmonic spectra, 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. However, if they are determined by the linear combination of atomic orbitals at different centers in the molecule, the angles for which this suppression occurs will be shifted for the heteronuclear molecules. Hence, in principle, one may use a homonuclear molecule as a reference in molecular imaging, in order to observe the wavefunction distortions in its heteronuclear counterpart.

© 2011 Optical Society of America