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Molecular high-order harmonic generation: analysis of a destructive interference condition

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S Odžak1 and D B Milošević1,2

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The multiple-slit type destructive interference in molecular high-order harmonic generation (HHG) leads to the minima in the harmonic yield for particular molecular orientation angle θL and the harmonic order n. For the case of homonuclear diatomic molecules, we have found a condition for this destructive interference in the form of a nonlinear equation over n and θL. This condition strongly depends on the molecular symmetry, on the atomic orbitals of which a particular highest occupied molecular orbital (HOMO) consists and on the internuclear distance R. Therefore, one can learn about the molecular structure and dynamics analysing the HHG spectra of aligned molecules. Using the example of an Ar2 molecule, having 5σu HOMO, for various internuclear distances, we analyse this interference condition and show that, in the (n, θL) plane, it manifests in the form of one or several continuous curves. Furthermore, in the (Rcos θL, λmin) plane, where λmin is an effective de Broglie wavelength of the recombining electron, this condition leads to a set of lines which are positioned between the limiting cases of molecular orbitals consisting of only one type (even or odd) of atomic orbitals (s and p in the Ar2 case).


PACS

42.65.Ky Frequency conversion; harmonic generation, including higher-order harmonic generation

33.80.-b Photon interactions with molecules

33.15.Bh General molecular conformation and symmetry; stereochemistry

Subjects

Atomic and molecular physics

Optics, quantum optics and lasers

Dates

Issue 7 (14 April 2009)

Received 11 February 2009

Published 23 March 2009



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