High-order harmonic generation from polyatomic molecules including nuclear motion and a nuclear modes analysis

Abstract

We present a generic approach for treating the effect of nuclear motion in the high-order harmonic generation from polyatomic molecules. Our procedure relies on a separation of nuclear and electron dynamics where we account for the electronic part using the Lewenstein model and nuclear motion enters as a nuclear correlation function. We express the nuclear correlation function in terms of Franck-Condon factors which allows us to decompose nuclear motion into modes and identify the modes that are dominant in the high-order harmonic generation process. We show results for the isotopes CH${}_4$ and CD${}_4$ and thereby provide direct theoretical support for a recent experiment [Baker {\it et al.}, Science {\bf 312}, 424 (2006)] that uses high-order harmonic generation to probe the ultra-fast structural nuclear rearrangement of ionized methane.

6 pages, 6 figures

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Cited by in corpus (2)

• Self-probing of Molecules with High Harmonic Generation
• Full-dimensional treatment of short-time vibronic dynamics in molecular high-harmonics generation process in methane