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

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

2010-01-27

arxiv.org/abs/1001.4882v2

Phys. Rev. A 81, 043413 (2010)

Physics

Atomic Physics

6 pages, 6 figures

Scientific paper

10.1103/PhysRevA.81.043413

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.

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