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Phys Rev Lett. 2005 Feb 11;94(5):053004. Epub 2005 Feb 11.

Attosecond probing of vibrational dynamics with high-harmonic generation.

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Max Planck Institute for the Physics of Complex Systems, Nöthnitzer Strasse 38, 01187 Dresden, Germany.


The numerical solution of the time-dependent Schrodinger equation for vibrating hydrogen molecules in few-cycle laser pulses shows that high-harmonic generation is sensitive to the laser-induced vibrational motion. More intense harmonics are generated in heavier isotopes, the difference increasing with the harmonic frequency. Analytical theory reveals a dependence of the harmonics on the vibrational autocorrelation function. With the help of a genetic algorithm, the nuclear motion can be reconstructed from the harmonic spectra with sub-fs time resolution.

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