Attosecond probing of vibrational dynamics with high-harmonic generation

Phys Rev Lett. 2005 Feb 11;94(5):053004. doi: 10.1103/PhysRevLett.94.053004. Epub 2005 Feb 11.


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.