Attosecond probing of nuclear dynamics with trajectory-resolved high-harmonic spectroscopy

Abstract

We report attosecond-scale probing of the laser-induced dynamics in molecules. We apply the method of high-harmonic spectroscopy, where laser-driven recolliding electrons on various trajec- tories record the motion of their parent ion. Based on the transient phase-matching mechanism of high-order harmonic generation, short and long trajectories contributing to the same harmonic order are distinguishable in both the spatial and frequency domains, giving rise to a one-to-one map between time and photon energy for each trajectory. The short and long trajectories in H2 and D2 are used simultaneously to retrieve the nuclear dynamics on the attosecond and angstrom scale. Compared to using only short trajectories, this extends the temporal range of the measurement to one optical cycle. The experiment is also applied to methane and ammonia molecules.

arXiv comment6 pages, 5 figures .To be published in Physical Review Letter

References in corpus (5)

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• Full-dimensional treatment of short-time vibronic dynamics in molecular high-harmonics generation process in methane
• Analytically controlling laser-induced electron phase in sub-cycle motion
• Influence of coherent vibronic excitation on the high harmonics generation of diatomic molecules
• Local most-probable routes and classic-quantum correspondence in strong-field two-dimensional tunneling ionization
• Attosecond delays of high harmonic emissions from isotopes of molecular hydrogen measured by Gouy phase XUV interferometer