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Deciphering attosecond molecular dynamics with pump-probe schemes


Deciphering attosecond molecular dynamics with pump-probe schemes

Fernando Martín1*

1Universidad Autonoma de Madrid, Spain

The development of attosecond laser pulses allows one to probe the inner working of atoms, molecules and surfaces on the timescale of the electronic response. In molecules, attosecond pump-probe spectroscopy enables investigations of the prompt charge redistribution and localization that accompany photo-excitation processes, where a molecule is lifted from the ground Born-Oppenheimer potential energy surface to one or more excited surfaces, and where subsequent photochemistry evolves on femto- and attosecond timescales. In this talk I will present a few theoretical examples of realistic molecular attosecond pump-probe experiments in which simple molecules are ionized with a single attosecond pulse (or a train of attosecond pulses) and are subsequently probed by one or several infrared or xuv few-cycle pulses. The evolution of the electronic and nuclear densities in the photo-excited molecule or remaining molecular ions is calculated with attosecond time-resolution and is visualized by varying the delay between the pump and probe pulses. The results of these calculations [1-7] allow us to explain several experimental observations as well as to guide future experimental efforts to uncover ultrafast electron and nuclear dynamics in molecules.


[1] G. Sansone et al, Nature 465, 763 (2010).

[2] S. E. Canton et al, Proc. Natl. Acad. Sci. 108, 7302 (2011)

[3] A. González-Castrillo et al, Phys. Rev. Lett. 108, 063009 (2012)

[4] A. Palacios et al, Proc. Natl. Acad. Sci. 111, 3973 (2014).

[5] F. Calegari et al, Science 346, 336 (2014)

[6] C. Ott et al, Nature 516, 374 (2014)

[7] P. Ranitovic et al, Proc. Natl. Acad. Sci. 111, 912 (2014)