High harmonic interferometry of multi-electron dynamics in molecules

Olga Smirnova (1, 2) , Yann Mairesse (2, 3) , Serguei Patchkovskii (2) , Nirit Dudovich (2, 4) , David Villeneuve (2) , Paul Corkum (2) , Misha Yu. Ivanov (2, 5)

1 MBI - Max-Born-Institut für Nichtlineare Optik und Kurzzeitspektroskopie
2 NRC - National Research Council of Canada
3 CELIA - Centre d'Etudes Lasers Intenses et Applications
4 Department of Physics of Complex System
5 Department of Physics [Imperial College London]

High harmonic emission occurs when an electron, liberated from a molecule by an incident intense laser field, gains energy from the field and recombines with the parent molecular ion. The emission provides a snapshot of the structure and dynamics of the recombining system, encoded in the amplitudes, phases and polarization of the harmonic light. Here we show with CO2 molecules that high harmonic interferometry can retrieve this structural and dynamic information: by measuring the phases and amplitudes of the harmonic emission, we reveal 'fingerprints' of multiple molecular orbitals participating in the process and decode the underlying attosecond multi-electron dynamics, including the dynamics of electron rearrangement upon ionization. These findings establish high harmonic interferometry as an effective approach to resolving multi-electron dynamics with sub-Ångström spatial resolution arising from the de Broglie wavelength of the recombining electron, and attosecond temporal resolution arising from the timescale of the recombination event

Domains: Strongly Correlated Electrons [cond-mat.str-el]; Atomic and Molecular Clusters [physics.atm-clus]

Olga Smirnova, Yann Mairesse, Serguei Patchkovskii, Nirit Dudovich, David Villeneuve, et al.. High harmonic interferometry of multi-electron dynamics in molecules. Nature, 2009, 460 (7258), pp.972-977. ⟨10.1038/nature08253⟩. ⟨cea-00909919⟩