High harmonic interferometry of multi-electron dynamics in molecules

• Published in: Nature (London) 2009-08, Vol.460 (7258), p.972-977
• Main Authors: Smirnova, Olga, Mairesse, Yann, Patchkovskii, Serguei, Dudovich, Nirit, Villeneuve, David, Corkum, Paul, Ivanov, Misha Yu
• Format: Article
• Language: English
• Subjects: Analytical chemistry; Atomic and Molecular Clusters; Atomic and molecular physics; Carbon dioxide; Condensed Matter; Electrons; Emissions; Energy conservation; Exact sciences and technology; Fiber optic interferometers; Frequency conversion; harmonic generation, including high-order harmonic generation; Fundamental areas of phenomenology (including applications); Humanities and Social Sciences; Interferometry; Ionization; Molecular properties and interactions with photons; Molecules; multidisciplinary; Multiphoton ionization and excitation to highly excited states (e.g., rydberg states); Nonlinear optics; Optics; Photon interactions with molecules; Physics; Quantum electrodynamics; Quantum optics; Science; Science (multidisciplinary); Strong-field excitation of optical transitions in quantum systems; multi-photon processes; dynamic stark shift; Strongly Correlated Electrons
• ISSN: 0028-0836; 1476-4687
• DOI: 10.1038/nature08253

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 CO 2 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. Electronic movies: attosecond sight The high harmonic emission that accompanies the recombination of an electron with its parent molecular ion in an intense laser field provides a snapshot of the structure and dynamics of the recombining system. Experiments with CO 2 molecules now show that high harmonic interferometry can retrieve this structural and dynamic information by measuring the phases and amplitudes of the harmonic emission. The resulting 'fingerprints' of the multiple molecular orbitals participating in the process can be used to decode the underlying attosecond multi-electron dynamics, including the dynamics of electron rearrangement upon ionization. The light emitted from the system contains images of moving electrons that can be processed into a movie. 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. The high harmonic emission that accompanies the recombination of an electron with its parent molecular ion in an intense laser field provides a snapshot of the structure and dynamics of the recombining system. Experiments on CO 2 molecules now show how to extract information from the properties of the emitted light about the underlying multi-electron d