Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 111, Issue 11, Pages 3973-3978Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1316762111
Keywords
attosecond molecular dynamics; free electron lasers; high harmonic generation; XUV pump-probe spectroscopy
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Funding
- Ministerio de Ciencia e Innovacion [FIS2010-15127, CSD 2007-00010]
- European Research Area-Chemistry Project [PIM2010EEC-00751]
- European Grant MC-ITN CORINF
- European Grant MC-RG ATTOTREND [268284]
- European Research Council [XCHEM 290853]
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Understanding the coupled electronic and nuclear dynamics in molecules by using pump-probe schemes requires not only the use of short enough laser pulses but also wavelengths and intensities that do not modify the intrinsic behavior of the system. In this respect, extreme UV pulses of few-femtosecond and attosecond durations have been recognized as the ideal tool because their short wavelengths ensure a negligible distortion of the molecular potential. In this work, we propose the use of two twin extreme UV pulses to create a molecular interferometer from direct and sequential two-photon ionization processes that leave the molecule in the same final state. We theoretically demonstrate that such a scheme allows for a complete identification of both electronic and nuclear phases in the wave packet generated by the pump pulse. We also show that although total ionization yields reveal entangled electronic and nuclear dynamics in the bound states, doubly differential yields (differential in both electronic and nuclear energies) exhibit in addition the dynamics of autoionization, i.e., of electron correlation in the ionization continuum. Visualization of such dynamics is possible by varying the time delay between the pump and the probe pulses.
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