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We present the first systematic wavelength-dependent study of laser Coulomb explosion of deuterium molecules at various peak intensities and polarizations. We measured the kinetic energy spectra of D+ for laser wavelengths in the range 480-2000 nm. In addition to the well-known enhanced ionization channel present for all wavelengths, we observe a new high-energy band at short wavelengths. This new band exhibits wavelength dependence, with fragment energy decreasing with increasing wavelengths until it merges with the enhanced ionization band for 800 nm and longer. We attribute the emergence of this band to a new pathway that involves resonant three-photon coupling to the first excited electronic state of the molecular ion during the Coulomb explosion process. This pathway should be accounted for in controlling molecular dynamics of hydrogen by intense laser pulses.
The full text is found in New Journal of Physics, 10, 83011 (07 Aug 2008).
The direct observation of molecular dynamics initiated by x-rays has been hindered to date by the lack of bright femtosecond sources of short-wavelength light. We used soft x-ray beams generated by high-harmonic upconversion of a femtosecond laser to photoionize a nitrogen molecule, creating highly excited molecular cations. A strong infrared pulse was then used to probe the ultrafast electronic and nuclear dynamics as the molecule exploded. We found that substantial fragmentation occurs through an electron-shakeup process, in which a second electron is simultaneously excited during the soft x-ray photoionization process. During fragmentation, the molecular potential seen by the electron changes rapidly from nearly spherically symmetric to a two-center molecular potential. Our approach can capture in real time and with angstrom resolution the influence of ionizing radiation on a range of molecular systems, probing dynamics that are inaccessible with the use of other techniques.
The full text of this paper is found in Science, 317, 1374 (07 Sep 2007).
Last updated on Friday, 17-Oct-2008