Research ArticleChemistry

Reconstruction of the time-dependent electronic wave packet arising from molecular autoionization

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Science Advances  24 Aug 2018:
Vol. 4, no. 8, eaat3962
DOI: 10.1126/sciadv.aat3962
  • Fig. 1 Vibrationally resolved photoionization cross sections normalized to that for the v = 2 state of H2+ as a function of photon energy.

    Circles with error bars: Experimental data. Full lines: Ab initio calculation. Dashed lines: Fit to the experimental data by using the extended Fano model described in the text [see also (35)].

  • Fig. 2 Evolution of the nuclear wave packets generated in the H2 doubly excited states by the XUV radiation.

    The nuclear wave packets follow the potential energy curves of the Q1 and Q2 states until the latter autoionizes by emitting an electron and leaving the H2+ cation in the 1sσg electronic state. The longer the autoionization time, the longer the wave packet travels in the Q states and the higher the vibrational state in which H2+ is left after autoionization, because the overlap between the moving nuclear wave packet and the final vibrational state is only efficient near the classical turning points of the latter. The Franck-Condon region where the transition from the ground state to the continuum takes place is indicated by a shadowed orange area.

  • Fig. 3 Buildup in time of the interference between direct ionization and autoionization from the lowest Q1 1Σu+ (left panels) and Q2 1Πu (right panels) doubly excited states corresponding to the v = 5 vibrational state of the remaining H2+ ion.

    Similar plots can be obtained for other final v’s. (Top) Square of the wave packet densities obtained from experiment as a function of photoelectron energy (y axis) and time (x axis). (Bottom) Results of the ab initio calculations for a pulse of 200 as. For a better visualization, the monotonic decreasing background associated with the direct ionization channel has been subtracted in all cases.

Supplementary Materials

  • Supplementary material for this article is available at http://advances.sciencemag.org/cgi/content/full/4/8/eaat3962/DC1

    Section S1. Measured photoelectron spectra

    Section S2. Validity and limitations of the reconstruction model

    Section S3. Fit to the experimental data

    Fig. S1. Measured photoelectron spectra as a function of photon and binding energies.

    Fig. S2. Same as in fig. S1 but now with spectra obtained at different photon energies overlaying.

    Fig. S3. Comparison between the experimental and fitted photoionization cross sections for v = 3.

    Reference (51)

  • Supplementary Materials

    This PDF file includes:

    • Section S1. Measured photoelectron spectra
    • Section S2. Validity and limitations of the reconstruction model
    • Section S3. Fit to the experimental data
    • Fig. S1. Measured photoelectron spectra as a function of photon and binding energies.
    • Fig. S2. Same as in fig. S1 but now with spectra obtained at different photon energies overlaying.
    • Fig. S3. Comparison between the experimental and fitted photoionization cross sections for v = 3.
    • Reference (51)

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