Filters

2017 - 20182

More filters

20232
Reset filters

Settings

Author: Bello, Roger Y. × Type: Article ×

Search Results

Now showing 1 - 2 of 2
  • Thumbnail Image
    Item
    A molecular clock for autoionization decay
    (Bristol : IOP Publ., 2017-06-14) Medišauskas, Lukas; Bello, Roger Y.; Palacios, Alicia; González-Castrillo, Alberto; Morales, Felipe; Plimak, Lev; Smirnova, Olga; Martín, Fernando; Ivanov, Misha Yu
    The ultrafast decay of highly excited electronic states is resolved with a molecular clock technique, using the vibrational motion associated to the ionic bound states as a time-reference. We demonstrate the validity of the method in the context of autoionization of the hydrogen molecule, where nearly exact full dimensional ab-initio calculations are available. The vibrationally resolved photoionization spectrum provides a time–energy mapping of the autoionization process into the bound states that is used to fully reconstruct the decay in time. A resolution of a fraction of the vibrational period is achieved. Since no assumptions are made on the underlying coupled electron–nuclear dynamics, the reconstruction procedure can be applied to describe the general problem of the decay of highly excited states in other molecular targets.
  • Thumbnail Image
    Item
    Reconstruction of the time-dependent electronic wave packet arising from molecular autoionization
    (Washington, DC [u.a.] : Assoc., 2018) Bello, Roger Y.; Canton, Sophie E.; Jelovina, Denis; Bozek, John D.; Rude, Bruce; Smirnova, Olga; Ivanov, Mikhail Y.; Palacios, Alicia; Martín, Fernando
    Autoionizing resonances are paradigmatic examples of two-path wave interferences between direct photoionization, which takes a few attoseconds, and ionization via quasi-bound states, which takes much longer. Time-resolving the evolution of these interferences has been a long-standing goal, achieved recently in the helium atom owing to progress in attosecond technologies. However, already for the hydrogen molecule, similar time imaging has remained beyond reach due to the complex interplay between fast nuclear and electronic motions. We show how vibrationally resolved photoelectron spectra of H2 allow one to reconstruct the associated subfemtosecond autoionization dynamics by using the ultrafast nuclear dynamics as an internal clock, thus forgoing ultrashort pulses. Our procedure should be general for autoionization dynamics in molecules containing light nuclei, which are ubiquitous in chemistry and biology.