Signatures of attosecond electronic-nuclear dynamics in the one-photon ionization of molecular hydrogen: analytical model versus ab initio calculations
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Author(s)
Type
Journal Article
Abstract
We present an analytical model based on the time-dependent WKB approximation to reproduce the photoionization spectra of an H2 molecule in the autoionization region. We explore the nondissociative channel, which is the major contribution after one-photon absorption, and we focus on the features arising in the energy differential spectra due to the interference between the direct and the autoionization pathways. These features depend on both the timescale of the electronic decay of the autoionizing state and the time evolution of the vibrational wavepacket created in this state. With full ab initio calculations and with a one-dimensional approach that only takes into account the nuclear wavepacket associated to the few relevant electronic states we compare the ground state, the autoionizing state, and the background continuum electronic states. Finally, we illustrate how these features transform from molecular-like to atomic-like by increasing the mass of the system, thus making the electronic decay time shorter than the nuclear wavepacket motion associated with the resonant state. In other words, autoionization then occurs faster than the molecular dissociation into neutrals.
Date Issued
2015-05-12
Date Acceptance
2015-04-08
Citation
New Journal of Physics, 2015, 17
ISSN
1367-2630
Publisher
IOP Publishing
Journal / Book Title
New Journal of Physics
Volume
17
Copyright Statement
Content from this work may be used under the terms of the Creative Commons Attribution 3.0 licence. Any further distribution of this work must maintain attribution to the author(s) and the title of the work, journal citation and DOI.
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Sponsor
Engineering & Physical Science Research Council (EPSRC)
Commission of the European Communities
Grant Number
EP/I032517/1
264951
Subjects
Science & Technology
Physical Sciences
Physics, Multidisciplinary
Physics
attosecond dynamics
time-dependent WKB
semiclassical
autoionization
VIBRATIONALLY RESOLVED PHOTOIONIZATION
DISSOCIATIVE PHOTOIONIZATION
CONFIGURATION-INTERACTION
H-2
AUTOIONIZATION
D-2
SPECTROSCOPY
CONTINUUM
STATES
PHASE
Publication Status
Published
Article Number
UNSP 053011