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research article

Search for long-lasting electronic coherence using on-the-fly ab initio semiclassical dynamics

Scheidegger, Alan  
•
Vanicek, Jiri  
•
Golubev, Nikolay V.
January 21, 2022
Journal Of Chemical Physics

Using a combination of high-level ab initio electronic structure methods with efficient on-the-fly semiclassical evaluation of nuclear dynamics, we performed a massive scan of small polyatomic molecules searching for a long-lasting oscillatory dynamics of the electron density triggered by the outer-valence ionization. We observed that in most of the studied molecules, either the sudden removal of an electron from the system does not lead to the appearance of the electronic coherence or the created coherences become damped by the nuclear rearrangement on a time scale of a few femtoseconds. However, we report several so far unexplored molecules with the electronic coherences lasting up to 10 fs, which can be good candidates for experimental studies. In addition, we present the full-dimensional simulations of the electronic coherences coupled to nuclear motion in several molecules which were studied previously only in the fixed nuclei approximation. (c) 2022 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/).

  • Details
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Type
research article
DOI
10.1063/5.0076609
Web of Science ID

WOS:000747476200003

Author(s)
Scheidegger, Alan  
Vanicek, Jiri  
Golubev, Nikolay V.
Date Issued

2022-01-21

Publisher

AIP Publishing

Published in
Journal Of Chemical Physics
Volume

156

Issue

3

Article Number

034104

Subjects

Chemistry, Physical

•

Physics, Atomic, Molecular & Chemical

•

Chemistry

•

Physics

•

ultrafast charge migration

•

molecular-dynamics

•

approximation scheme

•

quantum coherence

•

energies

•

ionization

•

excitation

•

efficient

•

pyrazine

•

states

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
LCPT  
Available on Infoscience
February 14, 2022
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/185311
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