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research article

Efficient Semiclassical Evaluation of Electronic Coherences in Polyatomic Molecules

V. Golubev, Nikolay
•
Vanicek, Jiri  
June 1, 2022
Chimia

Exposing a molecule to an intense light pulse can create a nonstationary quantum state, thus launching correlated dynamics of electrons and nuclei. Although much had been achieved in the understanding of fundamental physics behind the electron-nuclear interactions and dynamics, accurate numerical simulations of light-induced processes taking place in polyatomic molecules remain a formidable challenge. Here, we review a recently developed theoretical approach for evaluating electronic coherences in molecules, in which the ultrafast electronic dynamics is coupled to nuclear motion. The presented technique, which combines accurate ab initio on-the-fly simulations of electronic structure with efficient semiclassical procedure to compute the dynamics of nuclear wave packets, is not only computationally efficient, but also can help shed light on the underlying physical mechanisms of decoherence and revival of the electronic coherences driven by nuclear rearrangement.

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Type
research article
DOI
10.2533/chimia.2022.575
Web of Science ID

WOS:000823036600005

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

2022-06-01

Publisher

SWISS CHEMICAL SOC

Published in
Chimia
Volume

76

Issue

6

Start page

575

End page

581

Subjects

Chemistry, Multidisciplinary

•

Chemistry

•

ultrafast electron dynamics

•

electron-nuclear couplings

•

first-principles calculations

•

semiclassical methods

•

ultrafast charge migration

•

quantum coherence

•

nuclear motion

•

dynamics

•

wavepackets

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
LCPT  
Available on Infoscience
August 1, 2022
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/189543
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