Article (Scientific journals)
Pumping and probing vibrational modulated coupled electronic coherence in HCN using short UV fs laser pulses: A 2D quantum nuclear dynamical study
van den Wildenberg, Stéphan; Mignolet, Benoît; Levine, Raphaël David et al.
2017In Physical Chemistry Chemical Physics, 19 (30), p. 19837-19846
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Abstract :
[en] The coupled electronic-nuclear coherent dynamics induced by a short strong VUV fs pulse in the low excited electronic states of HCN is probed by transient absorption spectroscopy with a second weaker fs UV pulse. The nuclear time-dependent Schrodinger equation is solved on a 2D nuclear grid with several electronic states with a Hamiltonian including the dipole coupling to the pump and the probe electric fields. The two internal nuclear coordinates describe the motion of the light H atom. There is a band of several excited electronic states at about 8 eV above the ground state (GS) that is transiently accessed by the pump pulse. We tailored the pump so as to selectively populate the lowest 1A′′ electronic state thereby the pulse creates an electronic coherence with the GS. Our simulations show that this electronic coherence is modulated by the nuclear motion and persists all the way to dissociation on the 1A′′ state. Transient absorption spectra computed as a function of the delay time between the pump and the probe pulses provide a detailed probe of the electronic amplitude and its phase, as well as of the modulation of the electronic coherence by the nuclear motion, both bound and dissociative. © the Owner Societies 2017.
Disciplines :
Chemistry
Author, co-author :
van den Wildenberg, Stéphan ;  Université de Liège - ULiège > Département de chimie (sciences) > Département de chimie (sciences)
Mignolet, Benoît ;  Université de Liège - ULiège > Département de chimie (sciences) > Laboratoire de chimie physique théorique
Levine, Raphaël David;  Fritz Haber Research Center for Molecular Dynamics, Institute of Chemistry, Hebrew University of Jerusalem, Jerusalem, Israel, Crump Institute for Molecular Imaging, Department of Molecular and Medical Pharmacology, David Geffen School of Medicine, University of California, Los Angeles, CA, United States
Remacle, Françoise  ;  Université de Liège - ULiège > Département de chimie (sciences) > Laboratoire de chimie physique théorique
Language :
English
Title :
Pumping and probing vibrational modulated coupled electronic coherence in HCN using short UV fs laser pulses: A 2D quantum nuclear dynamical study
Publication date :
2017
Journal title :
Physical Chemistry Chemical Physics
ISSN :
1463-9076
eISSN :
1463-9084
Publisher :
Royal Society of Chemistry
Volume :
19
Issue :
30
Pages :
19837-19846
Peer reviewed :
Peer Reviewed verified by ORBi
Tags :
CÉCI : Consortium des Équipements de Calcul Intensif
Funders :
This work was supported by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES) under Award #DE-SC0012628
FRFC - Fonds de la Recherche Fondamentale Collective [BE]
COST action CM1204 XLIC
CÉCI - Consortium des Équipements de Calcul Intensif [BE]
F.R.S.-FNRS - Fonds de la Recherche Scientifique [BE]
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