Controlling coherent quantum nuclear dynamics in LiH by ultra short IR atto pulses

[en] We examine computationally how ultrashort polarized strong one cycle IR pulses can be used for steering coherent nuclear dynamics in LiH. The nuclear motion is described using the time-dependent Schrödinger equation on a grid for several coupled electronic states. The coupling to the strong field of the pump and probe pulses is included in the Hamiltonian as well as the non adiabatic coupling between the different electronic states. LiH possesses low lying Σ and Π states that can be selectively accessed by controlling the polarization of the pump pulse along the bond or perpendicularly to it. In addition, when using a one cycle pulse, controlling the carrier envelope phase (CEP) allows to select the states that will be coherently excited according to their polarity. Since some of the excited Σ states and all the Π states are repulsive, polarization and CEP control of the pump pulse leads to controlling the dissociation yields. In particular, our quantum dynamics simulations show that the ratio of the fragmentation yields of the Σ2 and Σ3 states can be changed by a factor 10 when the CEP of a one cycle IR pulse polarized along the bond is switched from 0 to π. In addition to probing the dynamics by following the fragmentation, we also report on probing the coherent vibronic wave packet using transient absorption spectra that results from the interaction of the molecular transition dipole with the electric fields of the pump and the probe pulses. The emission spectrum retrieves the different time scales of the vibronic dynamics and probes the time evolution of the coherences. © Springer International Publishing AG 2017.

Research Center/Unit :

Chimie Physique Theorique
Theoretical Physical Chemistry

Disciplines :

Chemistry

Author, co-author :

Nikodem, Astrid ; Université de Liège - ULiège > Département de chimie (sciences) > Laboratoire de chimie physique théorique

Levine, Raphaël David; The Fritz Haber Center for Molecular Dynamics and Institute of Chemistry, The Hebrew University of Jerusalem, Jerusalem, Israel, Crump Institute for Molecular Imaging and Department of Molecular and Medical Pharmacology, David Geffen School of Medicine and Department of Chemistry and Biochemistry, 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 :

Controlling coherent quantum nuclear dynamics in LiH by ultra short IR atto pulses

Publication date :

2017

Main work title :

Progress in Ultrafast Intense Laser Science XIII

Editor :

Yamanouchi, K.

Hill, W.

Paulus, F. G

Publisher :

Springer, Dordrecht, Netherlands

Collection name :

Springer Series in Chemical Physics

Pages :

41-65

Peer reviewed :

Peer reviewed

Name of the research project :

ultrafast molecular dynamics
Steering chemical reactivity DCS0012628

Funders :

DOE - United States. Department of Energy
F.R.S.-FNRS - Fonds de la Recherche Scientifique
COST - European Cooperation in Science and Technology

Funding text :

This work is supported by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES) under Award #DE-SC0012628. We benefited from our participation in the COST action CM1204 XLIC. FR is a director of research with FNRS (Fonds National de la Recherche Scientifique), Belgium.

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