Post-Ionization Dynamics of the Polar Molecule OCS in Asymmetric Laser Fields

We have investigated the dissociation mechanisms of the prototypical heavy polar molecule OCS into the two break-up channels of the dication, OCS2+ → O+ + CS+ and OC+ + S+, in phase-locked two-color intense laser fields. The branching ratio of the breaking of the C–O and C–S bonds followed a pronoun...

Full description

Bibliographic Details
Main Authors: Tomoyuki Endo, Karl Michael Ziems, Martin Richter, Friedrich G. Fröbel, Akiyoshi Hishikawa, Stefanie Gräfe, François Légaré, Heide Ibrahim
Format: Article
Language:English
Published: Frontiers Media S.A. 2022-04-01
Series:Frontiers in Chemistry
Subjects:
Online Access:https://www.frontiersin.org/articles/10.3389/fchem.2022.859750/full
_version_ 1819045441453424640
author Tomoyuki Endo
Tomoyuki Endo
Karl Michael Ziems
Karl Michael Ziems
Martin Richter
Friedrich G. Fröbel
Akiyoshi Hishikawa
Akiyoshi Hishikawa
Stefanie Gräfe
Stefanie Gräfe
François Légaré
Heide Ibrahim
author_facet Tomoyuki Endo
Tomoyuki Endo
Karl Michael Ziems
Karl Michael Ziems
Martin Richter
Friedrich G. Fröbel
Akiyoshi Hishikawa
Akiyoshi Hishikawa
Stefanie Gräfe
Stefanie Gräfe
François Légaré
Heide Ibrahim
author_sort Tomoyuki Endo
collection DOAJ
description We have investigated the dissociation mechanisms of the prototypical heavy polar molecule OCS into the two break-up channels of the dication, OCS2+ → O+ + CS+ and OC+ + S+, in phase-locked two-color intense laser fields. The branching ratio of the breaking of the C–O and C–S bonds followed a pronounced 2π-oscillation with a modulation depth of 11%, depending on the relative phase of the two-color laser fields. The fragment ejection direction of both break-up channels reflects the anisotropy of the tunneling ionization rate, following a 2π-periodicity, as well. The two dissociation pathways in the C–S bond breaking channel show different phase dependencies of the fragment ejection direction, which are assigned to post-ionization dynamics. These observations, resulting from the excitation with asymmetric two-color intense laser fields, supported by state-of-the-art theoretical simulations, reveal the importance of post-ionization population dynamics in addition to tunneling ionization in the molecular fragmentation processes, even for heavy polar molecules.
first_indexed 2024-12-21T10:28:37Z
format Article
id doaj.art-d5e03d14fe3d410bbaf9930b3fc69550
institution Directory Open Access Journal
issn 2296-2646
language English
last_indexed 2024-12-21T10:28:37Z
publishDate 2022-04-01
publisher Frontiers Media S.A.
record_format Article
series Frontiers in Chemistry
spelling doaj.art-d5e03d14fe3d410bbaf9930b3fc695502022-12-21T19:07:15ZengFrontiers Media S.A.Frontiers in Chemistry2296-26462022-04-011010.3389/fchem.2022.859750859750Post-Ionization Dynamics of the Polar Molecule OCS in Asymmetric Laser FieldsTomoyuki Endo0Tomoyuki Endo1Karl Michael Ziems2Karl Michael Ziems3Martin Richter4Friedrich G. Fröbel5Akiyoshi Hishikawa6Akiyoshi Hishikawa7Stefanie Gräfe8Stefanie Gräfe9François Légaré10Heide Ibrahim11Institut national de la recherche scientifique, Centre Énergie Matériaux et Télécommunications, Varennes, QC, CanadaKansai Photon Science Institute, National Institutes for Quantum Science and Technology, Kizugawa, JapanInstitute of Physical Chemistry and Abbe Center of Photonics, Friedrich Schiller University Jena, Jena, GermanyMax Planck School of Photonics, Jena, GermanyInstitute of Physical Chemistry and Abbe Center of Photonics, Friedrich Schiller University Jena, Jena, GermanyInstitute of Physical Chemistry and Abbe Center of Photonics, Friedrich Schiller University Jena, Jena, GermanyDepartment of Chemistry, Graduate School of Science, Nagoya University, Nagoya, JapanResearch Center for Materials Science, Nagoya University, Nagoya, JapanInstitute of Physical Chemistry and Abbe Center of Photonics, Friedrich Schiller University Jena, Jena, GermanyMax Planck School of Photonics, Jena, GermanyInstitut national de la recherche scientifique, Centre Énergie Matériaux et Télécommunications, Varennes, QC, CanadaInstitut national de la recherche scientifique, Centre Énergie Matériaux et Télécommunications, Varennes, QC, CanadaWe have investigated the dissociation mechanisms of the prototypical heavy polar molecule OCS into the two break-up channels of the dication, OCS2+ → O+ + CS+ and OC+ + S+, in phase-locked two-color intense laser fields. The branching ratio of the breaking of the C–O and C–S bonds followed a pronounced 2π-oscillation with a modulation depth of 11%, depending on the relative phase of the two-color laser fields. The fragment ejection direction of both break-up channels reflects the anisotropy of the tunneling ionization rate, following a 2π-periodicity, as well. The two dissociation pathways in the C–S bond breaking channel show different phase dependencies of the fragment ejection direction, which are assigned to post-ionization dynamics. These observations, resulting from the excitation with asymmetric two-color intense laser fields, supported by state-of-the-art theoretical simulations, reveal the importance of post-ionization population dynamics in addition to tunneling ionization in the molecular fragmentation processes, even for heavy polar molecules.https://www.frontiersin.org/articles/10.3389/fchem.2022.859750/fulltwo-color laser fieldcoherent control experimentpost-ionization dynamicsreal-time real-space time-dependent density functional theoryCoulomb explosion imaging
spellingShingle Tomoyuki Endo
Tomoyuki Endo
Karl Michael Ziems
Karl Michael Ziems
Martin Richter
Friedrich G. Fröbel
Akiyoshi Hishikawa
Akiyoshi Hishikawa
Stefanie Gräfe
Stefanie Gräfe
François Légaré
Heide Ibrahim
Post-Ionization Dynamics of the Polar Molecule OCS in Asymmetric Laser Fields
Frontiers in Chemistry
two-color laser field
coherent control experiment
post-ionization dynamics
real-time real-space time-dependent density functional theory
Coulomb explosion imaging
title Post-Ionization Dynamics of the Polar Molecule OCS in Asymmetric Laser Fields
title_full Post-Ionization Dynamics of the Polar Molecule OCS in Asymmetric Laser Fields
title_fullStr Post-Ionization Dynamics of the Polar Molecule OCS in Asymmetric Laser Fields
title_full_unstemmed Post-Ionization Dynamics of the Polar Molecule OCS in Asymmetric Laser Fields
title_short Post-Ionization Dynamics of the Polar Molecule OCS in Asymmetric Laser Fields
title_sort post ionization dynamics of the polar molecule ocs in asymmetric laser fields
topic two-color laser field
coherent control experiment
post-ionization dynamics
real-time real-space time-dependent density functional theory
Coulomb explosion imaging
url https://www.frontiersin.org/articles/10.3389/fchem.2022.859750/full
work_keys_str_mv AT tomoyukiendo postionizationdynamicsofthepolarmoleculeocsinasymmetriclaserfields
AT tomoyukiendo postionizationdynamicsofthepolarmoleculeocsinasymmetriclaserfields
AT karlmichaelziems postionizationdynamicsofthepolarmoleculeocsinasymmetriclaserfields
AT karlmichaelziems postionizationdynamicsofthepolarmoleculeocsinasymmetriclaserfields
AT martinrichter postionizationdynamicsofthepolarmoleculeocsinasymmetriclaserfields
AT friedrichgfrobel postionizationdynamicsofthepolarmoleculeocsinasymmetriclaserfields
AT akiyoshihishikawa postionizationdynamicsofthepolarmoleculeocsinasymmetriclaserfields
AT akiyoshihishikawa postionizationdynamicsofthepolarmoleculeocsinasymmetriclaserfields
AT stefaniegrafe postionizationdynamicsofthepolarmoleculeocsinasymmetriclaserfields
AT stefaniegrafe postionizationdynamicsofthepolarmoleculeocsinasymmetriclaserfields
AT francoislegare postionizationdynamicsofthepolarmoleculeocsinasymmetriclaserfields
AT heideibrahim postionizationdynamicsofthepolarmoleculeocsinasymmetriclaserfields