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Duration of an intense laser pulse can determine the breakage of multiple chemical bonds

Control over the breakage of a certain chemical bond in a molecule by an ultrashort laser pulse has been considered for decades. With the availability of intense non-resonant laser fields it became possible to pre-determine femtosecond to picosecond molecular bond breakage dynamics by controlled dis...

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Autores principales: Xie, Xinhua, Lötstedt, Erik, Roither, Stefan, Schöffler, Markus, Kartashov, Daniil, Midorikawa, Katsumi, Baltuška, Andrius, Yamanouchi, Kaoru, Kitzler, Markus
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group 2015
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4536518/
https://www.ncbi.nlm.nih.gov/pubmed/26271602
http://dx.doi.org/10.1038/srep12877
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author Xie, Xinhua
Lötstedt, Erik
Roither, Stefan
Schöffler, Markus
Kartashov, Daniil
Midorikawa, Katsumi
Baltuška, Andrius
Yamanouchi, Kaoru
Kitzler, Markus
author_facet Xie, Xinhua
Lötstedt, Erik
Roither, Stefan
Schöffler, Markus
Kartashov, Daniil
Midorikawa, Katsumi
Baltuška, Andrius
Yamanouchi, Kaoru
Kitzler, Markus
author_sort Xie, Xinhua
collection PubMed
description Control over the breakage of a certain chemical bond in a molecule by an ultrashort laser pulse has been considered for decades. With the availability of intense non-resonant laser fields it became possible to pre-determine femtosecond to picosecond molecular bond breakage dynamics by controlled distortions of the electronic molecular system on sub-femtosecond time scales using field-sensitive processes such as strong-field ionization or excitation. So far, all successful demonstrations in this area considered only fragmentation reactions, where only one bond is broken and the molecule is split into merely two moieties. Here, using ethylene (C(2)H(4)) as an example, we experimentally investigate whether complex fragmentation reactions that involve the breakage of more than one chemical bond can be influenced by parameters of an ultrashort intense laser pulse. We show that the dynamics of removing three electrons by strong-field ionization determines the ratio of fragmentation of the molecular trication into two respectively three moieties. We observe a relative increase of two-body fragmentations with the laser pulse duration by almost an order of magnitude. Supported by quantum chemical simulations we explain our experimental results by the interplay between the dynamics of electron removal and nuclear motion.
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spelling pubmed-45365182015-09-04 Duration of an intense laser pulse can determine the breakage of multiple chemical bonds Xie, Xinhua Lötstedt, Erik Roither, Stefan Schöffler, Markus Kartashov, Daniil Midorikawa, Katsumi Baltuška, Andrius Yamanouchi, Kaoru Kitzler, Markus Sci Rep Article Control over the breakage of a certain chemical bond in a molecule by an ultrashort laser pulse has been considered for decades. With the availability of intense non-resonant laser fields it became possible to pre-determine femtosecond to picosecond molecular bond breakage dynamics by controlled distortions of the electronic molecular system on sub-femtosecond time scales using field-sensitive processes such as strong-field ionization or excitation. So far, all successful demonstrations in this area considered only fragmentation reactions, where only one bond is broken and the molecule is split into merely two moieties. Here, using ethylene (C(2)H(4)) as an example, we experimentally investigate whether complex fragmentation reactions that involve the breakage of more than one chemical bond can be influenced by parameters of an ultrashort intense laser pulse. We show that the dynamics of removing three electrons by strong-field ionization determines the ratio of fragmentation of the molecular trication into two respectively three moieties. We observe a relative increase of two-body fragmentations with the laser pulse duration by almost an order of magnitude. Supported by quantum chemical simulations we explain our experimental results by the interplay between the dynamics of electron removal and nuclear motion. Nature Publishing Group 2015-08-14 /pmc/articles/PMC4536518/ /pubmed/26271602 http://dx.doi.org/10.1038/srep12877 Text en Copyright © 2015, Macmillan Publishers Limited http://creativecommons.org/licenses/by/4.0/ This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/
spellingShingle Article
Xie, Xinhua
Lötstedt, Erik
Roither, Stefan
Schöffler, Markus
Kartashov, Daniil
Midorikawa, Katsumi
Baltuška, Andrius
Yamanouchi, Kaoru
Kitzler, Markus
Duration of an intense laser pulse can determine the breakage of multiple chemical bonds
title Duration of an intense laser pulse can determine the breakage of multiple chemical bonds
title_full Duration of an intense laser pulse can determine the breakage of multiple chemical bonds
title_fullStr Duration of an intense laser pulse can determine the breakage of multiple chemical bonds
title_full_unstemmed Duration of an intense laser pulse can determine the breakage of multiple chemical bonds
title_short Duration of an intense laser pulse can determine the breakage of multiple chemical bonds
title_sort duration of an intense laser pulse can determine the breakage of multiple chemical bonds
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4536518/
https://www.ncbi.nlm.nih.gov/pubmed/26271602
http://dx.doi.org/10.1038/srep12877
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