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The importance of Rydberg orbitals in dissociative ionization of small hydrocarbon molecules in intense laser fields

Much of our intuition about strong-field processes is built upon studies of diatomic molecules, which typically have electronic states that are relatively well separated in energy. In polyatomic molecules, however, the electronic states are closer together, leading to more complex interactions. A co...

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Autores principales: Jochim, Bethany, Siemering, R., Zohrabi, M., Voznyuk, O., Mahowald, J. B., Schmitz, D. G., Betsch, K. J., Berry, Ben, Severt, T., Kling, Nora G., Burwitz, T. G., Carnes, K. D., Kling, M. F., Ben-Itzhak, I., Wells, E., de Vivie-Riedle, R.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2017
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5493692/
https://www.ncbi.nlm.nih.gov/pubmed/28667335
http://dx.doi.org/10.1038/s41598-017-04638-0
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author Jochim, Bethany
Siemering, R.
Zohrabi, M.
Voznyuk, O.
Mahowald, J. B.
Schmitz, D. G.
Betsch, K. J.
Berry, Ben
Severt, T.
Kling, Nora G.
Burwitz, T. G.
Carnes, K. D.
Kling, M. F.
Ben-Itzhak, I.
Wells, E.
de Vivie-Riedle, R.
author_facet Jochim, Bethany
Siemering, R.
Zohrabi, M.
Voznyuk, O.
Mahowald, J. B.
Schmitz, D. G.
Betsch, K. J.
Berry, Ben
Severt, T.
Kling, Nora G.
Burwitz, T. G.
Carnes, K. D.
Kling, M. F.
Ben-Itzhak, I.
Wells, E.
de Vivie-Riedle, R.
author_sort Jochim, Bethany
collection PubMed
description Much of our intuition about strong-field processes is built upon studies of diatomic molecules, which typically have electronic states that are relatively well separated in energy. In polyatomic molecules, however, the electronic states are closer together, leading to more complex interactions. A combined experimental and theoretical investigation of strong-field ionization followed by hydrogen elimination in the hydrocarbon series C(2)D(2), C(2)D(4) and C(2)D(6) reveals that the photofragment angular distributions can only be understood when the field-dressed orbitals rather than the field-free orbitals are considered. Our measured angular distributions and intensity dependence show that these field-dressed orbitals can have strong Rydberg character for certain orientations of the molecule relative to the laser polarization and that they may contribute significantly to the hydrogen elimination dissociative ionization yield. These findings suggest that Rydberg contributions to field-dressed orbitals should be routinely considered when studying polyatomic molecules in intense laser fields.
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spelling pubmed-54936922017-07-05 The importance of Rydberg orbitals in dissociative ionization of small hydrocarbon molecules in intense laser fields Jochim, Bethany Siemering, R. Zohrabi, M. Voznyuk, O. Mahowald, J. B. Schmitz, D. G. Betsch, K. J. Berry, Ben Severt, T. Kling, Nora G. Burwitz, T. G. Carnes, K. D. Kling, M. F. Ben-Itzhak, I. Wells, E. de Vivie-Riedle, R. Sci Rep Article Much of our intuition about strong-field processes is built upon studies of diatomic molecules, which typically have electronic states that are relatively well separated in energy. In polyatomic molecules, however, the electronic states are closer together, leading to more complex interactions. A combined experimental and theoretical investigation of strong-field ionization followed by hydrogen elimination in the hydrocarbon series C(2)D(2), C(2)D(4) and C(2)D(6) reveals that the photofragment angular distributions can only be understood when the field-dressed orbitals rather than the field-free orbitals are considered. Our measured angular distributions and intensity dependence show that these field-dressed orbitals can have strong Rydberg character for certain orientations of the molecule relative to the laser polarization and that they may contribute significantly to the hydrogen elimination dissociative ionization yield. These findings suggest that Rydberg contributions to field-dressed orbitals should be routinely considered when studying polyatomic molecules in intense laser fields. Nature Publishing Group UK 2017-06-30 /pmc/articles/PMC5493692/ /pubmed/28667335 http://dx.doi.org/10.1038/s41598-017-04638-0 Text en © The Author(s) 2017 Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.
spellingShingle Article
Jochim, Bethany
Siemering, R.
Zohrabi, M.
Voznyuk, O.
Mahowald, J. B.
Schmitz, D. G.
Betsch, K. J.
Berry, Ben
Severt, T.
Kling, Nora G.
Burwitz, T. G.
Carnes, K. D.
Kling, M. F.
Ben-Itzhak, I.
Wells, E.
de Vivie-Riedle, R.
The importance of Rydberg orbitals in dissociative ionization of small hydrocarbon molecules in intense laser fields
title The importance of Rydberg orbitals in dissociative ionization of small hydrocarbon molecules in intense laser fields
title_full The importance of Rydberg orbitals in dissociative ionization of small hydrocarbon molecules in intense laser fields
title_fullStr The importance of Rydberg orbitals in dissociative ionization of small hydrocarbon molecules in intense laser fields
title_full_unstemmed The importance of Rydberg orbitals in dissociative ionization of small hydrocarbon molecules in intense laser fields
title_short The importance of Rydberg orbitals in dissociative ionization of small hydrocarbon molecules in intense laser fields
title_sort importance of rydberg orbitals in dissociative ionization of small hydrocarbon molecules in intense laser fields
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5493692/
https://www.ncbi.nlm.nih.gov/pubmed/28667335
http://dx.doi.org/10.1038/s41598-017-04638-0
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