Cargando…

Attosecond timing of electron emission from a molecular shape resonance

Shape resonances in physics and chemistry arise from the spatial confinement of a particle by a potential barrier. In molecular photoionization, these barriers prevent the electron from escaping instantaneously, so that nuclei may move and modify the potential, thereby affecting the ionization proce...

Descripción completa

Detalles Bibliográficos
Autores principales: Nandi, S., Plésiat, E., Zhong, S., Palacios, A., Busto, D., Isinger, M., Neoričić, L., Arnold, C. L., Squibb, R. J., Feifel, R., Decleva, P., L’Huillier, A., Martín, F., Gisselbrecht, M.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Association for the Advancement of Science 2020
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7399650/
https://www.ncbi.nlm.nih.gov/pubmed/32789174
http://dx.doi.org/10.1126/sciadv.aba7762
_version_ 1783566183249739776
author Nandi, S.
Plésiat, E.
Zhong, S.
Palacios, A.
Busto, D.
Isinger, M.
Neoričić, L.
Arnold, C. L.
Squibb, R. J.
Feifel, R.
Decleva, P.
L’Huillier, A.
Martín, F.
Gisselbrecht, M.
author_facet Nandi, S.
Plésiat, E.
Zhong, S.
Palacios, A.
Busto, D.
Isinger, M.
Neoričić, L.
Arnold, C. L.
Squibb, R. J.
Feifel, R.
Decleva, P.
L’Huillier, A.
Martín, F.
Gisselbrecht, M.
author_sort Nandi, S.
collection PubMed
description Shape resonances in physics and chemistry arise from the spatial confinement of a particle by a potential barrier. In molecular photoionization, these barriers prevent the electron from escaping instantaneously, so that nuclei may move and modify the potential, thereby affecting the ionization process. By using an attosecond two-color interferometric approach in combination with high spectral resolution, we have captured the changes induced by the nuclear motion on the centrifugal barrier that sustains the well-known shape resonance in valence-ionized N(2). We show that despite the nuclear motion altering the bond length by only 2%, which leads to tiny changes in the potential barrier, the corresponding change in the ionization time can be as large as 200 attoseconds. This result poses limits to the concept of instantaneous electronic transitions in molecules, which is at the basis of the Franck-Condon principle of molecular spectroscopy.
format Online
Article
Text
id pubmed-7399650
institution National Center for Biotechnology Information
language English
publishDate 2020
publisher American Association for the Advancement of Science
record_format MEDLINE/PubMed
spelling pubmed-73996502020-08-11 Attosecond timing of electron emission from a molecular shape resonance Nandi, S. Plésiat, E. Zhong, S. Palacios, A. Busto, D. Isinger, M. Neoričić, L. Arnold, C. L. Squibb, R. J. Feifel, R. Decleva, P. L’Huillier, A. Martín, F. Gisselbrecht, M. Sci Adv Research Articles Shape resonances in physics and chemistry arise from the spatial confinement of a particle by a potential barrier. In molecular photoionization, these barriers prevent the electron from escaping instantaneously, so that nuclei may move and modify the potential, thereby affecting the ionization process. By using an attosecond two-color interferometric approach in combination with high spectral resolution, we have captured the changes induced by the nuclear motion on the centrifugal barrier that sustains the well-known shape resonance in valence-ionized N(2). We show that despite the nuclear motion altering the bond length by only 2%, which leads to tiny changes in the potential barrier, the corresponding change in the ionization time can be as large as 200 attoseconds. This result poses limits to the concept of instantaneous electronic transitions in molecules, which is at the basis of the Franck-Condon principle of molecular spectroscopy. American Association for the Advancement of Science 2020-07-31 /pmc/articles/PMC7399650/ /pubmed/32789174 http://dx.doi.org/10.1126/sciadv.aba7762 Text en Copyright © 2020 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC). https://creativecommons.org/licenses/by-nc/4.0/ https://creativecommons.org/licenses/by-nc/4.0/This is an open-access article distributed under the terms of the Creative Commons Attribution-NonCommercial license (https://creativecommons.org/licenses/by-nc/4.0/) , which permits use, distribution, and reproduction in any medium, so long as the resultant use is not for commercial advantage and provided the original work is properly cited.
spellingShingle Research Articles
Nandi, S.
Plésiat, E.
Zhong, S.
Palacios, A.
Busto, D.
Isinger, M.
Neoričić, L.
Arnold, C. L.
Squibb, R. J.
Feifel, R.
Decleva, P.
L’Huillier, A.
Martín, F.
Gisselbrecht, M.
Attosecond timing of electron emission from a molecular shape resonance
title Attosecond timing of electron emission from a molecular shape resonance
title_full Attosecond timing of electron emission from a molecular shape resonance
title_fullStr Attosecond timing of electron emission from a molecular shape resonance
title_full_unstemmed Attosecond timing of electron emission from a molecular shape resonance
title_short Attosecond timing of electron emission from a molecular shape resonance
title_sort attosecond timing of electron emission from a molecular shape resonance
topic Research Articles
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7399650/
https://www.ncbi.nlm.nih.gov/pubmed/32789174
http://dx.doi.org/10.1126/sciadv.aba7762
work_keys_str_mv AT nandis attosecondtimingofelectronemissionfromamolecularshaperesonance
AT plesiate attosecondtimingofelectronemissionfromamolecularshaperesonance
AT zhongs attosecondtimingofelectronemissionfromamolecularshaperesonance
AT palaciosa attosecondtimingofelectronemissionfromamolecularshaperesonance
AT bustod attosecondtimingofelectronemissionfromamolecularshaperesonance
AT isingerm attosecondtimingofelectronemissionfromamolecularshaperesonance
AT neoricicl attosecondtimingofelectronemissionfromamolecularshaperesonance
AT arnoldcl attosecondtimingofelectronemissionfromamolecularshaperesonance
AT squibbrj attosecondtimingofelectronemissionfromamolecularshaperesonance
AT feifelr attosecondtimingofelectronemissionfromamolecularshaperesonance
AT declevap attosecondtimingofelectronemissionfromamolecularshaperesonance
AT lhuilliera attosecondtimingofelectronemissionfromamolecularshaperesonance
AT martinf attosecondtimingofelectronemissionfromamolecularshaperesonance
AT gisselbrechtm attosecondtimingofelectronemissionfromamolecularshaperesonance