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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...
Autores principales: | , , , , , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American Association for the Advancement of Science
2020
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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 |
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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 |
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