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Attosecond timing of electron emission from a molecular shape resonance

Nandi, S. LU ; Plésiat, E. ; Zhong, S. LU ; Palacios, A. ; Busto, D. LU orcid ; Isinger, M. LU ; Neoričić, L. LU ; Arnold, C. L. LU ; Squibb, R. J. and Feifel, R. , et al. (2020) In Science Advances 6(31). p.7762-7762
Abstract

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 N2. 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... (More)

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 N2. 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.

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organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Science Advances
volume
6
issue
31
pages
7762 - 7762
publisher
American Association for the Advancement of Science (AAAS)
external identifiers
  • scopus:85089613548
  • pmid:32789174
ISSN
2375-2548
DOI
10.1126/sciadv.aba7762
project
Attosecond chronoscopy of electron wave-packets probing entanglement and time-ordering of quantum processes
language
English
LU publication?
yes
id
4d16fa39-d17d-4157-8777-d4d5910599a5
date added to LUP
2020-08-27 14:55:44
date last changed
2024-06-27 23:48:54
@article{4d16fa39-d17d-4157-8777-d4d5910599a5,
  abstract     = {{<p>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 N2. 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.</p>}},
  author       = {{Nandi, S. and Plésiat, E. and Zhong, S. and Palacios, A. and Busto, D. and Isinger, M. and Neoričić, L. and Arnold, C. L. and Squibb, R. J. and Feifel, R. and Decleva, P. and L'Huillier, A. and Martín, F. and Gisselbrecht, M.}},
  issn         = {{2375-2548}},
  language     = {{eng}},
  number       = {{31}},
  pages        = {{7762--7762}},
  publisher    = {{American Association for the Advancement of Science (AAAS)}},
  series       = {{Science Advances}},
  title        = {{Attosecond timing of electron emission from a molecular shape resonance}},
  url          = {{http://dx.doi.org/10.1126/sciadv.aba7762}},
  doi          = {{10.1126/sciadv.aba7762}},
  volume       = {{6}},
  year         = {{2020}},
}