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Rapid bond rearrangement in core-excited molecular water.

Laksman, Joakim LU ; Månsson, Erik LU ; Sankari, Anna LU ; Céolin, Denis LU ; Gisselbrecht, Mathieu LU orcid and Ristinmaa Sörensen, Stacey LU (2013) In Physical Chemistry Chemical Physics 15(44). p.19322-19329
Abstract
The angular anisotropy of fragments created in the dissociation of core-electron excited water molecules is studied to probe the correlation between fragmentation channels, kinematics and molecular geometry. We present fragment kinetic measurements for water molecules where the inner-shell oxygen electron is excited to the unoccupied 4a1 and 2b2 valence molecular orbitals. The kinematics of individual fragmentation channels are measured using fully three-dimensional momentum imaging of fragments. The results show that the geometry of the molecule and the kinetic energy of fragments are strongly coupled in the atomisation process. In addition we identify a fragmentation process arising from bond rearrangement evidenced by the H2(+)-O(+) ion... (More)
The angular anisotropy of fragments created in the dissociation of core-electron excited water molecules is studied to probe the correlation between fragmentation channels, kinematics and molecular geometry. We present fragment kinetic measurements for water molecules where the inner-shell oxygen electron is excited to the unoccupied 4a1 and 2b2 valence molecular orbitals. The kinematics of individual fragmentation channels are measured using fully three-dimensional momentum imaging of fragments. The results show that the geometry of the molecule and the kinetic energy of fragments are strongly coupled in the atomisation process. In addition we identify a fragmentation process arising from bond rearrangement evidenced by the H2(+)-O(+) ion pair which is accessible for resonant excitation of the 1s electron. In all of the two-body fragmentation processes the dissociation takes place along the potential-energy surface, while atomisation reveals both dissociation along the potential surface and Coulomb explosion. The angular distribution of fragments suggests that the bond rearrangement is very rapid; likely on a sub 10 fs time scale. (Less)
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author
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organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Physical Chemistry Chemical Physics
volume
15
issue
44
pages
19322 - 19329
publisher
Royal Society of Chemistry
external identifiers
  • wos:000326220000027
  • pmid:24121279
  • scopus:84886781316
  • pmid:24121279
ISSN
1463-9084
DOI
10.1039/c3cp52625a
language
English
LU publication?
yes
id
755b0416-5e7e-4bbd-8222-1d3fed403a14 (old id 4143322)
date added to LUP
2016-04-01 10:58:17
date last changed
2022-01-26 04:20:10
@article{755b0416-5e7e-4bbd-8222-1d3fed403a14,
  abstract     = {{The angular anisotropy of fragments created in the dissociation of core-electron excited water molecules is studied to probe the correlation between fragmentation channels, kinematics and molecular geometry. We present fragment kinetic measurements for water molecules where the inner-shell oxygen electron is excited to the unoccupied 4a1 and 2b2 valence molecular orbitals. The kinematics of individual fragmentation channels are measured using fully three-dimensional momentum imaging of fragments. The results show that the geometry of the molecule and the kinetic energy of fragments are strongly coupled in the atomisation process. In addition we identify a fragmentation process arising from bond rearrangement evidenced by the H2(+)-O(+) ion pair which is accessible for resonant excitation of the 1s electron. In all of the two-body fragmentation processes the dissociation takes place along the potential-energy surface, while atomisation reveals both dissociation along the potential surface and Coulomb explosion. The angular distribution of fragments suggests that the bond rearrangement is very rapid; likely on a sub 10 fs time scale.}},
  author       = {{Laksman, Joakim and Månsson, Erik and Sankari, Anna and Céolin, Denis and Gisselbrecht, Mathieu and Ristinmaa Sörensen, Stacey}},
  issn         = {{1463-9084}},
  language     = {{eng}},
  number       = {{44}},
  pages        = {{19322--19329}},
  publisher    = {{Royal Society of Chemistry}},
  series       = {{Physical Chemistry Chemical Physics}},
  title        = {{Rapid bond rearrangement in core-excited molecular water.}},
  url          = {{http://dx.doi.org/10.1039/c3cp52625a}},
  doi          = {{10.1039/c3cp52625a}},
  volume       = {{15}},
  year         = {{2013}},
}