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Ionic-Charge Dependence of tie Intermolecular Coulombic Decay Time Scale for Aqueous Ions Probed by the Core-Hole Clock

Pokapanich, Wandared; Kryzhevoi, Nikolai V.; Ottosson, Niklas; Svensson, Svante; Cederbaum, Lorenz S.; Öhrwall, Gunnar LU and Bjorneholm, Olle (2011) In Journal of the American Chemical Society 133(34). p.13430-13436
Abstract
Auger electron spectroscopy combined with theoretical calculations has been applied to investigate the decay of the Ca 2p core hole of aqueous Ca2+. Beyond the localized two-hole final states on the calcium ion, originating from a normal Auger process, we have further identified the final states delocalized between the calcium ion and its water surroundings and produced by core level intermolecular Coulombic decay (ICD) processes. By applying the core-hole clock method, the time scale of the core level ICD was determined to be 33 +/- 1 fs for the 2p core hole of the aqueous Ca2+. The comparison of this time constant to those associated with the aqueous K+, Na+, Mg2+, and Al3+ ions reveals differences of 1 and up to 2 orders of magnitude.... (More)
Auger electron spectroscopy combined with theoretical calculations has been applied to investigate the decay of the Ca 2p core hole of aqueous Ca2+. Beyond the localized two-hole final states on the calcium ion, originating from a normal Auger process, we have further identified the final states delocalized between the calcium ion and its water surroundings and produced by core level intermolecular Coulombic decay (ICD) processes. By applying the core-hole clock method, the time scale of the core level ICD was determined to be 33 +/- 1 fs for the 2p core hole of the aqueous Ca2+. The comparison of this time constant to those associated with the aqueous K+, Na+, Mg2+, and Al3+ ions reveals differences of 1 and up to 2 orders of magnitude. Such large variations in the characteristic time scales of the core level ICD processes is qualitatively explained by different internal decay mechanisms in different ions as well as by different ion solvent distances and interactions. (Less)
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author
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Journal of the American Chemical Society
volume
133
issue
34
pages
13430 - 13436
publisher
The American Chemical Society
external identifiers
  • wos:000295551600042
  • scopus:80052079747
ISSN
1520-5126
DOI
10.1021/ja203430s
language
English
LU publication?
yes
id
e4dfc6e9-cac3-4d08-9719-1b1969ce19e3 (old id 2208190)
date added to LUP
2011-11-28 13:08:13
date last changed
2017-10-22 04:13:31
@article{e4dfc6e9-cac3-4d08-9719-1b1969ce19e3,
  abstract     = {Auger electron spectroscopy combined with theoretical calculations has been applied to investigate the decay of the Ca 2p core hole of aqueous Ca2+. Beyond the localized two-hole final states on the calcium ion, originating from a normal Auger process, we have further identified the final states delocalized between the calcium ion and its water surroundings and produced by core level intermolecular Coulombic decay (ICD) processes. By applying the core-hole clock method, the time scale of the core level ICD was determined to be 33 +/- 1 fs for the 2p core hole of the aqueous Ca2+. The comparison of this time constant to those associated with the aqueous K+, Na+, Mg2+, and Al3+ ions reveals differences of 1 and up to 2 orders of magnitude. Such large variations in the characteristic time scales of the core level ICD processes is qualitatively explained by different internal decay mechanisms in different ions as well as by different ion solvent distances and interactions.},
  author       = {Pokapanich, Wandared and Kryzhevoi, Nikolai V. and Ottosson, Niklas and Svensson, Svante and Cederbaum, Lorenz S. and Öhrwall, Gunnar and Bjorneholm, Olle},
  issn         = {1520-5126},
  language     = {eng},
  number       = {34},
  pages        = {13430--13436},
  publisher    = {The American Chemical Society},
  series       = {Journal of the American Chemical Society},
  title        = {Ionic-Charge Dependence of tie Intermolecular Coulombic Decay Time Scale for Aqueous Ions Probed by the Core-Hole Clock},
  url          = {http://dx.doi.org/10.1021/ja203430s},
  volume       = {133},
  year         = {2011},
}