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Highest electron affinity as a predictor of cluster anion structures

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NatMat120021.pdf
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2002

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Kronik, Leeor
Fromherz, Roland
Ko, Eunjung
Ganteför, Gerd
Chelikowsky, James R.

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Nature Materials. 2002, 1(1), pp. 49-53. Available under: doi: 10.1038/nmat704

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Small clusters have a range of unique physical and chemical phenomena that are strongly size dependent. However, analysis of these phenomena often assumes that thermodynamic equilibrium conditions prevail. We compare experimentally measured and ab initio computed photoelectron spectra of bare and deuterated silicon cluster anions produced in a plasma environment. We find that the isomers detected experimentally are usually not the ground-state isomers, but metastable ones, which indicates that cluster relaxation is strongly limited kinetically by a dwell time that is much shorter than the relaxation time. We show that, under these conditions, the highest electron affinity replaces the traditional lowest total energy as the appropriate criterion for predicting isomer structures. These findings demonstrate that a stringent examination of non-equilibrium effects can be crucial for a correct analysis of cluster properties.

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530 Physik

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ISO 690KRONIK, Leeor, Roland FROMHERZ, Eunjung KO, Gerd GANTEFÖR, James R. CHELIKOWSKY, 2002. Highest electron affinity as a predictor of cluster anion structures. In: Nature Materials. 2002, 1(1), pp. 49-53. Available under: doi: 10.1038/nmat704
BibTex
@article{Kronik2002Highe-4996,
  year={2002},
  doi={10.1038/nmat704},
  title={Highest electron affinity as a predictor of cluster anion structures},
  number={1},
  volume={1},
  journal={Nature Materials},
  pages={49--53},
  author={Kronik, Leeor and Fromherz, Roland and Ko, Eunjung and Ganteför, Gerd and Chelikowsky, James R.}
}
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