Observation and ultrafast dynamics of a nonvalence correlation-bound state of an anion

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Science Advances  19 May 2017:
Vol. 3, no. 5, e1603106
DOI: 10.1126/sciadv.1603106

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Nonvalence states of molecular anions play key roles in processes, such as electron mobility, in rare-gas liquids, radiation-induced damage to DNA, and the formation of anions in the interstellar medium. Recently, a class of nonvalence bound anion state has been predicted by theory in which correlation forces are predominantly responsible for binding the excess electron. We present a direct spectroscopic observation of this nonvalence correlation-bound state (CBS) in the para-toluquinone trimer cluster anion. Time-resolved photoelectron velocity map imaging shows that photodetachment of the CBS produces a narrow and highly anisotropic photoelectron distribution, consistent with detachment from an s-like orbital. The CBS is bound by ~50 meV and decays by vibration-mediated autodetachment with a lifetime of 700 ± 100 fs. These states are likely to be common in large and/or polarizable anions and clusters and may act as doorway states in electron attachment processes.

  • excited state
  • Ultrafast Spectroscopy
  • non-valence state
  • anion dynamics
  • photoelectron spectroscopy
  • photoelectron imaging
  • dipole-bound state
  • electron attachment

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