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Spatial Separation of Molecular Conformers and Clusters
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Size-Resolved Electron Solvation in Neutral Water Clusters.

Loren Ban1, Bruce L Yoder1, Ruth Signorell1

  • 1Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir-Prelog-Weg 2, CH-8093 Zurich, Switzerland.

The Journal of Physical Chemistry. A
|June 11, 2021
PubMed
Summary

The study reveals a minimum cluster size of approximately 14 water molecules is needed to sustain solvated electrons. Larger clusters show increased solvated electron yields over time due to more efficient formation and less loss.

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Area of Science:

  • Physical Chemistry
  • Chemical Physics
  • Spectroscopy

Background:

  • The behavior of solvated electrons in water is crucial for understanding numerous chemical and biological processes.
  • Investigating water clusters provides insights into the transition from gas-phase to bulk liquid properties.

Purpose of the Study:

  • To determine the minimum size of neutral water clusters required to stabilize solvated electrons.
  • To elucidate the size-dependent ultrafast dynamics of solvated electrons in water clusters.

Main Methods:

  • Pump-probe time-of-flight mass spectrometry was employed to study ultrafast dynamics.
  • Below band gap excitation was used to generate electrons in water clusters ranging from n=3 to ~200 molecules.

Main Results:

  • Solvated electrons were not detected in clusters smaller than approximately n=14 molecules.
  • A systematic increase in the number of solvated electrons per molecule was observed with increasing cluster size (n > 14) on femtosecond to picosecond timescales.
  • The observed size dependence suggests more effective electron formation and less effective electron loss pathways in larger clusters.

Conclusions:

  • A minimum cluster size is necessary for the stabilization of solvated electrons in water.
  • Ultrafast dynamics are influenced by cluster size, with larger clusters favoring electron persistence.
  • Size-dependent solvent relaxation dynamics are unlikely to be the primary factor influencing observed time-resolved ion yields.