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Related Experiment Videos

Hydrated electron dynamics: from clusters to bulk.

A E Bragg1, J R R Verlet, A Kammrath

  • 1Department of Chemistry, University of California, Berkeley, CA 94720, USA.

Science (New York, N.Y.)
|September 18, 2004
PubMed
Summary
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Comment on "Characterization of excess electrons in water-cluster anions by quantum simulations".

Science (New York, N.Y.)·2005

Size-selected water clusters reveal electronic relaxation dynamics. Ultrafast laser pulses show electron (ec-) excited states decay and repopulate, supporting the nonadiabatic relaxation mechanism for hydrated electrons (eaq-).

Area of Science:

  • Physical Chemistry
  • Chemical Physics
  • Femtochemistry

Background:

  • The behavior of excess electrons in water is crucial for understanding various chemical and biological processes.
  • Hydrated electrons (eaq-) are fundamental species in aqueous solutions, influencing reactions and biological systems.
  • Previous studies suggest complex relaxation dynamics for excess electrons in water clusters.

Purpose of the Study:

  • To investigate the electronic relaxation dynamics of size-selected water clusters, specifically (H2O)n- and (D2O)n-.
  • To elucidate the mechanism of internal conversion between excited electronic states of excess electrons in water clusters.
  • To provide experimental support for the nonadiabatic relaxation mechanism of the bulk hydrated electron (eaq-).

Main Methods:

Related Experiment Videos

  • Time-resolved photoelectron imaging was employed to study the electronic relaxation dynamics.
  • Size-selected (H2O)n-/(D2O)n- clusters (25 <= n <= 50) were used as the experimental system.
  • An ultrafast laser pulse excited the excess electron (ec-) from its s-state to a p-state (ec-(p)<--ec-(s)), and subsequent evolution was monitored.

    • Main Results:

    • All studied water clusters exhibited decay of the p-state population with simultaneous repopulation of the s-state (internal conversion).
    • The internal conversion lifetimes ranged from 180 to 130 femtoseconds for (H2O)n- and 400 to 225 femtoseconds for (D2O)n-.
    • Lifetimes were observed to decrease with increasing cluster size, indicating size-dependent relaxation dynamics.

    Conclusions:

    • The experimental results support the "nonadiabatic relaxation" mechanism proposed for the bulk hydrated electron (eaq-).
    • This mechanism involves an internal conversion lifetime of approximately 50 femtoseconds for the hydrated electron's p-state to a relaxed state (eaq-(p)-->eaq-(s(dagger))).
    • The study highlights the importance of cluster size in governing the electronic relaxation pathways of excess electrons in water.