Excess electron localization sites in neutral water clusters

L. Túri, Ádám Madarász, Peter J. Rossky

Research output: Contribution to journalArticle

44 Citations (Scopus)

Abstract

We present approximate pseudopotential quantum-mechanical calculations of the excess electron states of equilibrated neutral water clusters sampled by classical molecular dynamics simulations. The internal energy of the clusters are representative of those present at temperatures of 200 and 300 K. Correlated electronic structure calculations are used to validate the pseudopotential for this purpose. We find that the neutral clusters support localized, bound excess electron ground states in about 50% of the configurations for the smallest cluster size studied (n=20), and in almost all configurations for larger clusters (n>66). The state is always exterior to the molecular frame, forming typically a diffuse surface state. Both cluster size and temperature dependence of energetic and structural properties of the clusters and the electron distribution are explored. We show that the stabilization of the electron is strongly correlated with the preexisting instantaneous dipole moment of the neutral clusters, and its ground state energy is reflected in the electronic radius. The findings are consistent with electron attachment via an initial surface state. The hypothetical spectral dynamics following such attachment is also discussed.

Original languageEnglish
Article number014308
JournalThe Journal of Chemical Physics
Volume125
Issue number1
DOIs
Publication statusPublished - 2006

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Electrons
Water
Surface states
Ground state
water
electrons
Dipole moment
Electron energy levels
pseudopotentials
Electronic structure
Molecular dynamics
Structural properties
Stabilization
Temperature
ground state
electron attachment
Computer simulation
electron distribution
electron states
configurations

ASJC Scopus subject areas

  • Atomic and Molecular Physics, and Optics

Cite this

Excess electron localization sites in neutral water clusters. / Túri, L.; Madarász, Ádám; Rossky, Peter J.

In: The Journal of Chemical Physics, Vol. 125, No. 1, 014308, 2006.

Research output: Contribution to journalArticle

Túri, L. ; Madarász, Ádám ; Rossky, Peter J. / Excess electron localization sites in neutral water clusters. In: The Journal of Chemical Physics. 2006 ; Vol. 125, No. 1.
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