Proton transfer in ammonia cluster cations: molecular dynamics in a self consistent field

J. C. Greer, R. Ahlrichs, I. V. Hertel

Research output: Journal PublicationArticlepeer-review

43 Citations (Scopus)

Abstract

A theoretical study of the energetics and intramolecular dynamics for ammonia cluster cations (NH3)2+ and (NH3)3+ is presented. The proton transfer mechanism after a vertical ionisation is followed in detail. Structural and energetic calculations are performed near the Hartree-Fock self consistent field (HF-SCF) limit; all open shell calculations are spin restricted (RHF). The calculations reconcile experimental results from thermochemical and photoionisation measurements: discrepancies in the energetics are shown to be due to the probing of different regions of the potential energy surface (PES). For the dynamics calculations, it is impractical to determine a large region of the multidimensional PES and then integrate Newton's equations. The calculations therefore incorporate a quantum mechanical determination of the electronic energy of the system after each time increment while nuclear degrees of freedom are handled classically. In this way, the classical reaction path across the Born-Oppenheimer surface is obtained.

Original languageEnglish
Pages (from-to)413-426
Number of pages14
JournalEuropean Physical Journal D
Volume18
Issue number4
DOIs
Publication statusPublished - Dec 1991
Externally publishedYes

Keywords

  • 36.40 + d
  • 82.20.Kh
  • 82.30.Nr

ASJC Scopus subject areas

  • Atomic and Molecular Physics, and Optics

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