Consecutive reactions of small, free tantalum clusters with dioxygen controlled by relaxation dynamics

J. F. Eckhard, D. Neuwirth, C. Panosetti, H. Oberhofer, K. Reuter, M. Tschurl, U. Heiz

Research output: Contribution to journalArticlepeer-review

11 Scopus citations

Abstract

The reaction of small cationic tantalum clusters (Tan +, n = 4-8) with molecular oxygen is studied under multi-collision conditions in the gas phase, and the reaction kinetics are analyzed in order to elucidate underlying mechanisms. Reaction pathways as well as relevant apparent rate constants are reported. Two principal pathways in the consecutive oxidation reaction are present in this size regime: solely oxidative degradation (loss of a TaO fragment) in the beginning followed by parallel intact oxidation of certain intermediate species. Selected product structures and energies are subsequently determined via density functional theory calculations. The branching between oxidative fragmentation and intact oxidation is related to the corresponding relaxation dynamics.

Original languageEnglish
Pages (from-to)5985-5993
Number of pages9
JournalPhysical Chemistry Chemical Physics
Volume19
Issue number8
DOIs
StatePublished - 2017
Externally publishedYes

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