Interaction of Ga3 cluster with molecular hydrogen: combined DFT and CCSD(T) theoretical study
Faculty of Chemistry, Wroclaw University, F. Joliot-Curie 14, 50-383 Wroclaw, Poland
Corresponding author: a email@example.com
Revised: 31 March 2009
Published online: 1 May 2009
We have explored the lowest doublet and quartet potential energy surfaces (PES) for the reaction of gallium trimer with H2. This reaction was studied experimentally by Margrave and co-workers in a noble gas matrix. The detailed reaction paths ending up with the low-energy Ga3H2 hydride isomers have been predicted based on the high level ab initio coupled-cluster calculations (CCSD(T)) with large basis set. We have found that the reaction occuring on the lowest doublet PES is described by the activation barrier for H2 cleavage of about 15 kcal/mol, consistent with experiment. In the most stable Ga3H2 hydride structure, whose formation is exothermic by 15 kcal/mol, both H atoms assume three-fold bridged positions. The diterminal planar structure of Ga3H2, proposed experimentally from the observed IR spectra, is found to be only 1 kcal/mol less stable than the dibridged form.
PACS: 36.40.-c – Atomic and molecular clusters / 36.40.Jn – Reactivity of clusters / 82.20.Kh – Potential energy surfaces for chemical reactions
© EDP Sciences, Società Italiana di Fisica, Springer-Verlag, 2009