2024-03-28T22:05:01Zhttp://digital.csic.es/dspace-oai/requestoai:digital.csic.es:10261/205122021-06-14T09:01:48Zcom_10261_14181com_10261_4col_10261_14182
Zanchet, Alexandre
Roncero, Octavio
Omar, Salama
Paniagua, Miguel
Aguado, Alfredo
2010-02-01T10:38:55Z
2010-02-01T10:38:55Z
2010-01-15
Journal of Chemical Physics 132(3): 032301 (2010)
0021-9606
http://hdl.handle.net/10261/20512
10.1063/1.3290950
A global potential energy surface is obtained for the ground state of the endoergic Au(2S)+H2(X 1)AuH(1+)+H(2S) reaction. The global potential is obtained by fitting highly correlated ab initio calculations on the system, using relativistic pseudopotential for the gold atom. Several electronic states are calculated correlating with Au(2S)+H2, Au(2D)+H2, and H2, Au(2P)+H2 asymptotes. These states show several conical intersections and curve crossings along the minimum energy reaction path which are analyzed in detail. One of them gives rise to an insertion well in which there are important contributions from the Au(2D) and Au(2P) states of gold, which is interesting because it is analog to the deep chemisorption well appearing in larger gold clusters. Quantum wave packet and quasiclassical trajectory dynamical calculations performed for the reaction at zero total angular momentum are in good agreement, provided that a Gaussian binning method is used to account for the zero-point energy of products. Finally, integral and differential cross sections are calculated for the reaction with quasiclassical trajectories. Two different reaction mechanisms are found, one direct and the second indirect, in which the Au atom inserts in between the two hydrogen atoms because of the existence of the insertion well discussed above.
eng
openAccess
Potential energy surface and reactive collisions for the Au+H2 system
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