Journal of Chemical Physics, Vol.100, No.10, 7687-7695, 1994
Quantum-Mechanical Study of H(G)+cl-Au(111) - Eley-Rideal Mechanism
Beams of atomic hydrogen are known to react with halogens adsorbed on metal surfaces, and an Eley-Rideal mechanism has been suggested. The collinear reaction of gas phase H with Cl atoms adsorbed on an Au(111) surface is explored-using time dependent quantum techniques. Probabilities for reaction and reflection are computed as a function of incident ii energy and Cl-metal vibrational state. The time evolution is examined and a long lived intermediate is found to exist in which the Cl is bound to both the H and the metal. The probability for Eley-Rideal reaction is found to be small, on the order of a few to several percent, due primarily to the mass mismatch. The vibrational distribution of the product HCl and the temperature dependence of the reaction probability are in agreement with experiment.
Keywords:DEPENDENT SCHRODINGER-EQUATION;ATOMIC RECOMBINATION DYNAMICS;INTERNAL-STATE DISTRIBUTIONS;MOLECULE PROTON-TRANSFER;FOURIER METHOD SOLUTION;ASSOCIATIVE DESORPTION;VIBRATIONAL-EXCITATION;HYDROGEN DESORPTION;TRIATOMIC-MOLECULES;MONOHYDRIDE PHASE