Dynamics of interaction of H2 and D2 with Ni(110) and Ni(111) surfaces

Abstract

Elastic and direct-inelastic scattering as well as dissociative adsorption and associative desorption of H2 and D2 on Ni(110) and Ni(111) surfaces were studied by molecular beam techniques. Inelastic scattering at the molecular potential is dominated by phonon interactions. With Ni(110), dissociative adsorption occurs with nearly unity sticking probability s0, irrespective of surface temperature Ts and mean kinetic energy normal to the surface 〈 E⊥ 〉. The desorbing molecules exhibit a cos θe angular distribution indicating full thermal accommodation of their translation energy. With Ni(111), on the other hand, s0 is only about 0.05 if both the gas and the surface are at room temperature. s0 is again independent of Ts, but increases continuously with 〈 E⊥ 〉 up to a value of ∼0.4 for 〈 E⊥ 〉 = 0.12 eV. The cos5θe angular distribution of desorbing molecules indicates that in this case they carry off excess translational energy. The results are qualitatively rationalized in terms of a two-dimensional potential diagram with an activation barrier in the entrance channel. While the height of this barrier seems to be negligible for Ni(110), it is about 0.1 eV for Ni(111) and can be overcome through high enough translational energy by direct collision. The results show no evidence for intermediate trapping in a molecular “precursor” state on the clean surfaces, but this effect may play a role at finite coverages.