Department of Chemistry, University of Massachusetts, Amherst, Massachusetts 01003, USA.
Phys Rev Lett. 2009 Dec 18;103(25):253201. doi: 10.1103/PhysRevLett.103.253201.
The nature of the lattice motion during the dissociation of methane on Ni(111) is analyzed in great detail, and various models for including lattice effects are explored. It is shown that the thermal vibrations of the lattice strongly modify the reactivity, but that the lattice motion is relatively unperturbed by the incident molecule during the collision, in contrast with several earlier predictions. Based on these studies we propose a new model to describe the effects of lattice motion, which agrees well with exact quantum calculations.
甲烷在 Ni(111) 上离解过程中的晶格运动本质被详细分析，并探索了各种包含晶格效应的模型。结果表明，晶格热振动强烈地改变了反应性，但在碰撞过程中晶格运动相对不受入射分子的干扰，这与几个早期的预测相反。基于这些研究，我们提出了一个新的模型来描述晶格运动的影响，该模型与精确的量子计算吻合得很好。
