title: Communication: Methane dissociation on Ni(111) surface: Importance of azimuth and surface impact site.
abstract: Understanding the role of reactant ro-vibrational degrees of freedom (DOFs) in reaction dynamics of polyatomic molecular dissociation on metal surfaces is of great importance to explore the complex chemical reaction mechanism. Here, we present an expensive quantum dynamics study of the dissociative chemisorption of CH4 on a rigid Ni(111) surface by developing an accurate nine-dimensional quantum dynamical model including the DOF of azimuth. Based on a highly accurate fifteen-dimensional potential energy surface built from first principles, our simulations elucidate that the dissociation probability of CH4 has the strong dependence on azimuth and surface impact site. Some improvements are suggested to obtain the accurate dissociation probability from quantum dynamics simulations.
authors.affiliation: Research Center of Heterogeneous Catalysis and Engineering Sciences, School of Chemical Engineering and Energy, Zhengzhou University, Zhengzhou 450001, China.
authors.forename: Xiangjian
authors.initials: X
authors.lastname: Shen
authors.affiliation: State Key Laboratory of Molecular Reaction Dynamics and Center for Theoretical Computational Chemistry, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, People's Republic of China.
authors.forename: Zhaojun
authors.initials: Z
authors.lastname: Zhang
authors.affiliation: State Key Laboratory of Molecular Reaction Dynamics and Center for Theoretical Computational Chemistry, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, People's Republic of China.
authors.forename: Dong H
authors.initials: DH
authors.lastname: Zhang