高等学校化学学报

高等学校化学学报

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HO+CH4→H2O+CH3反应的偏分势能面与散射共振态理论研究

路熙1, 王华阳2, 蔡政亭1, 冯大诚1   

    1. 山东大学理论化学研究所, 济南 250100;
    2. 鲁东大学物理与电子工程学院, 烟台 264025
  • 收稿日期:2006-10-16 修回日期:1900-01-01 出版日期:2007-10-10 发布日期:2007-10-10
  • 通讯作者: 蔡政亭

Theoretical Study on the Partial Potential Energy Surface and Resonance State for HO+CH4→H2O+CH3 System

LU Xi1, WANG Hua-Yang2, CAI Zheng-Ting1*, FENG Da-Cheng1   

    1. Institute of Theoretical Chemistry, Shandong University, Jinan 250100, China;
    2. School of Physic and Electronic Engineering, Ludong University, Yantai 264025, China
  • Received:2006-10-16 Revised:1900-01-01 Online:2007-10-10 Published:2007-10-10
  • Contact: CAI Zheng-Ting

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摘要： 用ab initio方法构建了该体系的偏分势能面, 并用其研究了该体系中散射共振态的形成机理, 估算了第一共振态寿命.

关键词: HO+CH4→H2O+CH3反应, Feshbach共振, 偏分势能面, 瞬时碰撞络合物, 振动动力学

Abstract: Reaction resonance or Feshbach resonance in polyatomic reaction is one of the most fascinating phenomena in chemical reaction dynamics. The HO+CH4→H2O+CH3 reaction is one of the pivotal polyato-mic reactions concerned with both the experimental and theoretical scientists. Reaction probabilities and other dynamic properties of this system were calculated with quantum scattering theory method, but a simple QH(v)+HO(j)→Q+H2O(m,n) reaction model was used, in which only three degrees of freedom and the rotating of OH were considered while making CH3 as a pseudo atom. In this paper, by an ab initio method, partial potential energy surface(PPES) was constructed and all the 15 internal degrees-freedom were given. Feshbach resonance mechanism of this reaction can be obtained by the dynamic Eyring Lake on the PPES and the lifetime of the reactive resonance-state can be estimated using the gap of the vibrational energy levels of transient collision complex in the critical transition-state region. Above interesting dynamic properties would not be given by simple pseudo atomic reaction model.

Key words: HO+CH4→H2O+CH3 reaction, Feshbach resonance, Partial potential energy surface, Transient collision complex, Vibrational dynamics

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