摘要
Reaction resonance or Feshbach resonance in polyatomic reaction is one of the most fascinating phenomena in chemical reaction dynamics. The HO+CH4→HO+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.
Reaction resonance or Feshbach resonance in polyatomic reaction is one of the most fascinating phenomena in chemical reaction dynamics. The HO ＋ CH4→HO ＋ CH3 reaction is one of the pivotal polyatomic 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.
出处
《高等学校化学学报》
SCIE
EI
CAS
CSCD
北大核心
2007年第10期1981-1983,共3页
Chemical Journal of Chinese Universities
基金
国家自然科学基金(批准号:20573064)资助.
