Effect of the reactant vibration on quantum dynamics of the reaction H + CH(v = 0,1,2, j = 0) → H2 + C based on a new CH2(X3A″) potential energy surface

• Published in: Chemical physics 2022-10, Vol.562, p.111677, Article 111677
• Main Authors: Zhao, Juan, Zhang, Lulu, Yue, Daguang, Liu, Dong, Gao, Shang, Wang, Lifei, Meng, Qingtian
• Format: Article
• Language: English
• Subjects: Coriolis coupling effect; Integral cross sections; Time-dependent quantum wave pack method; Vibrational excitation of reactants
• ISSN: 0301-0104
• DOI: 10.1016/j.chemphys.2022.111677

Rate constants (100–2500 K) for the H+CH(v=0, j=0)→H2+C reaction. The solid and dashed lines are the QM-CC, and QCT results in this work (with a wider energy range 0.010–1.0 eV), respectively. The dashed dot and dot lines are QCT results calculated by Zhang et al.[14] and Harding et al.[6]. The experimental results are denoted by ■, and errors bars are ±30%. [Display omitted] •The effect of vibrational excitation of reactants on H + CH → H2 + C reaction probability and integral cross section has been studied using quantum time-dependent wave packet method.•The influence of vibrational excitation on the Coriolis coupling effect has been discussed in detail for the first time.•The effect of vibrational energy level of reactants on reaction mechanism is analyzed in detail.•The calculated reaction rate constants of H + CH(v = 0, j = 0) → H2 + C reaction in the temperature range of 1500–2000 K are much closer to the experimental center values than the existing theoretical ones. Based on the new ab initio potential energy surface of CH2 (X3A″) system, the influence of the reactant vibration on the H + CH → H2 + C reaction has been studied by using quantum time-dependent wave packet method. The results show that for the collision energy lower than 0.47 eV, the vibrational excitation of reactants inhibits the abstraction reaction H + CH → H2 + C, but promotes the exchange reaction H + CH → HC + H. In addition, the vibrational excitation of reactants has also a certain influence on the Coriolis coupling effect. Finally, because of the wider collision energy range (0.010–1.0 eV) in CC and QCT calculations in this work, the calculated reaction rate constants of H + CH(v = 0, j = 0) → H2 + C reaction in the temperature range of 1500–2000 K are much closer to the experimental center value than the existing theoretical results, which shows that the calculation results in this work are more reasonable and accurate.