The time-dependent quantum dynamics calculation for reaction O(3P)+CH4 →CH3+OH is made, using of the semirigid vibrating rotor target (SVRT) model and the time-dependent wave packet (TDWP) method. The corresponding r...The time-dependent quantum dynamics calculation for reaction O(3P)+CH4 →CH3+OH is made, using of the semirigid vibrating rotor target (SVRT) model and the time-dependent wave packet (TDWP) method. The corresponding reaction probabilities of different initial states are provided. From the calculation of initial rovibrational statej=0,v=0, 1, we can see that the excitation of the H-CH3 stretching vibration gives significant enhancement of reaction probability and the reaction threshold decreases dramatically with the enhancement of the vibrating excitation, which indicates that the vibrating energy of reagent molecules contributes a lot to the molecular collision. As for the calculation of reaction probability of statev=0,j=0,1,2,3, the results show that the reaction probability rises significantly with the enhancement of rotational quantum numberj while the reaction threshold has no changes. The spatial steric effect of the title reaction is studied and analyzed too after the calculation of reaction probability of statesj=5,k=0–2,n=0 andj=5,k=2,n=0–2 is made.展开更多
The four-dimensional time-dependent quantum dynamics calculations for reactions of group IV hydride with H are carried out by employing the semirigid vibrating rotor target model and the time-dependent wave packet met...The four-dimensional time-dependent quantum dynamics calculations for reactions of group IV hydride with H are carried out by employing the semirigid vibrating rotor target model and the time-dependent wave packet method. The reaction possibility, cross section and rate constants for reactions (H+SiH_4 and H+GeH_4) in different initial vibrational and rotational states are obtained. The common feature for such kind of reaction process is summarized. The theoretical result is consistent with available measurement, which indicates the credibility of this theory and the potential energy surface.展开更多
The semirigid vibrating rotor target (SVRT) model for the polyatomic reaction has been applied to the reaction of F+CH4→HF+CH3. The time-dependent wave packet approach has also been used in the calculation. In the cu...The semirigid vibrating rotor target (SVRT) model for the polyatomic reaction has been applied to the reaction of F+CH4→HF+CH3. The time-dependent wave packet approach has also been used in the calculation. In the current study, reaction probability, cross-section, and rate constant are calculated for the title reaction on the modified J1 (MJ1) potential energy surface (PES). Numerical calculation shows oscillatory structures in the energy dependence of the calculated reaction probability. Those structures are generally associated with broad dynamical resonance. They are almost washed-out in the energy dependence of integral cross-sections due to summation over partial waves. The calculated rate constant is in good agreement with experimental measurement.展开更多
基金supported by the National Natural Science Foundation of China(Grant Nos.19874040 and 10174046).
文摘The time-dependent quantum dynamics calculation for reaction O(3P)+CH4 →CH3+OH is made, using of the semirigid vibrating rotor target (SVRT) model and the time-dependent wave packet (TDWP) method. The corresponding reaction probabilities of different initial states are provided. From the calculation of initial rovibrational statej=0,v=0, 1, we can see that the excitation of the H-CH3 stretching vibration gives significant enhancement of reaction probability and the reaction threshold decreases dramatically with the enhancement of the vibrating excitation, which indicates that the vibrating energy of reagent molecules contributes a lot to the molecular collision. As for the calculation of reaction probability of statev=0,j=0,1,2,3, the results show that the reaction probability rises significantly with the enhancement of rotational quantum numberj while the reaction threshold has no changes. The spatial steric effect of the title reaction is studied and analyzed too after the calculation of reaction probability of statesj=5,k=0–2,n=0 andj=5,k=2,n=0–2 is made.
基金This work was supported in part by the National Natural Science Foundation of China (Grant Nos. 10174046, 10474060 and 10504017).
文摘The four-dimensional time-dependent quantum dynamics calculations for reactions of group IV hydride with H are carried out by employing the semirigid vibrating rotor target model and the time-dependent wave packet method. The reaction possibility, cross section and rate constants for reactions (H+SiH_4 and H+GeH_4) in different initial vibrational and rotational states are obtained. The common feature for such kind of reaction process is summarized. The theoretical result is consistent with available measurement, which indicates the credibility of this theory and the potential energy surface.
基金supported by the National Natural Science Foundation of China(Grant No.20028304)NKBRSF(National Key Basic Research Special Funds)(Grant No.1999075302)as well as the Knowledge Innovation Program of the Chinese Academy of Sciences(Grant No.DICP K2001/E3).
文摘The semirigid vibrating rotor target (SVRT) model for the polyatomic reaction has been applied to the reaction of F+CH4→HF+CH3. The time-dependent wave packet approach has also been used in the calculation. In the current study, reaction probability, cross-section, and rate constant are calculated for the title reaction on the modified J1 (MJ1) potential energy surface (PES). Numerical calculation shows oscillatory structures in the energy dependence of the calculated reaction probability. Those structures are generally associated with broad dynamical resonance. They are almost washed-out in the energy dependence of integral cross-sections due to summation over partial waves. The calculated rate constant is in good agreement with experimental measurement.
