A transition state view on reactive scattering: Initial state-selected reaction probabilities for the H+CH4→H2+CH3 reaction studied in full dimensionality

摘要: Initial state-selected reaction probabilities for the H+CH(4)→H(2)+CH(3) are computed vanishing total angular momentum by full-dimensional calculations employing multiconfigurational time-dependent Hartree approach. An ensemble of wave packets completely describing reactivity energies up to 0.58 eV is constructed in transition state region diagonalization thermal flux operator. These then propagated into reactant asymptotic obtain initial probabilities. Reaction reactants all rotational states vibrational 1A(1), 1F(2), and 1E levels methane presented. Vibrational excitation found decrease when at equivalent compared but increase comparison done basis collision energies. Only a fraction energy can be utilized promote reaction. The effect on differs depending methane. For 1A(1) 1F(2) methane, decreases probability even comparing In contrast, more efficient than translational increasing starts from All findings explained based interpretation process.