Quantum wave packet and quasiclassical trajectory studies of the reaction H(~2S) + CH(X~2Π; V = 0, j = 1) → C(~1D) + H_2(X~1 Σ g +): Coriolis coupling effects and stereodynamics

摘要

The quantum mechanics (QM) and quasiclassical trajectory (QCT) calculations have been carried out for the title reaction with the ground minimal allowed rotational state of CH (j = 1) on the 1 ~1A′ potential energy surface. For the reaction probability at total angular momentum J = 0, a similar trend of the QM and QCT calculations is observed, and the QM results are larger than the latter almost in the whole considered energy range (0.1-1.5 eV). The QCT integral cross sections are larger than the QM results with centrifugal sudden approximation, while smaller than those from QM method including Coriolis coupling for collision energies bigger than 0.25 eV. The quantum wave-packet computations show that the Coriolis coupling effects get more and more pronounced with increasing of J. In addition to the scalar properties, the stereodynamical properties, such as the average rotational alignment factor , the angular distributions P(θ_r), P(φ_r), P(θ_r, φ_r), and the polarization-dependent generalized differential cross sections have been explored in detail by QCT approach. ? 2013 Wiley Periodicals, Inc. The CH2 system plays an important role in atmospheric and combustion chemistry, thus, to know clearly the chemically dynamical properties will be of great importance. For H(~2S) + CH(X~2Π) → C(~1D) + H_2(X~1 Σg+), we presented the full information of reaction probability, integral cross section and rate constants, various angular distributions as well as the extracted polarization-dependent differential cross-sections. Both quasiclassical trajectory and time-dependent quantum wave-packet methods were carried out on BHL PES.