期刊
JOURNAL OF CHEMICAL PHYSICS
卷 132, 期 3, 页码 -出版社
AMER INST PHYSICS
DOI: 10.1063/1.3290946
关键词
chlorine; Coriolis force; excited states; ground states; hydrogen neutral atoms; potential energy surfaces; spin-orbit interactions
资金
- Chinese Academy of Science [DICP R200402, Y200601)]
- National Natural Science Foundation of China [20688301, 20773127]
- U.S. National Science Foundation [CHE-0848110]
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [0848110] Funding Source: National Science Foundation
We describe a time-dependent wavepacket based method for the calculation of the state-to-state cross sections for the Cl+H-2 reaction including all couplings arising from the nonzero spin and electronic orbital angular momenta of the Cl atom. Reactant-product decoupling allows us to use a physically correct basis in both the reactant and the product arrangements. Our calculated results agree well with the experimental results of Yang and co-workers. We also describe a model with two coupled potential energy surfaces, which includes the spin-orbit coupling, which is responsible for the largest non-Born-Oppenheimer effects in the Cl+H-2 reaction but neglects the off-diagonal electronically diabatic coupling and all Coriolis couplings due to the electronic spin and orbital angular momenta. The comparison of the results of the full six-state and two-state models with an electronically adiabatic (one-state) description reveals that the latter describes well the reaction out of the ground spin-orbit state, while the two-state model, which is computationally much faster than the full six-state model, describes well the reaction from both the ground and excited spin-orbit states.
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