Influence of collision energy on the dynamics of the reaction H (2S) + NH (X3Σ−) → N (4S) + H2 (X1Σg+) by the state-to-state quantum mechanical study

• Published in: Theoretical chemistry accounts Vol. 133; no. 6
• Main Authors: Yao, Cui-Xia, Zhang, Pei-Yu, Duan, Zhi-Xin, Zhao, Guang-Jiu
• Format: Journal Article
• Language: English
• Published: Berlin/Heidelberg Springer Berlin Heidelberg 01.06.2014
• Subjects: Atomic/Molecular Structure and Spectra; Chemistry; Chemistry and Materials Science; Inorganic Chemistry; Organic Chemistry; Physical Chemistry; Regular Article; Theoretical and Computational Chemistry; State-to-state; Wave packet; Differential cross sections; H + NH; H2; Nitrogen; GPU
• ISSN: 1432-881X; 1432-2234
• DOI: 10.1007/s00214-014-1489-2

State-to-state time-dependent quantum dynamics calculations have been carried out to study the abstraction processes in the title reaction for the first time. The ab initio potential energy surface of the lowest quartet electronic state of the system recently reported by Zhai et al. (J Chem Phys 135:104314/1–104314/7, 2011 ) is employed in this investigation. Influences of the collision energy on the product state-resolved differential cross sections (DCSs) are calculated and discussed. For low collision energies, we find that reactive collisions along the collinear pathway result in the H 2 product backward scattering. In the case of high collision energy, the stripping collisions with larger impact parameters tend to produce sideways scattering and furnish a high internal excitation of the H 2 . The product H 2 is found to have an inverted rotational distribution and no inversion in vibrational distributions. Moreover, the state-to-state DCSs provide a global perspective of the reaction mechanisms and their contribution to the final H 2 internal energy states. A reaction model is built and works well for our calculated results.