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Reaction of Np atom with H2O in the gas phase: reaction mechanisms and ab initio molecular dynamics study

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Abstract

The gas-phase reaction of an Np atom with H2O was investigated using density functional theory and ab initio molecular dynamics. The reaction mechanisms and the corresponding potential energy profiles for different possible spin states were analyzed. Three reaction channels were found in the mechanism study: the isomerization channel, the H2 elimination channel, and the H atom elimination channel. The latter two were observed in the dynamics simulation. It was found that the branching ratio of the title reaction depends on the initial kinetic energy along the transition vector. Product energy distributions for the reaction were evaluated by performing direct classical trajectory calculations on the lowest sextet potential energy surface. The results indicate that most of the available energy appears as the translational energy of the products. The overall results indicate that the H2 elimination channel with low kinetic energy is thermodynamically favored but competes with the H atom elimination channel with higher kinetic energy.

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Acknowledgments

We are very grateful to Dr. Xiaofeng Tian and Dr. Sobereva for many helpful discussions. Computer time made available by the Center of High Performance Computing at the Physics Discipline of Sichuan University is gratefully acknowledged. We would like to thank the reviewers for their valuable suggestions for improving our paper.

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Authors and Affiliations

  1. Institute of Atomic and Molecular Physics, Sichuan University, Chengdu, 610065, China

    Peng Li & Tao Gao

  2. College of Physical Science and Technology, Sichuan University, Chengdu, 610065, China

    Wenxia Niu

  3. School of Physical Science and Technology, Southwest Jiaotong University, Chengdu, 610031, China

    Hongyan Wang

Authors
  1. Peng Li
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  2. Wenxia Niu
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  3. Tao Gao
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  4. Hongyan Wang
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Correspondence to Tao Gao.

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Li, P., Niu, W., Gao, T. et al. Reaction of Np atom with H2O in the gas phase: reaction mechanisms and ab initio molecular dynamics study. J Mol Model 20, 2466 (2014). https://doi.org/10.1007/s00894-014-2466-3

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  • DOI: https://doi.org/10.1007/s00894-014-2466-3

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