Multilayer Multiconfiguration Time-Dependent Hartree Study on the Mode-/Bond-Specific Quantum Dynamics of Water Dissociation on Cu(111)

Qingfei Song, Xingyu Zhang, Fabien Gatti, Zekai Miao, Qiuyu Zhang, Qingyong Meng

科研成果: 期刊稿件文章同行评审

1 引用 (Scopus)

摘要

In this work, full-dimensional (9D) quantum dynamics calculations on mode-/bond-specific surface scattering of a water molecule on a copper (111) rigid surface are performed through the multilayer multiconfiguration time-dependent Hartree (ML-MCTDH) method. To easily perform the ML-MCTDH calculations on such a triatomic molecule-surface system, we first choose specific Jacobi coordinates as a set of coordinates of water. Next, to efficiently perform the 9D ML-MCTDH wavepacket propagation, the potential energy surface is transferred to a canonical polyadic decomposition form with the aid of a Monte Carlo-based method. Excitation-specific dissociation probabilities of H2O on Cu(111) are computed, and mode-/bond-specific dynamics are demonstrated by comparison with a probability curve computed for a water molecule in the ground state. The dependence of the dissociation probability of the initial state of H2O is studied, and it is found that the excitation-specific dissociation probabilities can be divided into three groups. We find that the vibrationally excited states enhance the dissociation reactivity of H2O, while the rotationally excited states hardly influence it.

源语言英语
页(从-至)6047-6058
页数12
期刊Journal of Physical Chemistry A
126
36
DOI
出版状态已出版 - 15 9月 2022

指纹

探究 'Multilayer Multiconfiguration Time-Dependent Hartree Study on the Mode-/Bond-Specific Quantum Dynamics of Water Dissociation on Cu(111)' 的科研主题。它们共同构成独一无二的指纹。

引用此