TY - JOUR
T1 - Multilayer Multiconfiguration Time-Dependent Hartree Study on the Mode-/Bond-Specific Quantum Dynamics of Water Dissociation on Cu(111)
AU - Song, Qingfei
AU - Zhang, Xingyu
AU - Gatti, Fabien
AU - Miao, Zekai
AU - Zhang, Qiuyu
AU - Meng, Qingyong
N1 - Publisher Copyright:
© 2022 American Chemical Society.
PY - 2022/9/15
Y1 - 2022/9/15
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=85138115103&partnerID=8YFLogxK
U2 - 10.1021/acs.jpca.2c03092
DO - 10.1021/acs.jpca.2c03092
M3 - 文章
C2 - 36054932
AN - SCOPUS:85138115103
SN - 1089-5639
VL - 126
SP - 6047
EP - 6058
JO - Journal of Physical Chemistry A
JF - Journal of Physical Chemistry A
IS - 36
ER -