Influence of the rotational degrees of freedom on the initial sticking probability of water on Pt{110}-(1 x 2): a molecular dynamics study.
Influence of the rotational degrees of freedom on the initial sticking probability of water on Pt{110}-(1 x 2): a molecular dynamics study.
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旋转自由度对水在 Pt{110}-(1 x 2) 上初始粘附概率的影响：分子动力学研究。
DOI：
10.1063/1.3459060
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发表时间：
2010
期刊：
影响因子：
--
通讯作者：
T. Warzocha
中科院分区：
文献类型：
--
作者：
T. Panczyk;V. Fiorin;T. Warzocha
本文用分子动力学方法研究了水在铂{110}-(1×2)表面的初始粘着几率。以前对该系统的研究[T.Panczyk等人，J.化学。太棒了。131,064703(2009年)]得出了以下结论：(I)水的吸附受与表面碰撞过程中初始动能的耗散效率控制，(Ii)该过程可能由电子-空穴对激发机制主导。在目前的工作中，我们将这一研究扩展到了解水分子的取向及其转动能对碰撞过程中能量交换几率的影响。模拟的分子动力学轨迹对应于水分子在不同转动能下的不同取向。我们发现，假设能量交换几率与角度的依赖关系可以解释用超音速分子束获得的实验结果，特别是对于高入射分子束能量。对于低束能，必须在模型中考虑入射动能的色散。这些都是使实验结果能够在良好的定性水平上建模的关键因素。
This work focuses on a molecular dynamics (MD) study of the initial sticking probability of water on the Pt{110}-(1 x 2) surface. Previous studies of the system [T. Panczyk et al., J. Chem. Phys. 131, 064703 (2009)] led to the following conclusions: (i) adsorption of water is controlled by the efficiency of the dissipation of the initial kinetic energy during collision with the surface and (ii) the process is probably dominated by the electron-hole pair excitation mechanism. In the current work, we extend this study to understand the influence of the orientation of the water molecule and its rotational energy on the probability of the energy exchange during collision. The simulated MD trajectories correspond to various orientations of water molecule at different rotational energies. We found that assuming the angular dependence on the probability of the energy exchange can explain the experimental results obtained using supersonic molecular beams, especially for high incident molecular beam energies. For low beam energies, dispersion of the incident kinetic energy must be incorporated into the model. These are the key factors that enable to model the experimental results on a good qualitative level.