An approximate full-dimensional quantum dynamics study of the mode specificity in the dissociative chemisorption of D2O on rigid Cu(111).
An approximate full-dimensional quantum dynamics study of the mode specificity in the dissociative chemisorption of D2O on rigid Cu(111).
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DOI：
10.1039/c7cp01770g
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发表时间：
2017-05
期刊：
影响因子：
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通讯作者：
Tianhui Liu;Bina Fu;Dong H Zhang
中科院分区：
文献类型：
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作者：
Tianhui Liu;Bina Fu;Dong H Zhang
采用七维(7D)量子力学计算和格点平均近似方法，计算了D2O在刚性Cu(111)表面的解离几率，研究了D2O在刚性表面上解离化学吸附的模式特异性.通过在精确的9D势能面(PES)上对9个碰撞位置上特定位置的7D结果进行平均，得到了初始处于各种振动状态的D2O的近似9D解离几率。标题反应具有很强的模式特异性，其中D2O的两个伸缩模式的振动激发比增加平动能更有效地促进反应，而单量子和双量子的弯曲激发在低动能下对提高反应活性的效果不如相同的平动能。
The mode specificity of the dissociative chemisorption of D2O on a rigid Cu(111) surface was investigated by calculating the approximate full-dimensional (9D) dissociation probabilities with the implementation of the seven-dimensional (7D) quantum dynamics calculations and site averaging approximations. The approximate 9D dissociation probabilities for D2O initially in various vibrational states were obtained by averaging the site-specific 7D results over 9 impact sites on an accurate 9D potential energy surface (PES). Strong mode specificity was observed for the title reaction, where vibrational excitations of the two stretching modes of D2O are more efficacious than increasing the translational energy in promoting the reaction, while the bending excitations with one and two quanta are less efficacious than the same amount of translational energy in enhancing the reactivity at low kinetic energies.