Smits B, Somers M F
Leiden Institute of Chemistry, Gorlaeus Building, Leiden University, 2300 RA Leiden, The Netherlands.
J Chem Phys. 2022 Oct 7;157(13):134704. doi: 10.1063/5.0112036.
We present results of our recently expanded static corrugation model (SCM) approach that included the relevant surface temperature effects, applied to the dissociative chemisorption reaction of H on a Cu(111) surface. The reaction and rovibrationally elastic scattering probabilities that we obtain at a quantum dynamical (QD) level, as an average of many statically distorted surface configurations, show great agreement with those of a dynamic surface model, which reinforces the validity of the sudden approximation inherent to the SCM. We further investigate several simple methods of binning the final rovibrational state of quasi-classical dynamics simulations, to find those best suited to reproduce the QD results for our system. Finally, we show that the SCM obtained results reproduce experimental dissociation curves very well, when the uncertainty in experimental saturation values is taken into account. Some indication of a slow channel, so far only observed in experiment, can also be found at low incidence energies, although more rigorous QD simulations are required to reduce the noise inherent to our propagation methods.
我们展示了最近扩展的静态波纹模型（SCM）方法的结果，该方法包含了相关的表面温度效应，并应用于H在Cu(111)表面的解离化学吸附反应。我们在量子动力学（QD）水平上获得的反应和振转弹性散射概率，作为许多静态扭曲表面构型的平均值，与动态表面模型的结果高度吻合，这强化了SCM固有的突然近似的有效性。我们进一步研究了几种对准经典动力学模拟的最终振转状态进行分箱的简单方法，以找到最适合重现我们系统QD结果的方法。最后，我们表明，当考虑到实验饱和值的不确定性时，SCM获得的结果能很好地重现实验解离曲线。在低入射能量下也能发现一些迄今为止仅在实验中观察到的慢通道迹象，尽管需要更严格的QD模拟来减少我们传播方法中固有的噪声。
