吸附
密度泛函理论
一氧化碳
材料科学
饱和(图论)
计算机科学
化学物理
物理
催化作用
物理化学
化学
计算化学
数学
组合数学
生物化学
作者
Peitao Liu,Jian-Tao Wang,Noah Avargues,Carla Verdi,Andreas Singraber,Ferenc Karsai,Xing‐Qiu Chen,Georg Kresse
标识
DOI:10.1103/physrevlett.130.078001
摘要
Adsorption of carbon monoxide (CO) on transition-metal surfaces is a prototypical process in surface sciences and catalysis. Despite its simplicity, it has posed great challenges to theoretical modeling. Pretty much all existing density functionals fail to accurately describe surface energies, CO adsorption site preference, as well as adsorption energies simultaneously. Although the random phase approximation (RPA) cures these density functional theory failures, its large computational cost makes it prohibitive to study the CO adsorption for any but the simplest ordered cases. Here, we address these challenges by developing a machine-learned force field (MLFF) with near RPA accuracy for the prediction of coverage-dependent adsorption of CO on the Rh(111) surface through an efficient on-the-fly active learning procedure and a $\Delta$-machine learning approach. We show that the RPA-derived MLFF is capable to accurately predict the Rh(111) surface energy, CO adsorption site preference as well as adsorption energies at different coverages that are all in good agreement with experiments. Moreover, the coverage-dependent ground-state adsorption patterns and adsorption saturation coverage are identified.
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