Insight into the description of van der Waals forces for benzene adsorption on transition metal (111) surfaces
Insight into the description of van der Waals forces for benzene adsorption on transition metal (111) surfaces
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DOI：
10.1063/1.4866175
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发表时间：
2014-02-28
影响因子：
4.4
通讯作者：
Tkatchenko, Alexandre
中科院分区：
文献类型：
--
作者：
Carrasco, Javier;Liu, Wei;Tkatchenko, Alexandre
近年来，由于密度泛函理论（DFT）的令人兴奋的发展，探索范德华力（vdW）对分子在延伸金属表面上吸附的作用成为可能。在这些新开发的包含vdW的方法中，原子间vdW方法考虑了体内的非局部筛选[V]。G. Ruiz， W. Liu， E. Zojer， M. Scheffler和A. Tkatchenko, Phys。[J] .中文信息学报，2014,32(1):1 - 2。Klimes， D. R. Bowler和A. Michaelides， J. Phys。:提供者。物质22,022201(2010)]已经成为有效和准确地解释大多数流行的DFT交换相关泛函中缺乏远程vdW力的有希望的候选者。在这里，我们使用这两种方法来计算苯在一系列紧密排列的（111）表面上的吸附，在这些表面上苯要么是物理吸附（Cu， Ag和Au），要么是化学吸附（Rh, Pd， Ir和Pt）。我们全面比较了两类包含vdw的方法的性能，并在可用的情况下将所得结果与实验数据进行了比较。通过检查计算的吸附能、平衡距离和结合曲线，我们得出结论，这两种方法都可以准确地处理在平衡吸附物-底物距离处的吸附。为此，必须在原子间vdW方案中明确包含电动力学筛选，并在非局部vdW密度泛函的情况下优化交换泛函。然而，这两类方法在大规模的吸附-底物分离中发现了一些差异。(C) 2014 AIP出版有限责任公司
Exploring the role of van der Waals (vdW) forces on the adsorption of molecules on extended metal surfaces has become possible in recent years thanks to exciting developments in density functional theory (DFT). Among these newly developed vdW-inclusive methods, interatomic vdW approaches that account for the nonlocal screening within the bulk [V. G. Ruiz, W. Liu, E. Zojer, M. Scheffler, and A. Tkatchenko, Phys. Rev. Lett. 108, 146103 (2012)] and improved nonlocal functionals [J. Klimes, D. R. Bowler, and A. Michaelides, J. Phys.: Condens. Matter 22, 022201 (2010)] have emerged as promising candidates to account efficiently and accurately for the lack of long-range vdW forces in most popular DFT exchange-correlation functionals. Here we have used these two approaches to compute benzene adsorption on a range of close-packed (111) surfaces upon which it either physisorbs (Cu, Ag, and Au) or chemisorbs (Rh, Pd, Ir, and Pt). We have thoroughly compared the performance between the two classes of vdW-inclusive methods and when available compared the results obtained with experimental data. By examining the computed adsorption energies, equilibrium distances, and binding curves we conclude that both methods allow for an accurate treatment of adsorption at equilibrium adsorbate-substrate distances. To this end, explicit inclusion of electrodynamic screening in the interatomic vdW scheme and optimized exchange functionals in the case of nonlocal vdW density functionals is mandatory. Nevertheless, some discrepancies are found between these two classes of methods at large adsorbate-substrate separations. (C) 2014 AIP Publishing LLC.