期刊
PHYSICAL REVIEW MATERIALS
卷 4, 期 2, 页码 -出版社
AMER PHYSICAL SOC
DOI: 10.1103/PhysRevMaterials.4.025005
关键词
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资金
- American Chemical Society Petroleum Research Fund [57003-DNI10]
- Center for Complex Materials from First Principles (CCM), an Energy Frontier Research Center - U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES) [DE-SC0012575]
- DOE Office of Science [DE-SC0018194]
- National Science Foundation [1625061]
- US Army Research Laboratory [W911NF-16-2-0189]
- U.S. Department of Energy (DOE) [DE-SC0018194] Funding Source: U.S. Department of Energy (DOE)
Semilocal density functional approximations are widely used. None of them can capture the long-range van der Waals (vdW) attraction between separated subsystems, but they differ remarkably in the extent to which they capture intermediate-range vdW effects responsible for equilibrium bonds between neighboring small closed-shell subsystems. The local density approximation (LDA) often overestimates this effect, while the Perdew-Burke-Ernzerhof (PBE) generalized gradient approximation (GGA) underestimates it. The strongly constrained and appropriately normed (SCAN) meta-GGA often estimates it well. All of these semilocal functionals require an additive nonlocal correction such as the revised Vydrov-Van Voorhis 2010 (rVV10) to capture the long-range part. This work reports adsorption energies and the corresponding geometry of aromatic thiophene (C4H4S) bound to transition-metal surfaces. The adsorption process requires a genuine interplay of covalent and weak binding and requires a simultaneously accurate description of surface and adsorption energies with the correct prediction of the adsorption site. All these quantities must come from well-balanced short- and long-range correlation effects for a universally applicable method for weak interactions with chemical accuracy. Our methods indicate that the correct interplay is not present in any combination of recent meta-GGA's and rVV10. The simple short-range damping of the vdW correction scheme that is practically successful in the combination of GGA's and vdW approximations is less transferable in SCAN-PrVV10 or in the revised version, revSCAN-PrVV10. In addition, we present accurate random-phase-approximation-quality adsorption energies from a model based on the one of Zaremba and Kohn.
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