Adsorption on transition metal surfaces: Transferability and accuracy of DFT using the ADS41 dataset

Shaama Mallikarjun Sharada, Rasmus K. B. Karlsson, Yasheng Maimaiti, Johannes Voss, Thomas Bligaard
Year of publication: 
Physical Review B

We present a benchmarking study of adsorption energies on transition metal surfaces computed with select functionals across different density functional theory codes. In addition to gradient corrected functionals, we evaluate the accuracies of representative metaGGAs, including MS2, SCAN, and SCAN+rVV10, as well as a short-range screened hybrid functional, HSE06. The study shows that the challenge of finding a functional that can simultaneously capture both covalent and noncovalent molecule-surface interactions persists, with no single functional in the benchmarking study with average errors <0.2 eV. We find that HSE06 on average does not improve the accuracy compared to PBE for the surface chemistry of transition metals. The BEEF-vdW dispersion-corrected generalized gradient approximation (GGA) and the MS2 metaGGA yield the lowest errors in both chemisorption and dispersion energies, demonstrating that moving up the Jacob's ladder of functionals to screened hybrids does not necessarily improve the description of transition metal surface chemistry.

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