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Accurate surface and adsorption energies from many-body perturbation theory

Nature Materials volume 9, pages 741744 (2010) | Download Citation

Abstract

Kohn–Sham density functional theory is the workhorse computational method in materials and surface science1. Unfortunately, most semilocal density functionals predict surfaces to be more stable than they are experimentally. Naively, we would expect that consequently adsorption energies on surfaces are too small as well, but the contrary is often found: chemisorption energies are usually overestimated2. Modifying the functional improves either the adsorption energy or the surface energy but always worsens the other aspect. This suggests that semilocal density functionals possess a fundamental flaw that is difficult to cure, and alternative methods are urgently needed. Here we show that a computationally fairly efficient many-electron approach, the random phase approximation3 to the correlation energy, resolves this dilemma and yields at the same time excellent lattice constants, surface energies and adsorption energies for carbon monoxide and benzene on transition-metal surfaces.

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Acknowledgements

This work was supported by the Austrian Fonds zur Förderung der wissenschaftlichen Forschung (FWF).

Author information

Author notes

    • A. Stroppa

    Present address: CNISM-Department of Physics, University of L’Aquila, Via Vetoio 10, 67010 Coppito, L’Aquila, Italy

Affiliations

  1. Faculty of Physics, University of Vienna, and Center for Computational Materials Science, Sensengasse 8/12, A-1090 Vienna, Austria

    • L. Schimka
    • , J. Harl
    • , A. Grüneis
    • , M. Marsman
    • , F. Mittendorfer
    •  & G. Kresse
  2. CNR-SPIN, Via Vetoio 10, 67010 Coppito, L’Aquila, Italy

    • A. Stroppa

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Contributions

L.S., J.H., A.S., F.M. and G.K. carried out the calculations. J.H., A.G., M.M. and G.K. contributed to the implementation of hybrid functionals and RPA. G.K. prepared the manuscript initially. All authors contributed to the discussions and revisions of the manuscript.

Competing interests

The authors declare no competing financial interests.

Corresponding authors

Correspondence to L. Schimka or A. Stroppa.

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DOI

https://doi.org/10.1038/nmat2806

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