Accurate surface and adsorption energies from many-body perturbation theory

Author(s)
Laurids Schimka, Judith Harl, Alessandro Stroppa, Andreas Grüneis, Martijn Marsman, Florian Mittendorfer, Georg Kresse
Abstract

Kohn-Sham density functional theory is the workhorse computational method in materials and surface science(1). Unfortunately, most semilocal density functionals predict surfaces to be more stable than they are experimentally. Naively, we would expect that consequently adsorpion energies on surfaces are too small as well, but the contrary is often found: chemisorption energies are usually overestimated(2). 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 approximation(3) 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.

Organisation(s)
Computational Materials Physics
External organisation(s)
Università degli Studi dell’Aquila
Journal
Nature Materials
Volume
9
Pages
741-744
No. of pages
4
ISSN
1476-1122
DOI
https://doi.org/10.1038/nmat2806
Publication date
2010
Peer reviewed
Yes
Austrian Fields of Science 2012
103018 Materials physics
Portal url
https://ucrisportal.univie.ac.at/en/publications/1c5589c1-9a92-4d62-b0cb-fc4d9cd514e9